5

This thesis has been submitted as partial fulfillment for obtaining the degree of D.Med.Sc. at the Faculty
of Medicine, University of Copenhagen. In addition, the thesis contains ten original studies (1-10) listed
below:

List of studies*
1. P. Wolkoff, L.F. Hansen, G.D. Nielsen (1988)
“&may-Irritating Effect of Carbonless Copy
Paper Examined by the Sensory Irritation Test
in Mice”, Environment International, 14, 4 3 4 8 .
2. P. Wolkoff (1990a) “Proposal of Methods for
Developing Healthy Building Materials - Lab-
oratory and Field Experiments”, Environmental
Technology, 11, 327-338.
3. P. Wolkoff (1990b) “Some Guides for Measure-
ments of Volatile Organic Compounds Indoors”,
Environmental Technology, 11, 339-344.
4. P. Wolkoff, P.A. Clausen, P.A. Nielsen, L.
Malhave (199 1a) “The Danish Twin Apartment
Study. Part I: Formaldehyde and Long-Term
Measurements of VOC”, Indoor Air, 1, 478-
490.
5. P. Wolkoff, G.D. Nielsen, L.F. Hansen, 0. Al-
brechtsen, C.R. Johnsen, J. Heinig, C. Franck,
P.A. Nielsen (199 1b) “A Study of Human Reac-
tions to Emissions from Building Materials in
Climatic Chambers. Part 11: VOC Measure-
ments, Mouse Bioassay, and Decipol Evaluation
in the 1-2 mg/m3 TVOC Range”, Indoor Air, 1,
389403.
6. P.A. Clausen, P. Wolkoff, E. Holst, P.A. Nielsen
(1991) “Long Term Emission of Volatile Or-
ganic Compounds from Waterborne Paints.
Methods of Comparison”, Indoor Air, 1, 562-
576.
7. P. Wolkoff, P.A. Clausen, P.A. Nielsen, H. Gus-
tafsson, B. Jonsson, E. Rasmusen (199 1c)
“Field and Laboratory Emission Cell: FLEC”,
LAQ ’91 Healthy Buildings, ASHRAE, pp. 160-
165.
8. P. Wolkoff, C.R. Johnsen, C. Franck, P. Wil-
hardt, 0. Albrechtsen (1992) “A Study of Hu-
man Reactions to Office Machines in a Cli-
matic Chamber”, Journal of Exposure Analysis
and Environmental Epidemiology, Suppl. 1, 7 1-
96.
9. P. Wolkoff, C. Wilkins, P.A. Clausen, K. Larsen
(1993a) “Comparison of Volatile Organic
Compounds from Processed Paper and Toners
from Office Copiers and Printers: Methods,
Emission Rates, and Modeled Concen-
tration~’~,Indoor Air, 3 113-123.
10. P. Wolkoff, P.A. Clausen, P.A. Nielsen and L.
Gunnarsen (1993b) “Documentation of Field
and Laboratory Emission Cell “FLEC” -
Identification of Emission Processes from Car-
pet, Linoleum, Paint, and Sealant”, Indoor Air,
3, 291-297.

*) The studies are marked with an asterisk in the list of references.

 7

Abbreviationsand Terminology

AER Air exchange rate (h-').

BTV Breakthrough volume (Vg). The volume of air at which
5% of a given VOC has eluted through 1 gram of sorbent
CNS- Central nervous system.
Concentration Quantity, mass or mol of volatile organic compound per
m3, normally in &m3 or ppb.
ECA European Collaborative Action, Indoor Air Quality & Its
Impact on Man.
Effective median dose that causes 10% of maximal re-
sponse.
Effective median dose that causes 50% of maximal re-
sponse.
Emission profile Time versus concentration data in a climatic chamber or
room.
Emission rate The release of a VOC per square meter per hour (mg/
(m2X h)) .
ETS Environmental tobacco smoke.
Exposure Concentration of volatile compounds that reaches the
target population, organ or tissue.
FID Flame ionization detector.
FLEC Field and laboratory emission cell.
FWIR Fourier transform infrared spectroscopy.
GC Gas chromatography.
Headspace Air sample above test (material) surface.
HWGC High resolution gas chromatography.
UQ Indoor air quality.
Lipophilicity Measure of solubility in fat. (k,w)i = the octanol-water
partition of VOCi dissolved in octanoVwater.
MS Mass spectrometry.
MVOC Microbiological originated volatile organic compounds.
Odor threshold Concentration of VOC at which 50% of panel can per-
ceive the odor of a given VOC.
PID Photoionization detector.
m50 Concentration which depresses the respiratory rate
(mice) to 50%.
RSD Relative standard deviation.
SBS Sick building syndrome.
SD Solvent desorption.
Source strength Emission rate multiplied by material area (mgh).
svoc Semi volatile organic compound.
TD Thermal desorption.
TLV Occupational threshold limit value.
Tvoc Total (non-reactive) volatile organic compounds; not well
defined.
VDT Video display unit.
voc Volatile organic compound.
woc Very volatile organic compound.
WHO World Health Organization.
8

Units

Dalton = Mass unit.

mg/m3 = Milligram per cubic meter.
CLg/m3 = Microgram per cubic meter.
ng/m3 = Nanogram per cubic meter.
Indoor A i r 199S, S u p p l 3: 9-73
Printed in Denmark ' all rights reserved
Preface
Indoor air research is a multidisciplinary science. It
became clear to me that an understanding of the
possible impact of volatile organic compounds
(VOCs) on the indoor air quality in non-industrial
buildings would include several disciplines. This in-
cludes methodologies of how to sample and ana-
lyze, knowledge of sources and their emission
characteristics, and methods for field investigation,
in addition to climatic chamber exposure studies.
And finally, methodologies for evaluation of the im-
pact on man of the emission from building materials
and office equipment.
The aim of this thesis is to provide an overview,
from a chemist's point of view, of the various
sources of volatile organics encountered in the in-
door environment. I intend the thesis to be an inspi-
ration for researchers to perform research about the
role of VOCs in combination with other indoor pol-
lutants on indoor air quality and the impact on
man.
This work would not have been possible without
the longstanding interest and encouragement from
director-general, D.Med. Sc. Ib Andersen of this insti-
tute, who initiated me into this research field.
Most of the work presented in this thesis has been
based on team work. It is with great pleasure that I
thank all my co-authors for fruitful collaboration.
I am indebted to my long-term co-worker, M. Sc.
Per A. Clausen, who did a great deal of the modeling
work. Aiso, I thank statistician, Ph.D. E. Holst for
statistical advice and assistance.
The mouse bioassay tests were carried out by
Ph. D. Lea E Hansen and my senior colleague, D. Sc.
(Pharm.) Gunnar Damgaard Nielsen whom I sin-
cerely thank for many stimulating discussions and
support over the years.
I would like to thank M. Sc. Peter Wilhardt for per-
forming some of the hygiene measurements and
senior scientist, Ph.D. C. K. Wilkins for valuable as-
sistance and input. Computational assistance was
given by Ph.D. PA. Lund.
I am indebted to Dr. Claus R. Johnsen (National
University Hospital) and Dr. Carsten Frank (Glo-
strup University Hospital, now Chief physician, Sla-
gelse Central Hospital) for assisting with the
Copyright 0 M u n k s g a a r d 1 9 9 5
Indoor Air
ISShT 0908-5920
ISBN 87-16-15184-4
chamber exposure studies and carrying out the
clinical investigations. Discussions with Dr. C .
Franck about the tear film have been much appreci-
ated.
I am grateful to associate professor Ole Albrechtsen
and his staff at The Danish Technical University
(Lyngby) for his help with conducting the chamber
studies.
I am indebted specially to senior scientist Peter A.
Nielsen for long-term collaboration and many fruit-
ful discussions and to senior scientist, Ph.D. L. Gun-
narsen for collaboration, both at The Danish Build-
ing Research Institute.
A Danish-Swedish joint project resulted in devel-
opment and documentation of the Field and Labo-
ratory Emission Cell (FLEC). I am indebted to
M.Sc. Hans Gustafson and B.Sc. B. Jonsson at The
Swedish National Testing and Research Institute for
their contribution.
I thank associate professor, D.Med. Sc. Lars
Molhave at the Institute of Environmental and Oc-
cupational Medicine (University of Aarhus) for col-
laboration in the Danish Twin Apartment Study.
I wish to express my gratitude to Mrs. Inger
Johansen, Mrs. Birthe Kvamm, and B.Sc. Elke
Rasmusen for carrying out the GC work, and special
thanks to M K I(je1d Larsen for technical support and
performing the G U M S work.
Mrs. Kirsten Selmer Pedersen and Mrs. Lisbeth Ro-
senmejer are thanked for their secretarial assistance.
The valuable linguistic assistance by Mrs. Inge Frisch
is much appreciated.
Several of the studies have been financially sup-
ported by The National Housing and Building Agency,
The National Agency for Trade and Indusmy (now
Danish Agency for Development of Trade and In-
dustry), and The Danish Working Environment Fund.
Finally, I would like to thank all subjects who volun-
teered in the chamber exposure studies.
Peder Wolkoff
National Institute of Occupational Health
Denmark
Copenhagen
May 1995
1, Introduction
1.1 Background
The energy crisis of the 1970s resulted in energy
conservation measures such as tighter buildings and
reduced ventilation requirements (Mage and
Gammage, 1985; Esmen, 1985). New building
styles accelerated the use of synthetic building ma-
terials, and there was a rapid increase in use of mo-
dern office technology, such as photocopying ma-
chines, computers, video display terminals, printers,
carbonless copy paper, etc. It is generally believed
that these changes resulted in a large number of new
and (possibly) higher concentrations of organic in-
door air pollutants, in particular in new buildings
(Brown et al., 1994; Lebret et al., 1986; Van der
Wal et al., 1991).
The widespread discontent with perceived de-
teriorated indoor air quality (IAQ complaints) be-
gan also in the 1970s. The term ‘sick building syn-
drome’ (SBS) was introduced (Akimenko et al.,
1986; Apter et al., 1994; ECA, 1989a; WHO
1989a). The SBS term denotes a complex of non-
specific symptoms in more than 20% of the work
force. The symptoms are irritation of mucous mem-
branes of the eye, the nose and the throat, and CNS
related, such as headache, fatigue and difficulties of
concentration. Relief of the symptoms usually oc-
curs upon leaving a building. The most commonly
reported IAQ and SBS complaints are stuffy air,
odor annoyance, and mucous irritation. It is often
hypothesized that increased SBS prevalence has a
multifactorial etiology (Mendell, 1993: Mralhave,
1991) and may arise from different exposure loads,
e.g. pollution, thermal, and psychosocial loads. In-
creased ventilation does not appear to be a panacea
for improving IAQ (Jayjock, 1994), since ventilation
systems have been found to be responsible for re-
duced acceptability among a panel of judges (Fan-
ger et al., 1988).
The IAQ is La. influenced by the universe of in-
door air pollutants. These are characterized by the
following:
They represent a complex mixture of pollutants.
The number of pollutants encountered often is
greater than found in the traditional occupational
environment where a few pollutants generally are
dominant.
Concentration levels are generally lower than
threshold limit values (TLVs) (Arbejdstilsynet,
1994) up to three orders of magnitude.
The number and variation of potential pollutant
sources are great.
The pollutants may be categorized into the follow-
ing three types:
Volatile Inorganic Compounds
1. Gases and vapors
’ Volatile Organic Compounds*
2. Particulate matter, including radioactive particles and en-
vironmental tobacco smoke (ETS)
3 . Biological air contaminants (bacteria, microfungi, etc)
*=W O C s , VOCs, SVOCs (see Table 1.2.1)
1.2 Volatile Organic Compounds
Volatile organics are a broad range of compounds
with boiling points from less than 0°C to about
400°C. WHO (1989a) has classified these into four
categories, see Table 1.2.1. The classification was
based on compound volatility. This overview deals
in particular with volatile organic compounds
(VOCs), i.e. those having boiling points from 50-
100°C to 240-260°C. The molecular weight range
is from 50-70 to about 300 dalton. VOCs exist
mainly in the gas phase in the temperature and hu-
midity ranges encountered indoors. SVOCs and
VOCs overlap to some extent and there is no clear
distinction except boiling point and vapor pressure.
Aldehydes, in general, are also considered in this
overview.
VOCs are ubiquitous in the indoor air. Several
hundred organic compounds have been found in
the indoor environment (Brown et al., 1994; WHO,
1989a). The major classes are shown in Table 1.2.2.
They are further characterized by their indoodout-
door concentration ratios. For typical indoor related
VOCs, the ratio is larger than one (Daisey et al.,
1994; De Bortoli et al., 1986; Cohen et al., 1989;
Lebret et al., 1986; Lewis, 1991; Wallace et al.,
1991). In addition, VOC concentrations are cha-
12 Peder Wolkoff: Volatile Organic Compounds

Table 1.2.1 Classification of organic indoor pollutants

Classification Abbr." Boiling point Vapor Irritation Odor

range pressureC thresholds' thresholds'
from "C to "C" Wad pdm3 Pdm'
Very volatile organic compounds WOCS <o 50-100
Volatile organic compounds VOCs 50-100 240-260",' > 1o-2
1-106 0.1-105
Semi-volatile organic compounds SVOCS 240-260 380-400 1o-2-1 0 - *
Organic compounds associated with POM >380
particulate (organic) matter
a) According to WHO (1989a). b) Polar VOCs appear at the higher end of the range. c) Lewis, 1989. d) 10.' KPa=0.08 mm
Hg. e) Mucous membrane irritation based on the mouse bioassay, RD5,X0.03 (Schaper, 1993). f) Odor detection thresholds
(Devos et al., 1990).

racterized by great variation both in time and space
characterized by the source dynamics (see 2.8) and
the building characteristics (Harrje, 1991). The lat-
ter is expressed by e.g. the great number of different
building types and ventilation systems applied.
The concentrations encountered indoors usually
are sub TLV levels, below airway irritation thres-
holds, but they may be above odor thresholds.
VOCs measured indoors, therefore, are generally
considered "non-reactive" as single substances, ex-
cept for formaldehyde and acrolein. An association
between VOC concentrations and increased SBS
prevalence is not straightforward, probably due to
the hypothesized multifactorial etiology of SBS.
Particles, in particular floor dust, can act as carriers
of VOCs and SVOCs (Gebefiigi, 1989; Wolkoff and
Wilkins, 1994) thus making resuspension of de-
posited dust on the skin an alternative exposure
pathway to inhalation. Water soluble W O C s like
formaldehyde may also be carried by dust
(Kirchherr et al., 1992; Rothenberg et al., 1989), in
addition to surfactants (Kreiss et al., 1982).
A listing of VOC concentrations measured in-
doors has been compiled by WHO (1989a) and re-
cently by Brown et al. (1994). Listings of measured
concentrations are found in major national studies
from Canada (Otson et al., 1992a), Germany
(Krause et al., 1991; Seifert et al., 1989a), The
Netherlands (Lxbret et al., 1986; Van der Wal et
al., 1991), Italy (De Bortoli et al., 1989), European
Parliament (De Bortoli et al., 1990), France (Bar-
guil et al., 1990) and United States (Shah and
Singh, 1988; Wallace et al., 1987a). The individual
VOC concentrations range from ng/m3 to mg/m3.
An American database showed that the majority of
66 indoor VOCs ranged from 0.4 to 4 pg/m3 as-
suming an average molecular weight of 100 (Shah
and Singh, 1988). This agrees with the Australian
review in which the mean concentration of single
VOCs, generally was found to be below 50 pg/m3,
with most below 5 &m3 (Brown et al., 1994). Peak
concentrations, however, will depend on the dy-
namics of the indoor environment and the sampling
strategy.
Qualitative studies of white collar workplaces by
north American government agencies have indi-
cated that indoor contaminants and building fabric
constitute about 12-25% of causes of IAQ pro-
blems (Kirkbridge et al., 1990; Wallingford, 1988).
This was based on identified problems by health

Table 1.2.3 Causes (%) of IAQ problems reported by two north

Table 1.2.2 List of VOC classes taken from WHO j 1989a] American government agencies and based on problems iden-
tified by investigators
VOCs and mean concentration ranges rrg/m3 ~~

Sources 446 buildings 1363 buildings

Alkanes, Cycioalkanes, Aldehydes 1-40 1978-1 986' 1984-1989'
Alkenes 1-20 Ketones 1
Indoor sources 17 12
Cycloalkenes 1-30 Esters Outdoor sources 11 9
Aromatic hydrocarbons 1-80 Other VOC classes: Building materials 3 2
Chlorinated hydrocarbons acids, amines, glycols, glycol Microbiological 5 0.4
1-10 ethers, siloxanes, sulfur con- Inadequate ventilation 52 52
taining VOCs Unknown 12 24
Alcohols 1-2 References: 1) Wallingford, 1988. 2) Kirkbridge et al., 1990.

officers. A major cause appeared to be inadequate
ventilation, less important appeared to be outdoor
sources, and microbiological sources, see Table
1.2.3. The results may not be directly comparable
to European buildings due to different building
styles and ventilation systems. However, when inter-
preting these results, one should be aware of the
study design, the division of causes, the possible
disciplinary bias of investigator and lack of inter-
vention.
Many of the VOCs found indoors may deterio-
rate the IAQ in terms of sensory reactions such as
odor annoyance and eye and airway irritation (Berg-
lund and Lmdvall, 1992: Burge and Hoyer, 1990;
WHO, 1989a). Another important aspect is the
possible loss of productivity by deteriorated IAQ
caused by VOC exposure. However, productivity is
difficult to measure and no clear indication of the
importance of VOCs is available today (Nunes et
al., 1993; Stolwijk and Zyla-Wisensale, 1992).
WHO (1989a) has recognized SBS and the po-
tential role of VOCs and proposed recommenda-
tions which included:
Irritants should not exceed EDlo.
Odors must not exceed ED50.
Emission of VOCs from building materials
should be evaluated.
Source control of emissions of VOCs should be
developed.
Methods of biological burden assessment should
be developed.
Total personal exposure assessment should be
carried out.
Odor (detection) thresholds of 529 VOCs have re-
cently been evaluated (Devos et al., 1990). The
odor thresholds vary across 12 orders of magnitude,
from grams to picograms per m3. The majority of
the thresholds range from mg to pg per m3. How-
ever, this does not exclude the possibility that some
indoor VOCs not yet measured may have thresholds
in the nano to picogram per m3 range, e.g. unsatu-
rated aliphatic aldehydes won Ranson and Belitz,
1992). In addition, the individual sensitivity also has
a wide variation. While odor complaints may not be
directly responsible for serious health effects, they
are still considered unacceptable in the industria-
lized world (poor IAQ) and may result in reduced
production and low morale (McJilton et al.,
1990).
A list as comprehensive as that for odor thres-
Peder Wolkoff: Volatile Organic Compounds I3
holds does not exist for airway irritation for VOCs.
Bos et al. (1992) and Schaper (1993) have reviewed
and compiled about 154 RD50values based on a
standard mouse bioassay (ASTM, 1984). The
RD50, the concentration inducing a 50% reduction
of the respiratory rate in mice, has been proposed
for occupational TLV assessment by TLV=
0.03XRD50 (see Bos et al. (1992) for limitations of
this approach). A substantial number of TLVs of
VOCs reflect airway irritation to a large extent
(Cometto-Muiiiz and Cain, 1991). The difference
between 8 normal working hours 5 days a week and
24 hours spent indoors 7 days a week (continuous
exposure) may lead to indoor relevant irritative
thresholdsz4h equal to about 1/4XTLV. Such a
value should protect against mucous membrane ir-
ritation because irritative effects generally have steep
dose-effect relationships (Commetto-Muiiiz and
Cain, 1991). IAQ evaluations based on TLVs have
been criticized (Hodgson et al., 1994; Pierson et al.,
1991), but this may be avoided by use of an ad-
ditional common safety factor of 10 (Shoaf, 1991).
This would result in a pragmatic “indoor TLV24h”
of 1/40XTLV (Nielsen et al., 1995), provided the
TLV is based on scientific criteria (Peterson, 1992).
A safety factor of about 35 of Dutch TLVs was sug-
gested by Verhoeff et al. (1988) for indoor evalu-
ation of VOC exposure.
1.3 The Office Environment the -
Future Occupational Environment
North Europeans and north Americans, especially
in urban environments, spend more than 90 percent
of their time indoors, at home, at work or during
transport (Letz, 1990). This amount of time is even
greater for children, elderly and sick people. The
more time spent indoors the greater is the total ex-
posure to indoor pollutants. It appears that more
than 60% of the worHorce work in offices or office-
like environments (Wahlberg and Stenberg, 1991).
This proportion of people is anticipated to increase
during the next decades because of modern tech-
nology, e.g. the use of VDTs and encapsulated ma-
chinery. An increase of people working at home is
also anticipated (Mage and Gammage, 1985).
Woods (1989) has estimated that about 20% of
all office workers who are exposed to an office cli-
mate would have adverse health effects like SBS
symptoms. The symptom prevalence of eye and air-
way irritation and CNS related symptoms in the
Danish town hall study was 26% and 23%, respec-
14 Peder Wolkoff Volatile Organic Compounds
tively (Skov et al., 1989). Similar ratings have been
found in other studies (Mendell, 1993). Norback
and Edling (199 1) found that in a normal Swedish
population 16% reported eye irritation experienced
during the last three months, nose and throat irri-
tation 19% and 13%, respectively, 10% had experi-
enced headache, and 30% fatigue. Complaint
symptoms have been reported up to 50-60%
(Kreiss, 1989).
Four out of 50 patients, examined by a medical
doctor, indicated office machines as the cause of
complaint (Terr, 1986). In a later review, including
additional 40 patients which also claimed “environ-
mental illness”, 19 had the office environment as
their workplace (Terr, 1989). It is striking that air-
way irritation and skin problems are more frequent
in the office environment (Wahlberg and Stenberg,
1991) relative to other non-industrial environments.
One ubiquitous symptom is the perception of dry
air despite relative humidity in the accepted range
20-60% (Eide et al., 1992). Sundell and Lindvall
(1993) considered this perception an important in-
dicator of increased risk of SBS prevalence.
The Danish town hall study showed that the use
of office machines, VDT work and handling of
paper was associated with eye and airway irritation
as well as with CNS related symptoms (Skov et al.,
1989) and in agreement with Sundell et al. (1994),
in particular with regard to photocopy machines as
a pollutant source. Similarly, other research groups
have found that handling of copying paper was as-
sociated with reported symptoms (Fisk et al., 1993;
Taylor et al., 1984) and Kjargaard and Brandt
(1993) found a weak association between photo-
copying and micro damage of the conjunctival epi-
thelium. There are only a few cases reporting symp-
toms related to the use of office equipment, like a
laser printer (Skoner et al., 1990), a photocopying
machine (Gallardo et al., 1994; Selner and Stau-
denmayer, 1985) and heat sensitive paper (Tencati
and Novey, 1983). The use of carbonless copy
paper (Buring and Hennekens, 1991) and VDT
work (Scansetti, 1984; Stenberg et al., 1993;
Wahlberg and Stenberg, 1991) have also been of
concern in some cases.
Fanger and his group (1988) found that the im-
mediately perceived air quality was decreased, 25%
by ETS and various activities, 13% by the users
themselves (bioeffluents), 42% by the building ma-
terials and 20% by the ventilation system. This im-
plied that the emission of pollutants from both the
building materials and the ventilation system is im-
portant and their impact on the IAQ may be greater
than that of bioeffluents from humans (Gunnarsen
and Fanger, 1992).
1.4 Determinationand Evaluation of
Indoor VOC Exposure
We experience in the office environment a variety of
different exposures. These are chemical, physical,
biological, and psychosocial. The removal rate of
VOCs is determined by the nature of ventilation
and ad- and desorption characteristics of materials
within a room and in addition to cleaning. Basically,
there are two major approaches for evaluation of the
exposure to chemicals in indoor air. These are 1)
measurements of VOCs in the indoor environment
combined with epidemiology, 2) human exposure
studies with VOCs, emissions from materials and
machines in climatic chambers, and in addition to
chemical, physical, sensory and biological emission
testing of building materials, products and equip-
ment in the laboratory.
It is important in this context to distinguish be-
tween the different purposes of indoor air sampling
and occupational hygiene sampling, respectively.
The latter should protect against adverse health ef-
fects. The purpose of indoor air sampling has ex-
panded to include emission testing for control of
IAQ and prevention of discomfort problems, such
as odor annoyance including eye and airway irri-
tation, in order to minimize SBS prevalence, in ad-
dition to exposure assessment, see Table 1.4.1.
1.5 Summary of Thesis Work
In view of the need for multidisciplinarity in indoor
air research, and in particular in the evaluation of
the possible link between VOC exposure and SBS
prevalence and deteriorated IAQ, the studies pre-
sented in this thesis had several goals.
These were:
To obtain information about VOC sources and
their emission characteristics (Chapter 2 and
studies 2, 3, 4, 5, 10).
To develop a method for VOC sampling and
analysis, to define sampling objectives and strate-
gies and to develop methods for identifymg emit-
ting VOC sources in the field in relation to alter-
native methods available (Chapter 3, studies 2
and 3).
To measure VOCs in city halls with a high samp-
 Peder Wolkoff: Volatile Orqonic Compounds 15

Table 1.4.1 Obiectives of indoor air sampling versus occupational hygiene air sampling

Objective Purpose
Indoor air sampling’ Control of IAQ and exposure assessment. Prevention of discomfort (e.g. odor an-
noyance) and eye and airway irritation (i.e. increased SBS prevalence)
Protection against adverse health effects
MateriaVequipment emission testing Development of healthier materials, better equipment and product control.
Exposure assessment by quantification of source strengths
Occupational hygiene air sampling Protection against adverse health effects. exuosure assessment
See also Table 3.3.2.

ling frequency and to review and relate the results
to other field studies (Chapter 4, study 3).
To develop methods for measuring the emission
of VOCs from building materials and office
equipment, to develop models describing the
emission rate over time, and to explore the use of
a bioassay as a potential emission test for airway
irritation. Finally, to relate chemical studies to
other methods of material testing (Chapter 5,
studies 1, 2, 5-7, 9, 10).
To study the impact of VOC emissions from
building materials and office equipment on per-
ceived IAQ, Additionally, to attempt to link VOC
exposure to physiological measures such as the
tear film quality and finally to relate these results
to other chamber studies including field studies
(Chapter 6, studies 5 and 8).
The major findings of the ten studies 1 to 10 are
shown below:
Study 1. First example of an animal bioassay applied
to a material used indoors: carbonless copy paper.
The results were compatible with reported symp-
toms and a large formaldehyde content of the copy
forms (Wolkoff et al., 1988).
Some guides for indoor VOC sampling are pre-
sented (Wolkoff, 1990b).
Study 4. VOCs and formaldehyde were monitored
in two new twin apartments (one vacant during the
measuring period) were monitored over a one year
period. VOC and formaldehyde concentrations are
discussed in terms of the influence of occupancy,
age, activity, and season. A guide for a “flushing
out” period prior to occupancy is proposed (Wol-
koff et al., 1991a).
Study 5. A combined multidisciplinary study with
subjects exposed to the emission of VOCs from
building materials. The VOC emission results are
discussed in terms of the immediate perceived air
quality in decipol, the tear film quality, and a mouse
bioassay. A proposed mechanism for eye irritation
is presented (Wolkoff et al., 1991b).
Study 6. The emission of VOCs from waterborne
paints has been measured in climatic chambers and
monitored over a one year period. A general prin-
ciple has been developed for ranking of building
materials with regard to their emission into the in-
door air environment (Clausen et al., 1991).

Study 2. Approaches for developing “healthy build-
ing materials” are presented and discussed. Three
cases are presented and discussed. Gas chromato-
graphy has been combined with a sniffing technique
to identify malodorous VOCs emitted from a build-
ing sealant. An example of comparing emission pro-
files of selected building materials with measured
room air (Wolkoff, 1990a).
Study 7. A portable, handy, and inexpensive field
and laboratory emission cell (FLEC) for the mea-
surement of VOC emissions from planar building
materials has been developed, tested and compared
with a small climatic chamber for repeatability and
reproducibility. The FLEC has been used in the
field on different surfaces and the results compared
with room air sampling (Wolkoff et al., 1991~).

Study 3. The experience of room air sampling of Study 8. Subjects have been exposed to a simulated
VOCs under high sampling frequency is discussed office environment in a climatic chamber and their
with reference i.a. to the Danish Town Hall study. reactions compared with air quality measurements.
16 Peder Wolkoff. Volatile Organic Compounds
The results showed that the subjects’ perception of
SBS symptoms was compatible with the decipol
evaluation and damage of the conjunctival epithe-
lium as the only clinical objective measure, despite
overall very low exposures (Wolkoff et al., 1992).
Study 9. To investigate the emission of VOCs from
office machines, their toner powders, and the pro-
cessed paper. It shows that processed paper emits
many different VOCs, due to toner powder emis-
sion, persistently for several days. The emissions
have been measured quantitatively and compared.
The emission profile has been determined for one
processed paper and modeling carried out (Wolkoff
et al., 1993a).
Study 10. Using the Field and Laboratory Emis-
sion Cell (FLEC) the emission processes of se-
lected VOCs from three pre-conditioned building
materials: a carpet, a waterborne paint, and a seal-
ant, have been identified by modeling of the emis-
sion profiles over time. One material, linoleum,
apparently had not reached a stable concentration
gradient in the material or oxidation may have oc-
curred to give good modeling (Wolkoff et al.,
1993b).
2. Sources of VOCs in the Indoor Environment
2.1 Introduction
The origin of VOCs is a plethora of various emis-
sion sources, each with its own emission characte-
ristics. There have been proposals to categorize
VOCs emitted to the indoor environment (Feron et
al., 1992; Miksch et al., 1982; Otson and Fellin,
1992; Rodes et al., 1991; Seifert and Ullrich, 1987;
Spengler, 1991). This overview differentiates be-
tween three emission source types categorized ac-
cording to their time emission profiles, see Scheme
2.1.1.
Generally, building related materials (Levin,
1989, 1992), including furniture and equipment
(Strobridge and Black, 1991), and consumer and
household related products (Knoppel and Schauen-
burg, 1989; Sack et al., 1992; Velvart, 1989; Walla-
ce et al., 1987b, 1991b), are major VOC sources.
Some sources may even dominate depending upon
spatial and temporal patterns, like human activities
(Clobes et al., 1992; Wallace et al., 1989; Wolkoff,
1987, 1990b), e.g. the use of office equipment
(Brooks and Davis, 1992). However, outdoor
sources may also contribute, depending on geo-
graphic location (Daisey et al., 1994; Ekberg,
1994). Two field investigations have indicated that
the two major sources of VOCs are the emissions of
building materials and human activities, approxi-
mately in a 1 : 1 ratio (Seifert et al., 1989a; Wolkoff
et al., 1991a).
The VOCs emitted from building materials may
originate from different types of pollutant sources.
Primary pollutant sources emit free (non-bound)
~
VOC sources indoors
Building related Human activity Outdoor related
related
building materials household and con- traffic, neigh-
ventilation, soil sumer products boring industry
humans, office
eauiDment
weeksjcontinuous minjhours hours
Scheme2.1.1 VOC sources indoors
VOCs. The primary pollutants, generally, are low
molecular weight VOCs, such as solvent residues,
additives and unreacted raw materials, e.g. mono-
mers. Secondary pollutants are chemically or phys-
ically bound VOCs, but a number of VOCs are
emitted or formed by several different reactions, see
Scheme 2.1.2. Emission by hydrolytic decompo-
sition is known, other examples are oxidative degra-
dation and reemission of adsorbed VOCs (sink ef-
fect).
2.2 Building Materials (interior use)
Table 2.2.1 lists selected examples of building ma-
terial related contributions of VOCs. The materials
emit a variety of different VOC classes found in
emission testing and field investigations.
Common to these is the time of emission decay.
Eventually, they will reach a “quasi steady” emission
rate for VOCs and SVOCs in new buildings, within
weeks to months (Berglund et al., 1982a, 1988;
Rothweiler et al., 1993; Seifert et al., 1989a; Wolk-
off et al., 199la) or even a year (Farant et al., 1992).
Renovation (new wallpaper and paint) in a tele-
phone switching office raised the TVOC level by a
factor three, but it returned to normal level within
four months (Shields and Weschler, 1992). The
perceived air quality has also been shown to de-
crease for 6-8 months after renovation of offices
(Gunnarsen and Valbjsrn, 1993). The emission de-
cay varies greatly for different material types, and it
may, for some materials, continue for more than a
year, e.g. waterborne paints (Clausen et al., 1991).
Wallace et al. (1987~)have measured average half-
lives of certain VOCs in new buildings to be from
2-8 weeks which is in essential agreement with a
study by Mslhave et al. (1986a). After the initial
equilibrium time usually other phenomena such as
oxidative degradation (Jensen et al., 1994; Weschler
et al., 1990a, 1992; Wolkoff et al., 1991a) and ad-
and desorption effects may take over (Berglund et
al., 1989; Miksch et al., 1982; Seifert and Schmall,
1987; Tichenor, 1992). The time scale of emission
from these sources is in the range from weeks to
continuous.
18 Peder Wolkoff: Volatile Organic Compounds

Type of VOCs sources Source material Mechanism of emission

dry
VOC free
as solvent, monomer,
reaction product, additive
VOCs chemically bound
Different formations of VOCs
VOCs physically bound
Scheme 2.1.2 Type of VOC sources indoors
wet
+ + Evaporation, Diffusion
+ Decomposition (hydrolysis), Acidity or basicity in material
Action of cleaning
Mechanical wear and maintenance, Humidity (microbiological
(MVOCs))
Oxidative degradation and chain scission
Ad- and desorption processes

Table 2.2.1 Selected examples of VOC sources - Building related materials (for indoor use]

Source References Typical VOCs emittedmeasured

Emission testing Field measurement
Adhesive 1, 2 C&, alkanes, toluene, styrene
Building elevator 3 C 3-C alkanes
Floor materials:
Carpets 4, 6-9, 11, 14-18 5, 10, 12, 13 C,-C6-alkyl aromatics, styrenes, 4-phenylcyclo-
hexene, vinylcyclohexene, 2-ethylhexanol, siloxan-
es, amines,
Cork 19 1,2-propandiol
Linoleum 6, 8, 19-21 16, 24 C5-C1, aldehydes, aliphatic acids, benzaldehyde
Parquet (wood) 19, 21 C5-C6 aldehydes, terpenes
Rubber 8, 17 Acetophenone, alkyl-aromatics, styrenes
Vinyl (pvc) 8, 22-25 Alkanes, aromatics, 2-ethyl-1-hexanol, glycol
esters, TXiB
Gvpsum board 8, 26 Diacid esters
Particle board 4, 17, 26-27 Alkanes, aldehydes, butanol, formaldehyde,
ketones
Sealandcaulk 5 , 7, 16, 27 16, 28 Ketones, esters, glycols, polychlorinated
biphenyls, siloxanes

Surface filmWall material:

Lacquer 26 Alkanes, aldehydes
Paint 7, 8, 16, 17, 21, 26-27, 29-34 Alkanes, glycols, glycol esters, Texanol
Varnish 8, 27 Alkanes, aromatics
Thermal insulation 35-36 35 Aldehydes, ketones, aromatics
Textileidrapery 37 Acetone, ethyl acetate, methylfuran, thiophene,
dimethvl disulfide
VaDor barrier 38 Naphthalenes
Ventilation system 39-4 1 Broad VOC spectrum
Wall paper 8, 21, 42 33 Hexanal, terpenes
References: 1) Girman et al., 1986. 2) Person et al., 1991. 3) Weschler et al., 1990b. 4) Black et al., 1991. 5) Davidson et al.,
1991. 6) Hodgson et al., 1993. 7) Miksch et al., 1982. 8) M~lhave,1982. 9) Pleil and Whiton, 1990. 10) Rathweiler et al.,
1992a. 11) Schroder, 1989. 12) Seifert et al., 1989b. 13) Singhvi et al., 1990. 14) Sollinger et al., 1994. 15) Wallace et al.,
1987b. 16) Wolkoff, 1990a. 17) Wolkoff et al., 1991a. 18) Wolkoff and Nielsen, 1993. 19) Saarela and Sandell, 1991. 20) Jensen
et al., 1995a. 21) Wolkoff et al., 1991b. 22) Kiselev et al., 1983. 23) Saarela et al., 1989. 24) Rittfeldt, 1991. 25) Wolkoff et al.,
1991c. 26) Colombo et al., 1990. 27) Tichenor and Mason, 1988. 28) Benthe et al., 1992. 29) Brown et al., 1990a. 30) Hansen
et al., 1987. 31) Clausen et al., 1991. 32) D e Bortoli et al., 1985. 33) Shields and Weschler, 1992. 34) Ullrich et al., 1982. 3 5 )
Van der Wal et al., 1989. 36) Krzymien, 1989. 37) Bayer and Black, 1988. 38) Brown et al., 1990b. 39) Berglund et al., 1988.
40) Cohen et al., 1989. 41) Lundin, 1991. 42) D e Bortoli et al., 1993
 Peder Wolkoff Volatile O r g a n i c Compounds 19

Table 2.3.1.1 Selected examples of VOC sources - human activity related emissions

Source References
Emission testing Field measurement 'OCs emitted/measured
~ ~ ~~

Correction fluid 3 Chlorinated hydrocarbons

Dish washing 4 Ethanol
Driving 5 ~
Aromatics
~ ~~ ~

Dry cleaning (visit) 5, 6 Chlorinated hydrocarbons (e.g. tetrachloro-

ethylene)

Householdiconsumer products 4, 7, 8-14 3, 5 A variety of different nonpolar and polar VOCs, in-
cluding fragrances. One study identified 84 VOCS.~
Human activities 3, 5, 6, 15-19 A variety of different VOCs
Human emissions 21, 23 20,22 Ethanol, methanol, acetone, butyric acid, isoprene,
toluene
~ ~

Job related activities 5 Chlorinated hydrocarbons

Painting 24 3, 5, 19, 24-26 Alkanes, glycols, glycol ethers, Texan01
Personal care products 14, 27 Siloxanes, oxygenates (fragrances)
Photocopying See Table 2.3.2.1
Renovation (painting) 28 Aromatics, glycols, glycol ethers and acetates, acids
Room freshener 11, 14, 25 5, 10 Alkanes, limonene, fragrances
Shampoo 3 Ethylene glycol butylether
Showering 29, 30 Chlorinated hydrocarbons
Social activities 18, 19 Ethanol, TVOC, terpenes, dodecane
Tobacco smoke (ETS) 5, 31-37 Aliphatic hydrocarbons, aldehydes
(+formaldehyde, acrolein), benzene, styrene,
3-vinylpyridine, 2- and 3-picolines
Wadpolish 9, 11, 25 A variety of different VOCs
References: 1) Ong et al., 1993. 2) Girman et al., 1993. 3) Seifert et al., 1989a. 4) Wooley et al., 1990. 5) Wallace et al., 1989.
6) Kawauchi and Nishiyama, 1989. 7) Bayer et al., 1988. 8) De Bortoli et al., 1985. 9) Knoppel and Schauenburg, 1989. 10)
Pled et al., 1989. 11) Person et al., 1991. 12) Sack et al., 1992. 13) Wallace et al., 1987b. 14) Wallace et al., 1991b. 15) Farant
et al., 1992. 16) Hodgson, 1992. 17) Lebret et al., 1986. 18) Wolkoff, 1990b. 19) Wolkoff et al., 1991a. 20) Cailleux et al., 1993.
21) Ellin et al., 1974. 22) Wang, 1975. 23) Sastry et al., 1980. 24) Hansen et al., 1987. 25) Tichenor and Mason, 1988. 26)
Shields and Weschler, 1992. 27) Shields and Weschler, 1992. 28) Rothweiler et al., 1993. 29) McKone, 1987. 30) Pleil et al.,
1989. 31) Ayer and Yeager, 1982. 32) Barrefors and Petersson, 1993. 33) Heavner et al., 1995. 34) Lofroth et al., 1989. 35)
Proctor et al., 1991. 36) Schlitt and Knoppel, 1989. 37) Wallace et a]., 1987d, 1989

pointed out that the human activity related sources

2.3 Human Activity
2.3.1 General Activity
Table 2.3.1.1 lists selected examples of human ac-
tivity related contributions of VOCs. These activi-
ties show an even greater variety of different VOC
classes than emissions &om building materials. Oc-
cupant activities in the office environment might in-
clude paper handling, photocopying and laser print-
ing, in addition to bioeffluents and ETS (see 2.3.2).
The effect of the exposure will especially be im-
portant at locations with a low air exchange rate
and, in particular, low ventilation efficiency, and,
sources of high emission rate. Rodes et al. (1991)
may be regarded as point sources and are closely
located to occupants, forming spatial and temporal
concentration patterns. Considering the convec-
tions around the body (Breum et al., 1990) includ-
ing human bioeffluents, this implies that the con-
centration in the breathing zone may be greater than
in the center of the room, where samples usually
have been taken.
Many of the listed emissions occur within min-
utes and hours depending on the number of per-
sons present in the room (Johansson, 1978) and on
ongoing activities (Hodgson, 1992; Wolkoff,
1990b). These are typical office work, e.g. photo-
20 Peder Wolkoff. Volatile Organic Compounds
-

copying work (Grot et al., 1991), including smoking
which occurs within minutes. Some activities may
result in a long-term emission like painting
(Clausen et al., 1991; Wolkoff et al., 1991a). The
emission of siloxanes from the use of personal care
products (Shields and Weschler, 1992) may also
add considerably and so does the use of fragrances
(Wolkoff, 1992b; Wolkoff et al., 1992). Even if the
activity is brief, the VOCs emitted can be adsorbed
to other materials (fleecy surfaces) (Tichenor,
1992) and dust particles (Wolkoff and Wilkins,
1994) and be reemitted at later stages depending
on the climatic conditions (Nielsen, 1988). Delayed
peak concentrations have been shown to occur after
cleaning activities (Gibson et al., 1991; Vejrup and
Wolkoff, 1994). An alternative exposure pathway
could be skin adsorption, e.g. halogenated hydro-
carbons from showering (Szejnwald Brown et al.,
1984).
2.3.2 Activities in the Office Environment
Only limited information is available on VOCs
emitted from office machines (Brooks and Davis,
1992; mksch et al., 1982; Sonnino et al., 1983;
Wolkoff et al., 1992, 1993a), see Table 2.3.2.1. The
emission of VOCs from wet photocopying machines
is encountered only in North America (Daisey et
al., 1994; Grot et al., 1991; Tsuchiya, 1988; Tsu-
chiya and Stewart, 1990; Walkinshaw et al., 1987).
Thirty-one VOCs with a wide range of volatility and
persistence were identified from processed paper
from photocopying machines, laser and matrix
printers (Wolkoff et al., 1993a). Several of the emit-
ted VOCs can be characterized as odorous (e.g.,
styrene and acrylates) or contact allergens (e.g.,
acrylates and azo-bis-isobutyronitrile) . The emis-
sion of other pollutants, from photocopying and
laser printer equipment, such as ozone and par-
ticles, however, has received much more attention
(Allen et al., 1978; Eggert et al., 1990; Bruun-
Hansen and Andersen, 1986; Olander, 1992). One
study has indicated that the formation of formalde-
hyde from office machines may be significant (Wol-
koff et al., 1992) and is possibly formed by reactions
of VOCs with ozone (see Table 2.5.2). The han-
dling of carbonless copy paper is another potential
VOC source (Norback et al., 1988; Wolkoff et al.,
1988) which has been found to be associated with
SBS symptoms jointly with photocopying and VDT
work (Skov et al., 1989; see also Fisk et al., 1993;

Table 2.3.2.1 list of pollutants emitted from office machines and other office equipment

Sourceref VOCs Particles Ozone Formal- Nitrogen Others

dehvde oxides
~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~

Photocopying machines - + +3,5 + + + Toner powder2, Fuser oil

dry'-*, wet9-14 Photoconducting material
Laser printer^*,'^-'^ + + + + +
Jet+matrix printer^'^ + N o information
ComputersNDTZ + (+I No information Fire retardant2
Carbonless copy paper's,19 + + (+I Color, Developer, Biocide, Capsule
material
Carbon paper + + No information
Human activities Table
2.3.1.1
Paper after p r o ~ e s s i n g ' ~ + + No information
Paper +
Cleaning agents4, 2o + Solvent, Surfactant,
Correcting + Reactant
Office furniturez4 + No information
Power cablesz5 +
Work stationz4 +
References: 1) Allen et al., 1978. 2) Brooks and Davis, 1992. 3) Bruun Hansen and Andersen, 1986. 4) Miksch et al., 1982. 5)
Schnell et al., 1992. 6 ) Selway et al., 1980. 7) Sonnino et al., 1983. 8) Wolkoff et al., 1992. 9) Daisey et al., 1994. 10) Grot et
al., 1991. 11) Hodgson et al., 1991a. 12) Tsuchiya, 1988. 13) Tsuchiya and Stewart, 1990. 14) Walkinshaw et al., 1987. 15)
Eggert et al., 1990. 16) Olander, 1992. 17) Wolkoff et al., 1993a. 18) Norback et al., 1988. 19) Wolkoff et al., 1988. 20) Wallace
et al., 198713. 21) Girman et al., 1993. 22) Ong et al., 1993. 23) Seifert et al., 1989a. 24) Strobridge and Black, 1991. 25) Shields
and Weschler, 1992
 Peder Wolkoff: Volatile Orqanic Compounds 21

Stenberg et al., 1993; Sundell et al., 1994; Taylor
et al., 1984).
Building materials in new buildings appear to be
the dominating primary pollutant sources for up to
about 12 months, see section 2.2, relative to other
sources. The emission decline depends on their
emission characteristics (Seifert and Ullrich, 1987).
The use of office equipment, such as printers, pho-
tocopying machines, in addition to the emission
fiom processed paper (Wolkoff et al., 1993a) and
cleaning and maintenance provide daily contri-
butions of pollutants. These daily periodic sources
have been proposed to cause malfunctioning of
electronic equipment (Shields and Weschler, 1992).
fungal VOCs. Norback et al. (1993) detected 2-
ethylhexanol and l-octen-3-01, respectively, in
about 33% of bedrooms and in personal samples in
39 homes. Strom et al. (1994) found elevated total
concentrations of MVOCs in buildings with odor
problems compared with reference buildings.
Cultivation studies of indoor microorganisms in-
dicate that the VOC formation i.a. depends on the
microbial strain, but the substrate composition ap-
pears to be even more important than incubation
time and microbial growth rates (Bjurman, 1993;
Rwers et al., 1992). The water activity within the
attacked object, rather than the relative humidity, is
another important factor determining the growth
rate (Flannigan, 1992).

2.4 Microorganisms(MVOCs)
Table 2.4.1 lists some examples of VOCs which are
believed to be formed microbiologically (MVOCs).
However, some of them may also have originated
fiom material decomposition (e.g. hydrolysis). Al-
cohols, in particular ethanol and ketones are major
MVOCs. A common trend is the formation of
branched aldehydes and 2-ketones, VOCs which
have also been identified in household and city hall
dust (Wilkins et al., 1993; Wolkoff and Wilkins,
1994). Several of the MVOCs found have very low
odor thresholds, e.g. geosmin (Hyppel, 1984;
Strom et al., 1994), unsaturated alcohols and alde-
hydes. Miller et al. (1988) found 3-methyl-l-buta-
no1 in 44% houses investigated for presence of
2.5 Outdoor Air and Indoor Air
Chemistry
One of the major outdoor sources is motor vehicle
emissions from the traffic. The VOCs are, generally,
alkanes and aromatics, see Table 2.5.1. Their entry
into living and workmg areas is often by infiltration
from an attached building like a print shop, garage
or crawl space. The contribution of aromatics and
alkanes &om motor vehicles in 12 California office
buildings has been measured to range from 70-90%
(Daisey et al., 1994). The contributions apparently
will depend strongly on the building characteristics
(Harrje, 1991) and on the outer climatic conditions
(Field et al., 1992). For example, Pleil et al. (1989)

Table 2.4.1 Some examples of VOCs (MVOCs)of microbiological origin in indoor ail

Sourceref Typical VOCs eminedmeasured

Human subjects' Ethanol, propanol, isobutanol, 3-methyl-l-butanol, 2-methyl-1 -propanol, esters,
2-ketones, dimethyl disulfide
HVAC unit' Geosmin (1,l O-dimethyl-trans-9-decalol)
Mold cultivation3 Various branched alcohols, branched alkenes, branched aldehydes
Mold cultivation4 2-methyl-l-propanol, 3-methyl-l-butanol, l-uentanol, 1-octen-3-01, 3-octanol
Mold cultivation5 (field study) l-butoxy-2-propanol, 2-butoxy ethanol, 2,7-dimethyl-3,5-octadiene,C 12-, C , ,-alkanes,
2-methyl-propionic butyl ester
Mold cultivation6 C z , C4-C,-alcohols, acetone, butanone, Cs-C7-aldehydes, benzaldehyde, phenol, indole,
methyl mercaptan, dimethyl di- and trisulfide
Thermal insulation materials7 Terpenes, phenylacetaldehyde, acetophenone, octanoic acid
Fiberglass' Benzene, 2-ethylhexanol
Field s t ~ d i e s ~ ~ ' ~ 2-ethylhexanol, 3-octanol, l-octen-3-01, 2-octen-1-01, geosmin, 2-methy1-iso-borneo1,
2-isopropyl-3-methoxypyrazine
References: 1) Cailleux et al., 1992; see also Ellin et al., 1974. 2) Hyppel, 1984. 3 ) Batterman et al., 1991. 4) Larsen and Frisvad,
1994. 5) McJilton et al., 1990. 6) Rivers et al., 1992. 7) Bjurman, 1993 (see also Van der Wal et al., 1989 in Table 2.6.1). 8)
Ezeonu et al., 1994. 9) Norback et al., 1993. 10) Strom et al., 1994
22 Peder Wolkoff Volatile Organic Compounds
Table 2.5.1 Selected examples of outdoor related VOC contri
butions
Sourceref Typical VOCs
Neighboring industry’,’ Aromatics, acetates,
ketones
Bitumen ulant3 Dimethvl disulfide
Polluted soil4, Gas station5, Alkanes, alkanes
Attached garage6-’’, Crawl (branched), aromatics,
space”, Elevator system”, Motor chlorinated aromatics
vehicle^'^-'^, Outdor air15
References: 1, 2) Verhoeff et al., 1987, 1988. 3) Scherer et al.,
1993. 4) IUiest et al., 1989. 5) Kullman and Hill, 1990. 6 )
Cohen et al., 1989. 7) Gammage and Matthews, 1988. 8)
Hawthorne et al., 1986. 9) Weisel and Lawryk, 1993. 10)
Hodgson et al., 1991a. 11) Wolkoff et al., 1991a. 12) Weschler
et al. 1990b. 13) Pleil et al., 1989. 14) Daisey et al., 1994. 15)
Lewis, 1991
found an increase of benzene and toluene with the
ventilation on, while the concentration of halocar-
bons increased, when the ventilation was off indi-
cating local sources. Similarly, Nagda et al. (1991)
found that TVOC was substantially higher at high
ventilation rate during summer time (the outdoor
level was also high).
Few studies have dealt with VOCs formed by oxi-
dation processes, i.e., autoxidation and reactions
with ozone and nitrate radicals. E.g., hexanal and
other aliphatic aldehydes have been reported to be
emitted from paints and paint resins after curing
(De Bortoli et al., 1985; Ullrich et al., 1982; Young,
1992). These aldehydes are very likely formed by
autoxidation processes. The exposure of carpet
emissions to ozone showed an increase of aldehyde
formation and TVOC (Weshler and Hodgson,
1992), while a marked increase of formaldehyde has
been found in a simulated office environment study
with ozone emitting machines (Wolkoff et al.,
1992). The aldehyde formation may arise, i.a., from
degradation of long-chain fatty acids in resins and
linoleum (Jensen et al., 1994, 1995a). Wolkoff et
al. (1991a) observed an increase of hexanal in an
inhabited apartment during the warm season. Some
VOCs formed by oxidative processes are listed in
Table 2.5.2. There are indications that atmospheric
(indoor air) chemistry, e.g. reflected in an increase
of aldehydes (Zhang et al., 1994a,b), may be im-
portant for understanding increased SBS prevalence
and loss of TVOC from intake to exhaust air (Sun-
dell et al., 1993). The formaldehyde yield from re-
actions of limonene and styrene, respectively, with
ozone was found to be from 125 to 150% molar
Table 2.5.2 Some examples of secondary VOCs formed by 0 x 1
dation
Precursor VOC VOCs formed by oxidation
Limonene Formaldehyde, 4-acetyl-1-methyl-
cyclohexene, cyclohexanone’,
formic and acetic acidzb
a-Pinene 6-methyl-5-heptene-2-one3
p-Pinene Formaldehyde, acetone,
cyclohexanone, nopinone’
Styrene Formaldehyde, benzaldeh~de’~.~
Un- and sat. hydro- Aldehydesza
carbons, fatty acids
Vinyl cyclohexene Formaldehyde and formic acid2b
References: 1) Grosjean et al., 1993. 2a, b) Zhang et al.,
1994a, b. 3) Cicclioli et al., 1992. 4) Tuazon et al., 1993
equivalents (Zhang et al., 1994b). The reported for-
mation of 6-methyl-5-heptene-2-one identified in
vacuum cleaner dust (Wolkoff and Wilkins, 1994;
Wilkins et al., 1993) is compatible with oxidation of
a-pinene (Ciccioli et al., 1992).
Reactions of other terpenes with ozone result in
formaldehyde and various ketones, see Table 2.5.2.
2.6 VOCs Reportedto Have Caused
IAQ Problems
Table 2.6.1 summarizes selected cases where VOCs
have been suspected to partially have caused some
discomfort, however, questionnaires have rarely
been used. The dominant symptoms reported have
been mucous membrane irritation and odor anno-
yance. A classical example is the emission of ali-
phatic amines, diamines and sulfides, including am-
monia fiom casein containing self-leveling mortar
on wet concrete (Karlsson et al., 1989; Lundholm
et al., 1990). Some VOCs have low irritation thresh-
olds such as aliphatic acids and amines, or may be
allergenic like shampqo constituents (Taylor and
Hindson, 1982). The VOCs may be (ma1)odorous
with low odor thresholds, like sulphur containing
VOCs from polysulfide based sealants (Wolkoff,
1990a) and 4-phenylcyclohexene from latex based
carpets (Hodgson et al., 1993). The VOCs emitted
are solvent residues, additives, and reactants from
the raw materials, decomposition products, which
are formed during the hardening processes and fi-
nally secondary pollutants caused by hydrolysis reac-
tions (e.g. plasticizers) or by microbiological action.
There are few intervention studies directly related
 Peder Wolkoff Volatile Organic Compounds 23

Table 2.6.1 Selected examples of VOC sources reported to have caused IAQ problems

Source References Typical VOCs emittedmeasured

Emission Field reported, o=odor annoyance, m=mucous membrane irritation
testing measurement
Carbonless copy paper 1 1 Mono-isopropylbiphenylm
Carvet 2 2 2-Ethvlhexanol, stvrene, 4-phenylcyclohexene"~'
Elevator 3 Alkanes
Fluorescent lighting fixture 4 Volatilized asphalt"
Freshlv oainted radiator 5 Hexanal, hexanoic acid","
~ ~~

Gas station 6 Petrol'

Linoleum 7-9 8 Aliphatic acids (C3-C6) and aldehydes (C,-C9)"
Microorganisms 10 MVOCs", see Table 2.4.1
Painted wooden frame 8 8 White spirit"'
Plastic flooring (pvc) 11 2-Ethylhexanol
Plant (bitumen) 12 Dimethvl disulfide"
Printing shop 13 Solvents'
Roof insulation (rubber) 11 Benzothiazole
Sealant in theater 8 1,2,5-Trithiepan, divinyl disulfide"
Self-leveling mortar 14-16 Aliphatic amines, diamines, and sulfides, " a m r n ~ n i a " '","
~
Shampoo 17, 18 Ally1 phenoxyacetate'', (sodium dodecyl sulphate")"
Thermal insulation material 20 20 Aromatics, aliphatic aldehydes, ketones
Wall-to-wall carpet 21 Aliphatic alcohols (C7-C9)'
References: 1) Norback et al., 1988. 2) Seifert et al., 1989b. 3) Weschler et al., 1990b. 4) Tavris et al., 1984. 5) Ullrich et al.,
1982. 6) Kullman and Hill, 1990. 7) Saarela and Sandell, 1991. 8) Wolkoff, 1990a. 9) Wolkoff et al., 1995. 10) Strom et al.,
1994. 11) Anderson et al., 1993a. 12) Scherer et al., 1993. 13) Verhoeff et al., 1987. 14) Karlsson et al., 1989. 15) Lundholm
et al., 1990. 16) Saarela, 1992. 17) Kreiss et al., 1982. 18) Taylor and Hindson, 1982. 19) Non-volatile surfactant. 20) Van der
Wal et al., 1989. 21) McLaughlin and Aigner, 1990

to building materials and their emission of VOCs.
In a longitudinal intervention study, the removal of
wall-to-wall carpets in schools resulted in a decrease
of reported SBS symptoms relative to a group not
exposed to carpets (Norback and Torgen, 1989).
The carpets were 8-10 years old, any VOC emis-
sion should have been low (decomposition or
MVOCs), and other pollutants, e.g. mites and
mold, may have been removed also.
2.7 Emission Rate
Most reported VOC emission rates (mass emitted
per area and time)) are based on one measurement,
usually the supposed "steady state" concentration
(Levin, 1992). From a practical viewpoint, emission
rate constants are preferable for purposes of
modeling emission profiles over time, e.g. in a stan-
dard room (Wolkoff and Nielsen, 1995). Reported
emission rates, usually obtained from "steady state"
measurements, are in the order of a few pg/(m2Xh)
to mg/(m2xh) (Black et al., 1991; Colombo et al.,
1990; Davidson et al., 1991; Miksch et al., 1982;
Merlhave, 1982; Saarela and Sandell, 1991; Strob-
ridge and Black, 1991; Wallace et al., 1987b). The
source strength in a room is obtained by multiplying
the material area with its emission rate. Many fac-
tors can influence the emission rate, like tempera-
ture, to a less extent the relative humidity and the
material age, for further discussion, see Chapter 5.
Body effluent emissions have been determined to
be about 0.2-0.3 mg/h per kg body weight
(Merlhave et al., 1995), in agreement with the clas-
sic study by Wang (1975). Isoprene appears to be a
major body VOC with an emission ca. 300400 pg/
h (Ellin et al., 1974). Lewis and Zweidinger (1992)
24 Peder Wolkoff Volatile Organic Compounds
estimated aldehyde emission rates to 9.4 m g h and
other non-methane TVOC to 100 mg/h in resi-
dences.
2.8 Pollutant Source Dynamics
The total indoor air pollution of VOCs comprises
the combined contributions from the building re-
lated, human activity related and outdoor sources.
Each pollutant source has its own emission charac-
teristic, i.e. temporal emission and spatial patterns.
Figure 2.8.1 shows the decline of the coalescent
agent Texanol, used in a waterborne paint, in a new
apartment over a one year period from the time of
completion (Wolkoff et al., 1991a). Several research
groups have suggested schemes to describe the vari-
ability of different emission sources. Seifert and
Ullrich (1987) distinguished between continuous
and discontinuous emission sources. These emis-
sions may further be subdivided into those behaving
in a regular or irregular mode as shown below in
Scheme 2.8.1. The time scale of the continuous
type was in the order of months or weeks while it
proceeded within hours or minutes for the discon-
tinuous type. Others distinguish between short and
long term temporal variations including spatial vari-
ations (Otson and Fellin, 1992) while Miksch et al.,
lg.m'3
4000n
Texanol
Texanol'
Ethanol'
Fig. 2.8.1 Average time/concentration profiles of long-term VOC
sampling (7-14 days) of acetone, ethanol, and Texanol in Danish
Twin Apartments (occupied and vacant). Date 0 (dote of building
completion) = 1 November 1987. * =occupied. J=Date of oc-
cupancy ?=20]une 1988 (Wolkoffetal., 1991a)
Regular (constant emission rate)
Continuous C Source:
7 Irregular (variable emission rate)
Pollutant
L Regular (constant time pattern)
Discontinuous C Distributed
Irregular (variable time pattern)
Scheme 2.8.1 Seiferi and Ullricli scheme [ 1987)
(1982) presented a simple model with three emis-
sion types such as constant generation, workday
generation and episodic generation. By combining
the temporal patterns with the spatial patterns Levin
(1992) ended up with a two-by-three matrix, see
Scheme 2.8.2, in which he distinguished between
point sources and distributed sources each having
constant, periodic (occupational) and episodic time
patterns.
The concentration-time pattern of VOCs in the of-
fice environment with activities may vary signifi-
cantly during the working hours and depends upon
a series of interrelated factors such as location, oc-
cupant density and user related activity (Crump and
Madany, 1993; Ekberg, 1994; Hodgson, 1992;
Johansson, 1978; Wolkoff, 1990b). This also in-
cludes photocopying (Daisey et al., 1994; Grot et
al., 1989; Hodgson et al., 1991a) and the use of
personal care products (Shields and Fleischer,
1993). The temperature, humidity, ad- and desorp-
tion processes (Borrazzo et al., 1993) and outside
activities (Ekberg, 1994; Pleil et al., 1989) can also
contribute. On a long-term basis, the primary
VOCs from building materials will dominate during
the first year in a new building. The contribution
from daily activities (e.g. office machines and other
human activities) and secondary pollutant sources
will progressively dominate the indoor air. This
could be one explanation for the identified associa-
I tion between use of photocopying machines and
SBS prevalence (e.g., Sundell et al., 1994). How-
ever, SBS has not been found to be associated with
the use of computers (Fisk et al., 1993).
The impact of the ad- and desorption processes
could be reflected in a typical office in which emit-
ted pollutants from human activities during the
workday are adsorbed on fleecy surfaces (textiles)
and shelves (paper). During the night, while the
ventilation system is turned off, and over time, the
equilibrium between VOCs in the air and sorbed
VOCs is reestablished, with a resulting increase in
air concentration which the occupants will be ex-
posed to the next morning. Conversely, if the
Constant Periodic Episodic
Point + Room Photocopying, Hobby
freshener paper handling activity
+ Carpets Smoking Painting
Scheme 2.8.2 Levin scheme I1992)

W A C system is turned on overnight with heating
the VOCs could be removed (Nielsen, 1988). The
association between the fleece factor (Nielsen,
1987) and increased SBS prevalence Uaakkola et
al., 1994), however, has not been found in two
other studies (Zweers et al., 1992; Sundell et al.,
1994).
The building characteristics (Harrje, 199l), i.e.
different ventilation conditions and wind direction
may also play an important role and add to the vari-
ability and temporality of indoor pollutants. Wesch-
ler et al. (1990a, 1992) found that indoor ozone
concentrations may vary greatly with the time of the
day and this may affect the types and concentrations
of VOCs found indoors (Weschler and Hodgson,
1992). Generally, TVOC levels have been found to
be inversely proportional to the air exchange rate,
i.e. concentrations increased when ventilation was
Peder Wolkoff Volatile Organic Compounds 25
reduced (e.g., Grot et al., 1991; Shields and
Weschler, 1992; Turiel et al., 1983). It was shown
in the Danish town hall study that the office size
and occupant density were important parameters
associated with increased SBS prevalence (Skov et
al., 1990). This may lead to the conclusion that lo-
cal pollutant sources (e.g. work stations, human ac-
tivities including bioeffluents) may play a more im-
portant role than ventilation (Farant et al., 1992;
Hodgson, 1992; Nagda et al., 1991).
The overall source dynamics of VOCs indoors
are reflected in the variability expressed by the fol-
lowing: the plethora of source types and their
emission characteristics as temporal and spatial
patterns; the concentration ranges encountered in-
doors. It is important to realize that the sampling
strategies should be related to these dynamics (cf.
Chapter 3).
3. Sampling Strategy and Methods of Sampling,
Analysis and Source Identification
3.1 Sampling overview
Sampling of indoor VOCs has three main purposes.
First, it is to measure time integrated mean concen-
trations for exposure assessment according to a de-
fined sampling objective, second, to carry out
source identification and third, to characterize
building materials and products according to their
emission profiles.
Both field air sampling and emission testing re-
quire a choice of sampling technique and method
for analysis. In addition, field sampling requires
consideration of sampling objective, data quality ob-
jective and a sampling strategy. Source characteriza-
tion by emission testing has to be conducted under
controlled environmental conditions, usually in a
climatic chamber (see Chapter 5).
The VOC measurement should end with inter-
pretation and evaluation of the potential impact on
IAQ and human health, e.g. in terms of odor an-
noyance and mucous membrane irritation.
Selection of the best sampling method will de-
pend on the nature of the potential VOCs of inter-
est, environmental conditions and the sampling ob-
jective.
The method of choice for analyzing VOCs de-
pends on the criteria of sensitivity and selectivity
and the time resolution required for sampling ac-
cording to the sampling objective. No single
method allows for sampling of the whole range of
volatile organics. There are several sampling tech-
niques available. These are continuous sampling,
grab sampling, active sampling and diffusive sam-
pling (Knoppel, 1992a,b; Wallace, 1991). Except
for continuous sampling, the remaining methods
all can include identification of single VOCs pres-
ent. Sampling integrates concentration over time
which may be short, requiring high analytical sen-
sitivity or long providing a long-term average con-
centration over time. The most common methods,
their advantages and disadvantages are summar-
ized in Table 3.3.1.
3.2 Sampling Strategy
A series of questions are prerequisite which allow a
resolution of the scientific hypothesis. The first and
second questions are: What is the hypothesis and
what is the sampling strategy that is needed to test
the hypothesis. This leads to the following questions
about strategy: Why measure; What to measure;
How to measure; When to measure; Where to
measure; How often to measure (sampling fre-
quency); and How long to measure (sampling dur-
ation). As a rule of thumb, short-term samples
monitoring peak concentrations may be related to
acute events of symptoms, while long-term meas-
urements expressing a mean time-integrated con-
centration could be associated with chronic effects
(ECA, 1989b).
The procedure for field air sampling for analysis
and identification of VOCs entails five steps: 1) Defi-
nition of the sampling objective(s) (McCharty et al.,
1991; ECA, 1989b; Thorsen and Mdhave, 1987;
Wolkoff, 1990b), 2) definition of the data quality ob-
jective (Keith, 1990), 3) design of the sampling strat-
egy including the selection of microenvironment
(ECA, 1989b, 1994), 4) choice of sampling tech-
nique and specificity, transport and storage prop-
erties and finally 5) the analysis, see Table 3.3.2. Al-
though sampling strategy is a well-known concept in
occupational hygiene, the sampling strategy of an in-
door environment must, in addition, be based on a
careful definition of the sampling objective with due
consideration of all IAQ parameters and their poss-
ible interrelationships (ECA, 1989b). Finally, the
sources dynamics (Weschler and Hodgson, 1992;
Wolkoff, 1992a) and building characteristics, includ-
ing the environmental conditions before and during
sampling should be considered.
The fundamental rule still is that the sampling
must be carried out according to the sampling ob-
jective. For example, in complaint cases the time of
sampling and sampling duration should fit with the
complaint event.
Table 3.3.1 Sampling techniques for measuring V V O C s , V O C s and some S V O C s i n indoor air

Sampling techniqueref Advantage Disadvantage Time resolution Method Exposure type

minimum p = personal sampling
sampling time
Continuous 'J Easy-to-use, Non-selective <1 min FID, PID3, FT/IR4, photo- peak
High time resolution acoustic detector5 activity related
mean
"Selective" Ion Trap MS6
Grab s a m p l i n g ' ~ 2 ~ 7 - 1 1 Repeated analysis, Preconcentration required, min +h Canister, direct injection and peak
(canistertflow restrictor) No breakthrough, Adsorption of polar VOCs, HRGC/MS mean
Time representativeness Sensitivity, or
Water vapor problem preconcentration and
TD/HRGC/MS
Active sampling: Peak conc. monitored, Only one sample run, <30 min-h Pumped sampling and peak
Thermal d e s ~ r p t i o n ' ~ ~ , * ~ . ' ~ -Sensitivity,
'' Blank build-up values, thermal elution and HRGCi activity related
No solvent, Breakthrough MSP mean
Sorbent reusable
Repeated
Solvent d e s o r p t i ~ n ' ~ ' ~ ~ ~~ analysis Lower sensitivity, >4h Solvent elution and HRGCi mean
(activated characoal) Incomplete desorption of polar VOCs, MSP
Solvent G C peak
Diffusive Repeated analysis, Lower sensitivity, 2-42 days Solvent elution and HRGC/ long-term mean
(activated charcoal) Ideal for mailing, Incomplete desorption of polar VOCs, MS@) -0
Solvent desorption No pumps required Solvent GC peak m
a
Back diffusion for weak sorbents, :
Thermal d e ~ o r p t i o n ~ ~ , ~ ~ Diffusion coefficients higher for W O C s ,
Peak concentrations not monitored,
Few diffusion coefficients are known, can
be estimated, <
Uptake rates decrease over time 0
g-
References: 1) Knoppel, 1992a,b. 2) Wallace, 1991c. 3) Gammage et al., 1989. 4) Clobes et al., 1992. 5) Ekberg, 1994. 6) Wise et al., 1990. 7) Gholson et al., 1989. 8) Hsu et m
al., 1991. 9) Jayanty, 1989. 10) Oliver et al., 1986. 11) Pate et al., 1992. 12) Atlas et al., 1985. 13) Bertoni et al., 1981. 14) Bishop and Valis, 1990. 15) Brown and Purnell,
1979. 16) Chan et al., 1990. 17) Cao and Hewitt., 1991. 18) Ciccioli et al., 1992. 19) Fabbri et al., 1987. 20) Health and Safety Executive, 1993. 21) Johansson, 1978. 22)
Krost et al., 1982. 23) Mangani et al., 1982. 24) Proctor et al., 1991. 25 Quintana et al., 1992. 26) Rothweiler et al., 1991, 1992b. 27) Rothweiler, 1992. 28) Vandendriessche
et al., 1991. 29) VDI, 1988. 30) Woolfenden and Broadway, 1992. 31) Brown, 1993. 32) Brown et al., 1992, 1993. 33) Cao and Hewitt, 1993b. 34) De Bortoli et al., 1989.
35) Lewis et al., 1985. 36) Shields and Weschler, 1987. 37) Ullrich, 1992
28 Peder Wolkoff: Volatile Oraanic Comoounds

Table 3.3.2 Important steps from sampling to analysis, and identification of VOCs indoors by use of preconcentration techniques

Sampling--tAnalysis Objectives and Criteria“‘ Pitfallsref

Definition of Sampling objective‘
sampling objective Compliance, conc. distributions, Indoor air chemistry
peak exposure, long-term mean exposure, popu- (reactions forming reactive species)
lation exposure study, source identification
Design of Sampling criteria ’J:
sampling strategy Selection of microenvironment Representativeness’
Sampling duration Temporal-short ~ a r i a t i o n ~ - ~
Sampling frequency Seasonal variation9-I3
Time of sampling Spatial
Location of sampling Ventilation efficiency

Data quality objective52 Breathing zone vs. room conc.I4

Sampling technique Sorbent criteria:
(Choice of sorbent) Desorption characteristic’ 5-23 Artifacts, reactions of ~ o r b e n t ~ ~ - ’ ~
Desorption efficiency Artifacts, reactions of adsorbed VOCs27-34
Hydrophobicity Breakthrough’ 6,17,19,30,35-37
Surface area Cleanliness of sampling
Therm~stability’~~’~~~’~~~ Displacement reactions15,40-42
Light”
Dependence on temperature17 Sorbent
Dependence on Sampling flow calibration
Dependence on sampling flow (Air velocity)43
Transport/ Blank value/background build-up Contamination by sorption/
storage of tubes storage ~ t a b i l i t y ’ ~ , ~ ~ ? ~ ~ L e a k a g e i l ~ s s ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~
Analysisiseparationi Analytical criteria:
identification of VOCs High sensitivity Analytical artifact^"'^^,^^
High selectivity Calibrati~n~~
Column performance
G C programming
Irreversibleiincomplete d e ~ o r p t i o n ~ ~ ~ ~ ~ , * ~ - ~ ~
Power of identification5’
Water c ~ n t e n t ~ ~ , ~ ~ ’ ~ ’
Data quality control Quality control5’
References: 1) ECA, 1994. 2) ECA, 1989b. 3) Brunekreef et al., 1987. 4) Johansson, 1978. 5) Grot et al., 1989; 6) Hodgson et
al., 1991a. 7) Pleil et al., 1989; 8) Wolkoff, 1990b. 9) Fellin and Otson, 1993 10) Gammage and Matthews, 1988. 11) Lebret et
al., 1986; 12) Seifert et al., 1989a; 13) Wolkoff et al., 1991a. 14) Rodes et al., 1991. 15) Bertoni et al., 1981. 16) Brown and
Purnell, 1979. 17) Clark et al., 1982. 18) Fabbri et al., 1987. 19) Figge et al., 1987; 20) Namiesnik, 1988; 21) Riba et al., 1985.
22) Hutte et al., 1984. 23) Knoppel, 1992b; 24) Daisey et al., 1994. 25) Schlitt et al., 1980. 26) Venema et al., 1983; see also
Cao and Hewitt, 1994b. 27) Bayer, 1994. 28) De Bortoli et al., 1989. 29) Pellizzari et al., 1984. 30) Pellizzari and Krost, 1984;
31) Rothweiler et al., 1991, 1992b; 32) Stromvall and Petersson, 1994. 33) Walling et al., 1986. 34) Shields and Weschler, 1992.
35) Harper, 1992. 36) Health and Safety Executive, 1993. 37) Krost et al., 1982. 38) Schmidbauer and Oehme, 1988. 39)
Mattsson and Petersson, 1982. 40) Peters and Bakkeren, 1994. 41) Schoene et al., 1990. 42) Vejrosta et al., 1983. 43) Particularly
relevant for diffusive sampling, Matthews et al., 1989. 44) Brown et al., 1992. 45) Cao and Hewitt, 1993a. 46) Cao and Hewitt,
1993c. 47) De Bortoli et al., 1992. 48) Konttinen et al., 1989. 49) Harper and Guild, 1992. SO) Pleil et al., 1988. 51) Ciccioli
et al., 1992. 52) Keith, 1990.

There are six different sampling objectives as
shown in Table 3.3.2. Furthermore, this Table sum-
marizes sampling criteria, strategy criteria, sampling
media criteria, storage criteria and criteria for the
analysis.
The quality of VOC measurements is a function
of the laboratory which is executing the methodo-
logy and its skill, competence and experience of
field air sampling. Sampling and analysis are expen-
sive tools and the personnel resources cover the
major part of the total cost (Knoppel, 1992a).
It is advisable to start an indoor complaint case
with a walk-through inspection (ECA, 1989a;
Gammage et al., 1989; McCharty et al., 1991) and
gather as much information about activities and
events as possible. The recognition of odors or irri-
tants may help to identify potential emitting sources
and to plan the sampling strategy accordingly.
If the sampling objective is a complaint case,
VOC sampling, usually, should be one of the last
steps of the investigation. The cost of VOC meas-
urements limits the number of samples, thus the

selection of spaces is restricted, thus requiring a de-
tailed sampling design.
The sampling methods listed in Table 3.3.1 have
different time resolutions of sampling, which pro-
vides the choice of obtaining short-term and long-
term time-integrated concentrations. These
methods should be adapted according to the sam-
pling objectives listed in Table 3.3.2. It is important
to remember that the sampling duration and the
analytical sensitivity are interlinked. In principle, it
should be possible to distinguish between different
emission source types in the field. Seifert and
Ullrich (1987) classified sampling procedures into
five different categories of sampling duration. These
were one week, 8-24 hours, 60-180 min, 5-30 min
and continuous monitoring. Both active and passive
sampling are available with the two first categories,
i.e., long-term sampling. While long-term sampling
provides information of long-term time integrated
mean concentrations, multiple, sequential short-
term samples can provide information about short-
term peak concentrations. It should be possible to
obtain information about short-term, discontinuous
(periodic) exposure events, such as activity related
events, traffic contribution or the effect of a tem-
perature increase by multiple sequential short-term
sampling together with a high sampling frequency.
Integrated sampling of VOCs with real-time non-
specific and semi-specific detection is also possible
(Clobes et al., 1992; Ekberg, 1994; Gammage and
Matthews, 1988; Wolkoff, 1987).
The selection of spaces within a room for sam-
pling is another important issue. Rodes et al. (1991)
have discussed the implications of concentration
gradients due to spatial variations, in particular near
point sources. Prior to selection of sampling loca-
tion it is important, depending on the sampling ob-
jective, to consider the history, ongoing activities,
and the climatic conditions and sample accordingly.
An understanding of these parameters will also be
a prerequisite for evaluation of the results. For ex-
ample, it was shown that benzene and toluene from
motor bike parts migrated from crawl space under
one apartment into a neighboring apartment during
a time span of about one month which resulted in
delayed peak concentrations (Wolkoff et al., 1991a).
3.3 Sampling Methods
Active Sampling on Sorbent
Thermal desorption vs. Solvent desorption. The VOC
concentrations encountered indoors are usually in
Peder Wolkofi. Volatile Organic Compounds 29
the pg/m3 range thus necessitating a preconcen-
tration step. The most widely used method is sam-
pling on a solid sorbent (porous organic polymer
or carbonaceous) either actively with the use of
a calibrated pump or in the passive mode (difi-
sion) with the use of a well defined sorbent bed.
Subsequently, the preconcentrated pollutants are
eluted prior to a gas chromatographic analysis.
Generally, thermal desorption has been applied to
porous organic polymers, such as Tenax TA, while
solvent elution has been applied to carbonaceous
sorbents, but the use of thermal desorption is in-
creasing.
The major difference between solvent and ther-
mal elution is the loss in sensitivity by solvent di-
lution of the pollutants followed by GC injection
of a small fraction of the original sample (typically
0.1-1%). The major advantage of active sampling
combined with thermal desorption is the flexibility
in time resolution of sampling, in particular when
monitoring short-term peak concentrations. Active
samplers are also typically used to collect time-in-
tegrated samples and so do not capture peak con-
centrations. With thermal elution, however, only
one sample run is normally available. The loss of
W O C s and solvent overlap during chromatogra-
phy when using solvent desorption, e.g. carbon di-
sulfide, may be overcome by use of dimethylform-
amide (Johansen and Wendelboe, 1981). An alter-
native to thermal desorption is microwave
desorption of carbonaceous sorbents in ceramic
tubes (Neu et al., 1982; Rektorik, 1985; Vu Duc
and Huynh, 1991; Wolkoff, 1986). Multiple analy-
ses of the same sample can be achieved by ther-
mal desorption, followed by micro-concentration
of VOCs on activated carbon and subsequent sol-
vent microextraction at the cost of some sensitivity
(Atlas et al., 1985).
The choice of sampling technique depends pri-
marily on the sampling strategy required. The
sampling and sorbent criteria are interlinked with
the breakthrough volume (BTV) and required
sampling volume, blank value of clean sorbent, de-
sorption efficiency, analytical sensitivity and ther-
mostability of the sorbent. One sorbent cannot
l l l y accommodate a complete range of VOCs
with different volatilities and polarities. The pre-
ferred sorbent should release the VOCs at tem-
peratures below degradation of the sorbent and
should not be susceptible to artifact formation.
Carbonaceous sorbents can release most W O C s
at reasonable temperatures, however to release
30 Peder Wolkoff Volatile Orqanic Compounds
VOCs and SVOCs higher temperatures are re-
quired with the possibility of artifact formation
(vide mfra).
The sorbent Tenax TA has been used for more
than 20 years, the first time for detecting mari-
juana smoke indoors (Novotny and Lee, 1973). It
appears to be the most versatile, thermostable, and
hydrophobic sorbent for indoor measurements
available (today) for monitoring VOCs (in the
range of C5-C6 to 2CI8) (Health & Safety Execu-
tive, 1993; Knoppel, 1992a,b; Rothweiler et al.,
1991). It fulfills many of the sorbent criteria. The
range may be extended to (C,-C,) using certain
precautions depending on the VOC polarity and
BTV. Other sorbents have been used, such as Por-
apak Q and Carbotrap Oohansson, 1978;
Rothweiler et al., 1991; Wallace, 1991), but these
have limited thermal stability or high background
build-up (high blank values) during storage (Cao
and Hewitt, 1993a, 1994a; De Bortoli et al.,
1992). Sorbents like Porapak Q, however, may be
better suited for polar WOCs (cf. Bayer, 1994).
Various forms of carbonaceous sorbents (Bertoni
et al., 1981; Fabbri et al., 1987; Mangani et al.,
1982) have been investigated and multibed tubes
(e.g. glass beads, Tenax TA and Ambersorb XE-
340) have been used (Bianchi and Varney, 1993;
Grot et al., 1991; Tsuchiya, 1988). The advantage
of multisorbents is that a wider range of VOCs
can be simultaneously sampled. However, the
most thermo-sensitive sorbent determines the
upper desorption temperature.
A new Tenax version, Tenax GR (Tenax matrix
with 23% graphitized carbon), has recently been
introduced. This sorbent appears not to be better
than Tenax TA with regard to BTV in comparison
of BTV data from Ventura et al. (1993) with Ten-
ax TA data from Health & Safety Executive
(1993), see also Cao and Hewitt (1994a). It has
high thermal stability, low hydrophobicity (BTV
for water, however, has doubled), but the back-
ground build-up is higher (Cao and Hewitt,
1993a) and the recovery of e.g., P-pinene is low
(Cao and Hewitt, 1993~).
Sampling of ambient air on Tenax at subambient
temperatures has been reported (Ullrich and Sei-
fert, 1978), but water removal is required, thus in-
creasing the chance of retention of polar VOCs. Re-
cently, Yokouchi et al. (1993) have reported quanti-
tative sampling of isoprene and dimethyl sulfide on
Tenax TA at 15°C and they found a doubling of
BTV going from 20 to 10°C.
Diffusive Sampling on Sorbent
Diffusive (passive) sampling (Brown, 1993) with
carbonaceous sorbents has been used extensively for
long-term sampling (Brown et al., 1992; Cohen et
al., 1989; De Bortoli et al., 1989; Lebret et al.,
1986; Seiferr and Abraham 1982, 1983; Seifert et
al., 1989a; Shields and Weschler, 1987, 1992; Wol-
koff et al., 1991a). The main advantage of passive
samplers is that they do not require a pump, are low
in cost, quiet, easy to use and to mail. They are
generally used for long-term sampling, where peak
concentrations cannot be monitored. Diffusion co-
efficients of VOCs are limited, but they can be esti-
mated by calculation (Nordstrand and Kristensson,
1994).
The reported sampling duration is from about
one to six weeks, see Tables 3.3.1 and 4.1.1. Lewis
et al. (1985) have developed a thermally desorbable
diffusive sample device with Tenax to overcome the
long sampling duration required and increase the
sensitivity. The sampling rate was comparable with
pump sampling and ppb levels were measurable
within one hour. Recently, Tenax TA has been ap-
plied for long-term diffusive sampling (Brown et al.,
1992, 1993).
For weak sorbents, such as Tenax TA, W O C s
like benzene may be underestimated, because of
their relatively higher diffusion coefficients, and
back diffusion cannot be ruled out, in particular for
long sampling periods (Brown et al., 1992). Al-
though ideal uptake rates can be estimated with
good accuracy, it has been shown that they change
to lower values over time (Brown et al., 1993; De
Bortoli et al., 1989). This implies that the uptake
rates should be determined for the required sam-
pling period (Bradshaw and Ballantine, 1995).
VOCs sampled on carbonaceous sorbents are hy-
drocarbons and only a few polar VOCs have been
reported. This is partly due to the incomplete de-
sorption of these compounds by solvent elution
using solvents of low polarity.
Another major caveat is the possibility of under-
estimated concentrations due to low air face velo-
cities encountered in indoor environments (Gir-
man, 1993) which may reduce the sampling rate
substantially. In addition, high humidity can reduce
the sampling rates (Lewis et al., 1985).
Pitfalls (active sampling on sorbent)
Pitfalls are possible in all steps from definition of the
sampling objective to the final analysis. The major
pitfalls with regard to air sampling and preconcen-

tration on solid sorbents, not considering the as-
pects of the indoor dynamics (temporal and spatial
variability), are the BTV, stability of sorbent, artifact
formation (e.g. oxidative reactions) before, during
and after sampling and displacement (competitive
adsorption effects of different VOCs). Finally, the
method of analysis and reporting may also become
potential errors. Table 3.3.2 summarizes potential
pitfalls associated with air sampling indoors.
Breakthrough volume. BTVs or safe sampling vol-
umes are available for some VOCs (Brown and Pur-
nell, 1979; Clark et al., 1982; Figge et al., 1987;
Health and Safety Executive, 1993; Krost et al.,
1982). Recent studies have shown that BTVs may
be greatly overestimated at TLV levels by use of the
indirect method (Harper, 1993). It has been recom-
mended to secure a safe sampling volume, that sam-
pling volumes should not exceed 70% of BTV
(Health and Safety Executive, 1993). It is also
known that BTVs are reduced by a factor of ca.
two by a 10°C increase (Brown and Purnell, 1979;
Harper, 1994). Reduction of the BTV (e.g. Porapak
and Carbotrap) at increased humidity is also known
(Harper, 1993, 1994; Cooper and Pellizzari, 1990)
and the sorbents are therefore, in some cases, less
suited than Tenax. It has been noted that high hu-
midity resulted in increased adsorbent resistance
(Fabbri et al., 1987), causing a reduction of the
sampling volume if the sampling flow cannot ,be
controlled. Measurements by the indirect method
at high relative humidities have indicated that BTVs
are about halved for organic polymer sorbents, but
reduced to one tenth for carbonaceous sorbents
(Health and Safety Executive, 1993; see also Clark
et al., 1982). Recent studies have indicated that the
indirect method may be less suitable to measure
BTVs for VOC mixtures because competitive VOCs
may displace already adsorbed VOCs (Comes et al.,
1994; Peters and Bakkeren, 1994; Schoene et al.,
1990; Vejrosta et al., 1983; Bertoni et al., 1981).
For W O C analysis, the choice of sorbent may
become important (Bayer, 1994) as an alternative
to cooled trapping. Harper (1994) has stated that
the BTV may increase considerably at low concen-
trations, however, displacement in VOC mixtures
appear also to be important (Peters and Bakkeren,
1994).
StabiliQ. The stability of samples collected on Tenax
have been reported to be at least two weeks at
-15°C (Knoppel, 1992b), but it is likely to be
Peder Wolkoff: Volatile Organic Compounds 31
longer (Health and Safety Executive, 1993). How-
ever, sample loss of, in particular, W O C s is poss-
ible, if the tubes are not properly sealed (Brown et
al., 1992; De Bortoli et al., 1989). Special pre-
cautions to produce very low blanks, for measuring
in the ng/m3 range have been reported by Schmid-
bauer and Oehme (1988). However, blank values
are built up depending on storage conditions and
long sampling durations (Cao and Hewitt,
1993aJ994a). De Bortoli et al. (1992) showed that
Carbotrap had more background build-up than
Tenax TA and the same was found for Tenax GR
(Cao and Hewitt, 1993a, 1994a).
Some sorbents, in particular the carbonaceous
ones, retain large amounts of water, which may not
only reduce BTV, but also can cause degradation
of the chromatographic resolution, clog the column
with water and may affect split ratios (Knoppel,
1992b; Health and Safety Executive, 1993). The
choice of analytical column and GC temperature
programming may therefore be critical. Proper pro-
gramming starting at subambient temperature and
using several temperature ramps makes it feasible to
identify and quantify a large range of W O C s and
VOCs using Tenax TA as sorbent (Bianchi et al.,
1989).
Artifact Formation. The formation of artifacts on
Tenax by reactive air pollutants (e.g ozone and ni-
trogen oxides) has been documented and may be
overcome for nonpolar VOCs by a scavenging so-
dium thiosulfate impregnated glass fiber filter (Pel-
lizzari et al., 1984). Caution should therefore be
taken using Tenax TA in ozone enriched environ-
ments (Knoppel, 1992b). The two most common
artifacts are benzaldehyde and acetophenone, if
their i/o ratios are below 1.35, they may in part indi-
cate the presence of nitrogen dioxide and ozone
(e.g. Daisey et al., 1994). Artifact formation and
incomplete desorption of adsorbed VOCs which
either disappear or rearrange, e.g. isomerization of
a-pinene to 3-carene or loss of haloalkanes have
been reported (Cao and Hewitt, 1993c; De Bortoli
et al., 1992; Konntinen et al., 1989; Rothweiler et
al., 1991; Stromvall and Petersson, 1992; Walling
et al., 1986). Some of these reactions are likely to
occur at high desorption temperatures. Artifact
degradation of alkenes has also been reported (Sei-
fert and Abraham, 1983). A few VOCs have been
reported to give unexplainable low recoveries, like
tertiary butanol (Health and Safety Executive,
1993). Walling et al. (1986) suggested that increas-
32 Peder Wolkoff. Volatile Organic Compounds
ing the sampling volume should give indication of
artifact formation.
3.4 Analysis, Reporting, Validation
Indoor air, usually, contains several hundred VOCs
and the identification thereof by combined GC/MS
is a major analytical task. Normally, full MS scans
are required, but selected ion monitoring (target
compound monitoring) may be applied if certain
VOCs are searched for. The number of analyses
may be reduced, depending on the sampling objec-
tive, e.g. the objective could be certain suspect
VOCs, responsible for irritation or odors. Alterna-
tively, the analytical criterion could be that VOC
concentrations less than e.g. 5 pg/m’ are disre-
garded in the first screening. Another criterion of
selection could be that concentrations below certain
comfort or health related thresholds are disre-
garded.
Morey and MacPhaul (1990) have proposed that
the VOC measurements should be ordered in chemi-
cal classes and ranked according to the highest con-
centration, rather than using TVOC. WHO (1989a)
recommended that “To facilitate the use of data on
exposure to VOCs, the distribution of the respective
concentrations should be reported as the 1Oth, 50th,
and 90th (if possible, 95th and 98th) percentiles”.
Recently, it was indicated that even short-term meas-
urements (15 min) may be inappropriate for evalu-
ating mucosal irritation and it was suggested that in
addition to the average concentration, peak concen-
trations and the time above relevant comfort values
should be reported (Jensen et al., 199%).
There have been several approaches to reduce the
analytical costs. These include quantitation of the
immediately perceived IAQ in decipol values (Fan-
ger et al., 1988). The TVOC concept (Mdhave and
Nielsen, 1992) has been suggested as another poss-
ible analytical short cut. There are not yet standard-
ized sampling nor analytical guide for TVOC and its
impact on IAQ and health is not well understood.
However, there are three basic strategies for re-
porting TVOC. These are:
1. Non-speciated TVOC (direct measurement). The
instrument signal from a direct reading instrument,
FID and PID (Gammage et al., 1989) is converted
into solvent (e.g. toluene) equivalentdm’. Infrared
(FT-IR) (Clobes et al., 1992) and photoacoustic
(Ekberg, 1994) detectors can in some cases monitor
specific VOCs.
2, Non-speciated TVOC (total GCIFID detector re-
sponse). Gas chromatography separation and the de-
tector response (FID) of the total integrated area of
all separated VOCs is converted to solvent equiva-
lentdm’, after correction for artifacts and back-
ground (Grot et al., 1991). Alternatively, the total
ion current from G U M S analysis is converted,
usually by the use of toluene-d8 or fluorinated hy-
drocarbons as standards.
3. Speciated TVOC (total GC separated VOCs). Gas
chromatography separation and summation of indi-
vidually separated and calibrated VOCs (Fellin and
Otson, 1993; Morey and MacPhaul, 1990; Seifert,
1990; Shields and Weschler, 1992; Wolkoff et al.,
199 1b) .
Seifert (1990) has suggested that TVOC means the
sum of GC separated and quantified VOCs (WHO
1989a definition). The ten most abundant VOCs of
each VOC class (- formaldehyde) (see Table 1.2.2)
should be summed up and finally all classes pooled
to give the TVOC value.
There appears to be both analytical and interpre-
tational pitfalls associated with the use of TVOC as
a marker for IAQ and SBS prevalence. From an
analytical viewpoint, VOC and TVOC measure-
ments depend on sampling volume and sampling
mediudsorbent type, BTVs and desorption tech-
nique applied. For example, Rothweiler et al.
(1992b) showed that the choice of sorbent may be
crucial for the determination of TVOC. In addition
to the sampling pitfalls, there are the principle of
quantitation, use of G C detector and response fac-
tors, the desorption efficiency and the use of stan-
dards. The most commonly used detector is FID
which underestimates, in particular, low molecular
weight oxygenates and halogenated hydrocarbons
because of their lower FID-response (Jorgensen et
al., 1990). This, however, may be overcome by use
of MS as the detector unit (Wallace et al., 1991). It
is not surprising that TVOC based on a total FID
integrated area response can differ markedly from a
TVOC value determined according to Seiferts’ ap-
proach, in particular when oxygenates or halogenat-
ed hydrocarbons are dominant (cf. Epstein et al.,
1990; Otson and Fellin, 1993; Rothweiler et al.,
1993). However, if the VOC composition is largely
hydrocarbons, generally, good agreement has been
found between TVOC based on the total FID inte-
grated area response and the summation of single
VOC concentrations.
A more basic problem using TVOC as an IAQ/

SBS marker is the non-specificity of TVOC. In
other words, we do not yet know how a mixture of
VOCs is assessed by the sensory system. The major
question is whether the TVOC concentration or a
defined subset, either in mass or molar concen-
trations, can provide an adequate description of the
exposure associated with SBS prevalence without
knowledge about the mechanism(s) of symptom
generation having been established (Berglund and
Lindvall, 1992; Brown et al., 1994). The TVOC
concept, implicitly, assumes that there exists a dose-
response relationship with VOCs concentrations.
Morey and MacPhaul (1990) found their rank
order assessment of individual VOCs indoors and
outdoors, was a good approach for evaluating build-
ings. Several field studies have not found relation-
ships between VOC measures and SBS prevalence.
Some studies have indicated even lower TVOC
levels in sick building than in healthy buildings, see
Chapter 4.
At present, it appears that a simple VOC meas-
urement cannot be used directly to describe the per-
ception of VOCs (TVOC) (cf. Sundell, 1994).
Therefore, it appears that further development is re-
quired before TVOC may be used as a relevant con-
centration measure and IAQ/SBS marker. One ap-
proach could be fractionation of TVOC according
to VOC classes, e.g. TVOC(aromatics) (cf. Shields
and Fleischer, 1993). It has been suggested that
lipophilic VOCs may have similar irritative thresh-
olds if their partial vapor pressure is divided by the
saturated vapor pressure (Ferguson principle, cf.
Abraham et al., 1994) rather than molar concen-
tration is used (Cometto-Muiiiz and Cain, 1991,
1992, 1993). Therefore, another approach to pres-
ent TVOC could be the total chemical activity ex-
pressed as the sum of ratios over the partial and
saturated vapor pressures of each VOC present
(Mdhave and Nielsen, 1992). Likewise, the total
lipophilicity could be another approach, cf. Chapter
6. However, one has to be aware that the chemical
activity, e.g. the irritative potential expressed in
RD,, values, can vary tremendously, due to small
chemical differences (Bos et al., 1992; Malhave and
Nielsen, 1992).
Combined TVOC and decipol results obtained
from the emission of selected building materials
have also indicated that these parameters should be
used cautiously as IAQ markers (Wolkoff et al.,
1991b). In another study it was shown that a GC-
odorgram (GC snifling) evaluation exhibited odor
perceptions with different intensities than the GC-
Peder Wolkoff. Volatile Organic Compounds 33
€?ID or GC-MS analysis of the same air sample
(Berglund et al., 1982b; Berglund and Lindvall,
1992) and similar experiences have been found for
headspace analyses of linoleum and a building seal-
ant, respectively aensen et al., 1995b; Wolkoff,
1990a). In other words, the two types of detectors
are not always compatible (Berglund and Lindvall,
1992). The link between perceived IAQ and VOC
concentrations is further complicated because odor
stimulus-response relationships usually become flat,
while pungency functions show steeper relation-
ships. (Odors follow Steven's law, S=I<XC", here
C=concentration and S=perceived odor magni-
tude, where n=0.1-0.8 (Cometto-Muiiiz and Cain,
1991)). The consequence is that the substantial re-
duction of the concentration of an odorous VOC
may result in little reduction in perceived odor in-
tensity. Hypersensitivity, has been reported
(Cometto-Mufiiz and Cain, 1991). Weak odors are
generally considered hypoadditive (Berglund and
Lindvall, 1992; Cometto-Muiiiz and Cain, 1991),
strong odors, usually, are additive (Berglund and
Lindvall, 1992), but hyperadditive effects are
known, but not often reported (Ahlstrom et al.,
1986; Arctander, 1969). It has also been shown that
single odorants below threshold, but in mixture,
may become perceptible (Patterson et al., 1993). Ir-
ritants are considered additive (Cometto-Muiiiz
and Cain, 1991, 1992, 1993) or even hyperadditive
(Cometto-Muiiiz and Cain, 1993).
Recent studies have indicated that a relative
change of VOCs (ATVOC) concentrations during
the workday may be better correlated with SBS
prevalence than (T)VOC concentrations (Lundin,
1993; Sundell et al., 1993). In a Canadian study,
the best correlation with symptom reporting was
obtained using the combined effect of the total pol-
lutant exposure load based on American air quality
standards and WHO guidelines, i.e. effects of car-
bon monoxide, TVOC, formaldehyde, nitrogen
dioxide, dust and fungi were included (Menzies et
al., 1993). This is compatible with the proposed ex-
posure model for eye irritation suggested by Wolkoff
et al. (1992).
Despite the above limitations associated with the
use of the TVOC measurement, it has its justifi-
cation for comparative purposes (e.g. intervention
study). When the VOC profile is known or relatively
constant, such as in product development, produc-
tion control and in studies with a controlled VOC
profile, TVOC can also be used. For example,
TVOC can be measured by a direct reading instru-
34 Peder Wolkoff Volatile Oraanic Cornoounds
ment and used on-line in production control, as a
source finder and as a crude indicator of the VOC
level in a room. However, caution should be taken
(Weschler and Hodgson, 1992) with regard to the
VOC dynamics (Wolkoff, 1992a); generally, there-
fore TVOC would not be usefid in interbuilding
comparisons.
Calibration and Validation. The traditional approach
for calibration is establishment of the recovery of
individual VOCs, in addition to determination of
the overall performance of the analytical system. In
the method, the following information should be in-
cluded: limit of detection or limit of quantitation,
calibration procedure, blank value and RSD of the
combined sampling and analysis.
Concentrations obtained by short-term sampling
(1 hr) may show large hourly and day-to-day fluctu-
ations due to the source dynamics (Weschler and
Hodgson, 1992; Wolkoff, 1990b). Although these
fluctuations may be markedly larger than the RSD
of the method, it is recommended to perform qual-
ity control and assurance of the method on a regular
basis, e.g. by use of internal and external laboratory
standards, in addition to control of the analytical
system by a quality assurance scheme. The use of
internal standards by spiking sampling tubes either
prior to or post sampling has also been applied, in
particular with GUMS.
Validation of a carbonaceous difisive sampler at
low VOC concentrations using the G U M S target
method has been reported. RSD of 13% for
220 measurements has been reported by Otson et
al. (1992a), similar to that reported by Shields and
Weschler (1987). Comparison of active sampling
with diffusive sampling showed good correlation
(1?=0.998) (Otson et al., 1992b). Brown et al.
(1992) compared two hours active sampling with
four week diffusive sampling under similar start
conditions, on Tenax TA, and found similar VOC
profiles, although somewhat different ranking or-
der of some of the major VOCs. The results
showed that the four week diffusive sampling can
provide useful quantitative data, at least for the
VOCs measured. In a repeatability test over 17-35
days sampling they found that RSD ranged from 2
to 12%. The reproducibility between laboratories
has been reported to be in the order of 25% with
diffusive samplers in an European intercalibration
study (De Bortoli et al., 1984).
3.5 Methods of Potential Source
Finding
It is important to have methods available to identify
and objectify exposure pathways, i.e. the route from
source + exposure -+ dose. In complaint cases it
can be relevant to search for potential VOC sources.
Another relevant topic is the apportionment of
VOCs from potential emitting sources. This should
help understand the impact on IAQ of each emit-
ting source and could lead to reduction of potential
emitting sources. There are four different ap-
proaches to source identification, in addition to
panel evaluations, as discussed below.
Direct reading instruments may be useful in the
field as a source finder, however, not yet as an odor
finder. Portable instruments, such as a photoioniza-
tion and flame ionization detectors, Fourier-trans-
form infrared spectrometry and photoacoustic spec-
trometry have been used to show the impact of ac-
tivities and use of products in homes (Clobes et al.,
1992; Ekberg, 1994; Gammage and Matthews,
1988; Sheldon et al., 1987; Wiese et al., 1990; Wol-
koff, 1987), see Table 3.3.1.
Seifert and Ullrich (1987) were the first to pro-
pose the use of passive samplers in a complaint case
to identify potential emitting sources by placing a
sampler near suspected sources, in addition to one
sampler located in the center of the room. The con-
centrations of different VOCs, however, did not
vary markedly. As an alternative to air sampling,
they had analyzed previously the lacquer used for a
radiator and they found a series of aliphatic alde-
hydes and fatty acids (cf. Ullrich et al., 1982). A
reinvestigation of the room air chromatogram re-
vealed hexanal, and a separate additional air sam-
pling of acids showed hexanoic acid. The example
illustrates how headspace analysis of suspected
emitting sources can be an aid to field measure-
ments. A static headspace of suspected materials
brought to the laboratory (Young, 1992; Wolkoff,
1990a) can provide qualitative information about
important emitting sources, when the results are
compared with a room air sample. Some materials
may change their emission characteristic (“dry
out”) during transportation, thereby invalidating the
method (Wolkoff et al., 1995). Field (non-destruc-
tive) emission testing with the FLEC (Wolkoff et al.,
1991c) can overcome this problem, see section 5.3.
Lebret et al. (1986) examined VOC patterns in
Dutch homes. Multivariate analysis was applied for
identification of common VOC patterns in the

homes. Two patterns were identified and assigned
to mixtures of common petroleum-based solvents
of different boiling ranges. The use of multivariate
statistical packages appears to be a powerful tool for
searching of common VOC patterns. Daisey et al.
(1 994) identified various sources in 12 buildings by
use of multivariate analysis. The indoor sources
were: dry cleaning, bioeffluents, products and out-
door sources like motor vehicle emission. Nelson et
al. (199 1) identified three groups, solvent-like
VOCs, one group of six aromatic VOCs and meth-
ylene chloride as a separate group. The VOC frac-
tionation approach applied by Shields and Fleischer
(1993) identified personal care products.
The impact of emissions from building materials,
the ventilation system, human activities including
bioeffluents, renovation and maintenance pro-
cedures on perceived IAQ may be evaluated by
panel of judges and quantified, e.g. by the olf
method (Fanger et al., 1988). The panel is trained
in a standardized manner to express different ace-
tone concentrations each corresponding to the per-
ceived air quality given in decipol values (ac-
ceptability rating). The evaluation provides a snap-
shot (in less than 1 min) of the perceived air quality
when entering a room and does not necessarily re-
flect the overall impact of the IAQ and SBS preva-
lence, in particular mucous airway irritation during
8 hours work. Such a method should also consider
the impact of temperature, i.e. perceived freshness
Peder Wolkoff: Volatile Organic Compounds 35
of the air (Berglund and Cain, 1989) and the per-
ceived odor intensity (Malhave et al., 1993a), in ad-
dition to lighting and noise (Clausen et al., 1993a).
However, neither high concentrations of carbon
dioxide (Jokl et al., 1993) nor about 0.75 mg/m3
formaldehyde concentration would be perceived by
a panel which reports the immediately perceived air
quality (Wolkoff et al., 1991b). There are several
other factors influencing such panel evaluation, i.a.
the different time scale of perception of odors versus
irritants (Engen, 1986; Hudnell et al., 1993). It has
been suggested that panel evaluation may be useful
as a total measure and identification of chemical
and biological odor loads (Moschandreas, 1992;
Cone and Shusterman, 1992).
3.6 Future Needs for Sampling and
Analysis
Apart from the reactive aldehydes, formaldehyde
and acrolein, little information is available about
other species which may cause increased SBS. One
theory is the indoor air chemistry, which may form
“reactive” organic species like peroxides, hydroper-
oxides, peroxy-acetyl nitrates and radicals formed
by reactions with ozone and nitrogen oxides. An-
other example of potentially irritative species is sur-
factants (cf. Kreiss et al., 1982; Taylor and Hind-
son, 1982). Some of these are carried in dust par-
ticles. They could destabilize mucous membranes
due to their surface tension reduction.
4, VOC Field Investigations
4.1 VOC Field Measurements
The concern for the impact on IAQ (and health)
by exposure to VOCs indoors has prompted VOC
measurements to be carried out as early as 1974 in
Skylab 4 (Bertsch et al., 1974). Later, investigations
have been performed in a college classroom (Wang,
1975), in offices (Johansson, 1978) and in homes
(Jarke et al., 1981). The classic work on offices by
Turiel et al. (1983) showed i.a. the increase of
VOCs when the ventilation was decreased, however,
the use of traditional TLV values could not explain
the reported complaints.
Field studies which included VOC measurements
and SBS symptom ratings, air sampling and symp-
tom reporting were rarely simultaneous. There are
several uncertainties associated with comparing
VOC concentration measurements with symptom
reporting. The prevalence of symptoms depends
upon the questionnaire design and it may suffer
from the Hawthorne Effect (unintentional overre-
porting due to subjects’ awareness of being
studied), selection of populations, confounding fac-
tors, (e.g. recall bias) (see Levin (1993) and Men-
dell (1993)) and stress (Apter et al., 1994). In retro-
spective questionnaires there is the possibility of bias
due to prior perceived sensations of e.g. a malodor,
which may result in overreporting of symptoms
(Knasko, 1993). The questionnaire design itself
may, depending on the character of questions (posi-
tive, neutral or negative), influence the reporting;
therefore, validation of the questionnaire design is
important. Differences between genders in evalu-
ating certain questionnaire words appear also to give
rise to bias or may reflect actual gender differences
in perception. For example, women can detect
odors at lower concentrations of some VOCs than
men (see section 6.2).
Many VOCs have been measured in national field
studies (for review, see Brown et al., 1994). The
sampling strategy, sampling techniques and analyses
applied (see sections 3.2 and 3.3) have been quite
different as shown in Table 4.1.1. Generally, the
sampling duration has been days and the sampling
medium either carbonaceous or of the porous or-
ganic polymer type, like Tenax. Only one of the na-
tional studies has used a short sampling duration
of less than one hour (Rothweiler et al., 1993) as
previously applied by Johansson (1978) and Wolkoff
(1990b). The reporting of VOC measurements
therefore becomes an important issue (cf. Chapter
3 ) . For example, measurements sampled in the
center of a room may not be representative of the
“true exposure” (Brunekreef et al., 1987; Rodes et
al., 1991), an issue for the identification of associ-
ations. The personal exposure, is sometimes higher
than in the center which again is higher than out-
door measurements (Sheldon et al., 1992). The dif-
ferent temporal and spatial patterns of VOC con-
centrations reflected in the source dynamics are an-
other important factor affecting the result of a
measurement (cf. 2.8 and 3.2).
Johansson showed already in 1978 that some
VOCs may be strongly (time) dependent or depend-
ent upon number of persons present. This has been
confirmed by several other groups (Farant et al.,
1992; Clobes et al., 1992; Crump and Madany,
1993; Grot et al., 1991; Hodgson et al., 1991a;
Shields and Weschler, 1992; Wolkoff, 1990b; Wol-
koff et al. 1991a). While the Johansson study showed
fluctuations ofVOCs of endogenous origin, like etha-
nol and acetone (cf. Table 2.3.1.1) and isoprene
(Cailleux et al., 1993), other studies have shown large
fluctuations related to, i.a. orange peeling (Anders-
son et al., 1993b), tea drinkmg (Wolkoff, 1990b) and
office equipment related activities, in particular the
use of “wet” photocopying machines (Daisey et al.,
1994; Grot et al., 1991; Tsuchiya, 1988,1990; Walk-
inshaw et al., 1987). The use of personal care prod-
ucts containing fragrances and siloxanes (Wallace et
al., 1991b; Shields and Fleischer, 1993; Wolkoff,
1992b; Wolkoff et al., 1992) may also add VOCs to
the indoor environment.
Considering the spatial and temporal variability,
it is difficult to characterize the exposure of individ-
ual occupants. Most epidemiological studies with
VOC measurements have relied on a relatively few
locations to characterize exposure.
 Peder Wolkoff Volatile Organic Compounds 37

Table 4.1.1 M a l o r national field studies of VOCs measured indoors and methods applied

Field study Number VOCs Sampling method Analytical method'

of quantified Sampling duration
buildings
Diffusive Active
davs hours
____~ ~_______

Andersson et al., 1990 26 1+TVOC 5 Charcoal, SD-GCIFID+MS

Brown et al., 1992 100 8 28 Tenax, TD-GCIFID
Cohen et al., 1989 35 17 21 Charcoal, SD-GCIMS
Daisey et al., 1994 12 39 8 Multibed sorbent, TD-GCIMS+FID
De Bortoli et al., 1986 15 35 4-7 days Tenax, TD-GCIFID
Krause et al., 1991 479 58 14 Charcoal, SD-GCIFIDIECD
Lebret et al., 1986 319 45 7 Charcoal, SD-GCIFID
Otson et al., 1992a ca. 800 26 14 Charcoal, SD-GCIMS
Rothweiler et al., 1993 22 7" 0.5 Tenax, TD-GCIMS
Shields and Fleischer, 1993 68 TVOC 42 Charcoal, SD-GC
Van der Wal et al., 1991 10 1 lb 2 Charcoal, SD-GCIFID
Wallace et al., 1987aI1991 760 20 2-12 Tenax, T D - G U M S
a) Consists of five different VOC classes, many VOCs. b) VOCs have been grouped together. c) SD=solvent desorption; T D =
thermal desorption, G C =gas chromatography, MS = mass spectrometry.

tween perceived odor intensity and a weekly based

4.2 Association Between VOC
Exposureand SBS
Table 4.2.1 lists some in-field studies in which an
association between reported SBS prevalence and
measured VOC concentrations has been identified,
their findings and sampling method applied, while
Table 4.2.2 lists studies with no associations iden-
tified.
The study by Hodgson et al. (199 lb) is so far the
only study where measurements of indoor par-
ameters including VOCs have been carried out sim-
ultaneously with SBS symptom reporting. This in-
dicated an association between TVOC, mucous
membrane irritation and CNS-symptoms, noise
and lighting. It should be noted, however, that work
most likely had to be interrupted during symptom
reporting. In a Canadian study in five buildings,
locations for investigation were selected on the basis
of having dry or wet photocopymg machines, the
latter type emitted isoparahs (Broder et al., 1993).
It was found that TVOC (median 3 mg/m3) ranked
third after work-related stress and gender as a pre-
dictor of an adverse outcome.
The complex dynamic behavior of VOCs (cf. 2.8)
usually results in large VOC fluctuations during the
workday including day-to-day variations (Weschler
and Hodgson, 1992; Wolkoff, 1990b), one would
not anticipate to find strong associations between
(T)VOC concentrations and SBS symptom preva-
lence or a panel's evaluation of the odor intensity
and acceptability. However, in the Danish town hall
study Zweers et al. (1990) found associations be-
TVOC. The result was surprising because TVOC
was shown to fluctuate markedly on an hourly and
daily basis (Wolkoff, 1990b), but also because odor
intensities are not necessarily additive at low con-
centrations encountered indoors (Berglund and
Lindvall, 1992; Cometto-MGiz and Cain, 1991)
(see 3.4).
The associations found in the studies by Nor-
back and colleagues are surprising not only be-
cause VOC concentrations and the number of re-
ported VOCs were low compared to other studies
(Noma et al., 1988; Wang, 1975; WHO, 1989a),
but also considering the time lag of months be-
tween questionnairing and air sampling. Further-
more, the SBS symptom score applied in the cor-
relation analysis was derived from pooling retro-
spective yesho answers of symptoms experienced
during the last six months. It is questionable
whether such an addition of symptom scores is
valid, if the symptoms have not been found to be
intercorrelated. Recently, Norback et al. (1995)
have reported markedly higher mean TVOC con-
centrations than in previous studies. It has been
suggested by Baird et al. (1987) and by Noma et
al. (1988), in their studies of a healthy and a sick
preschool and a control building, that the ex-
posure to VOCs may act in an overall integrated
manner as a pattern, e.g. concentration gradients
or spatial differences rather than as a quantitative
exposure to (T)VOC(s). They found that the
number of VOCs was greater in the healthy build-
ing than in the "sick" building, the latter, however,
38 Peder Wolkoff Volatile Organic Compounds

Table4.2.1 Examples of field studies in office-like environments and VOC measurements (associations found with SBS prevalence]
( i n alphabetic order of first author)

Literature Number Buildings VOC/ Range Results Sampling Method

of (rooms) TVOC Particles Sorbent (sampling flowimin)
subjects udm3 udm3
Baird et al., 3 (16)’ 158 VOCs not measured Number of identified VOCs Porapaq Q (1 limin for 15
1987 greater in healthy than in “sick” min), TD-GC
building
Broder et al., 647 5 (92) TVOC 1-803 Isoparaffines from wet process Tenax TA, TD-GC
1993 150-49100 photocopying machines in 213 of
examined units
Hodgson et al., 147 (5) TVOC 44-66 TVOC and particle exposures Measurement and ques-
1991b 1600-3800’ were higher for women than tionnaire simultaneous.
Hodgson, 1992 men; TVOC, CO, C 0 2 in- Photoionization detector
creased as the number of occu- calibrated against buta-
pants increased, TVOC incl. diene. Concentration meas-
lighting correlated with SBS ured over 20 min.
Lundin, library C33 VOCs not measured “TVOC and C 0 2 correlate with Porapaq Q (1 l/min for 15
1991 <10 symptom increase and change min), TD-GC
over the day in satisfaction with
the indoor climate”
Menzies et al., 1546 4 (8-12) TVOC 12-21 1 Higher concentrations of certain Activated charcoal (200 mli
1993 164-1645 pollutants were associated with min, 8 hrs), SD-GC
symptoms. TVOC, in particular
with mucosal irritation
Noma et al.3, 2 (17) 158 VOCs not measured Concentration gradients in Porapaq Q (1 limin for 15
1988 33 v o c s 3 “sick” building, healthy building min), TD-GC
exhibits less location-to-location
differences of VOCs
Norback et al.
1990a 205 11 50-1380 not measured Sum of 16 VOC hydrocarbons Activated charcoal (1 limin
1990b 129 6 70-180 8-24 correlates with SBS score for 2 h), SD-GC
Norback et al., 39 31 2-ethyl- not measured Activated charcoal (1 limin
Concentrations of octanols cor-
1993 hexanol for 2 h), SD-GC
related with rated IAQ
1-octen-3-01
Norback et al., 88 TVOC Sum of 16 VOCs, in particular Activated charcoal (1 limin
1995 (70-93 80) terpenes, correlated with asthma for 2 h), SD-GC
symptoms
Sundell et al., 1087 29 (86) “lost” TVOC 3-740 “Lost” TVOC (between supply 5 hrs on activated charcoal,
1993 formaldehyde 11-59 and room air values) was associ- SD-GC
ated with SBS prevalence and
low TVOC was associated with
high formaldehvde
Ware et al., 74 15 VOCs4 T h e exposure to a mixture of 8 weeks’ sampling of ambi-
1993 Mean TVOC VOCs (from a chemical plant) ent air on charcoal, GC/MS
25 was associated with respiratory
symptoms
Wilkins et al., 870 9 TVOC in dust Certain VOCs in dust were as- Dust sampled by vacuum
1993 sociated with SBS prevalence (ir- cleaner. T D at 120°C for
ritation and concentration diffi- 60 min sampled on Tenax
culty)6 TA, followed by TD-GC
Zweers et al., 4 (8) 100-3200 TVOC and the temperature cor- Tenax TA (45 mlimin for
1990 formaldehyde related with the odor intensity 45 min), high sampling fre-
fluctuating and odor acceptability5 quency, TD-GC
1) Two healthy buildings and one sick (closed), measurements at 17 locations. 2) For TVOC average mean molecular weight set
to 100 Dalton. 3) One healthy and one sick school, same study as Baird et al. (1987); only 33 VOCs identified and used in
analysis. 4) Ambient VOCs. 5) See also Wolkoff, 1991. 6) See also Gyntelberg et al., 1994.
 Peder Wolkoff Volatile Organic Compounds 39

Table 4.2.2 Examples of field studies in office-like environments and V O C measurements [no associations found with SBS prevolence]
[ i n alphabetic order of first author]

Literature Number Buildings Range Range Results Sampling Method

of (rooms) TVOC Particles Sorbent (sampling flowlmin)
subjects udm’ udm3
Berglund et al., 48 2 117l, 2582 16 Despite a sick building, it was 15 1 sampling on Porapak
1992 not possible to assess exposures Q, TD-GC
by use of human performance
testing
~~

Brown et al., review 80 VOCs VOC and TVOC in complaint

19943 of 50 buildings were not consistently
studies elevated relative to established
buildings
De Bortoli et al., 787 10 (83) 220-3930 Formaldehyde and short-term Tenax TA or Carbotrap,
1990 VOCs were not correlated with TD-GC
complaint index
Fisk et al., 880 12 3404 No correlation with VOCs and Multi-sorbent for 8 hrs,
1993 3805 SBS. Highest TVOC in air con- SD-GC. Measurements in
12006 ditioned rooms, partly because the week preceding ques-
of wet DhOtOCODV machines tionnaires
~~

Menzies et al., 740 2 VOCs and formaldehyde con-

1991 centrations, despite significant
changes from week to week, were
not associated with SBS
Moschandreas 30 (25%) 1 120-2507 20-60 Occupant perceived odor inten- Direct reading instrument
et al., 1990 sitv did not correlate with TVOC
Nelson et al., 383 100 sites 68 Not able to establish relation- 9 hour sampling (Tenax)
1991 ships between IAQ parameters
and self-reoorted auestionnaires
~~

Skov et al., 2369 14 100-1200 86-382 No association found between Single point 50 min sam-
1990 VOCs and SBS prevalence pling on Tenax TA, T D -
GC
Sundell et al., 4 14 160 Use of photocopiers were La. as-
1992 (1994) sociated with SBS prevalence.’
Sverdrup et al., 74 253-393 (T)VOC poor IAQ indicator. Sampling on Tenax, T D -
1990 GC
~~

1) Sick building, 3 persons present. 2) Healthy building, 3 persons present. 3) Review. 4) Mean value, natural ventilation. 5)
Mean value, mechanical ventilation. 6) Mean value, air conditioning. 7) A healthy building. 8) Sum of mean values for solvents,
aromatics, and methylene chloride. 9) See also Sundell et al. (1993) in Table 4.2.1

had a different ventilation system and it was unoc-
cupied (Baird et al., 1987). In a follow-up study,
it was suggested that the main distinction between
the healthy and sick building was “location-to-
location differences in chemistry within the build-
ings and not the concentrations of the chemicals
as a whole” (Noma et al., 1988). The healthy
building only exhibited minor differences with re-
gard to light hydrocarbons from the outdoor air.
Interpretation of the results is difficult, partly be-
cause the sick building had a different ventilation
system, was unoccupied during VOC sampling,
and it is questionable whether a 15 min air
sample, at a certain location, reflects representative
concentrations or VOC patterns (cf. Weschler and
Hodgson, 1992). Additionally, the multivariate
analyses carried out, in both studies, only incor-
porated about 20% of VOCs (nonpolar) present in
the air. (It is tempting to draw a parallel to the
finding that fluctuating exposures of m-xylene
(100400 ppm) resulted in greater effect (body
balance and reaction time) than a constant ex-
posure (Ruhimalu and Savolainen, 1980)). In a
later study, TVOC levels in a sick building and a
control building were both very low (ca. 80 pg/m3)
and so were the levels of other pollutants (par-
ticles, aldehydes and ionic species) (Berglund et
al., 1992).
40 Peder Wolkoff: Volatile Orqanic Compounds
Recently, some Swedish studies have identified a
loss of TVOC (A TVOC) during transport from the
intake to exhaust (Berglund et al., 1993; Lundin,
1993; Sundell et al., 1993). The results by Sundell
et a]. (1993) showed a weak indication that high
TVOC in room air was associated with reduced
symptom prevalence in 29 buildings. Mean geo-
metric TVOC levels, however, were generally below
100 pg/m3. Disregarding the generally low VOC
levels, the findings are compatible with the results
by Baird et al. (1987), the results obtained from the
studies of the reaction of carpet emissions with
ozone (Weschler et al., 1992) and a human ex-
posure study in a simulated office environment
study (Wolkoff et al., 1992, see 6.3). These Swedish
studies infer that reactive species (e.g. formaldehyde
and acetic acid from limonene) may be formed by
VOC reactions with ozone and nitrogen oxides (cf.
Table 2.5.2). These studies also indicate that the
relative change of VOCs or TVOC concentration
may be a better measure of the VOCs for the identi-
fication of associations between VOC exposure and
SBS prevalence. In the Swedish library study, a cor-
relation was found between changes in the preva-
lence of 8 SBS symptoms observed during one
workday and the mean concentration of 34 VOCs
as measured in the exhaust air (Berglund et al.,
1990; Lundin, 1991).
Norback et al. (1993) showed a relationship be-
tween the concentration of two MVOCs, l-octen-
3-01 and 2-ethylhexanol and rated air quality. This,
despite the fact that the odor detection thresholds
(Devos et al., 1990) for the MVOCs are about one
to two orders of magnitude higher than the meas-
ured concentrations. However, individual sensi-
tivities can range over several orders of magnitude
and that is not reflected in the reported odor thresh-
olds.
Finally, Menzies et al. (1993), used “that day”
questions and found associations between symptom
prevalence and the combination of all measurable
pollutants, thus calling for a multi-pollutant ex-
posure model compatible with the proposed ex-
posure model for eye irritation (Wolkoff et al.,
1992).
Some studies have not yielded association be-
tween VOCs and SBS prevalence (Fisk et al., 1993;
De Bortoli et al., 1990; Moschandreas et al., 1990;
Nelson et al., 1991) or occupant perception of IAQ
parameters (Moschandreas et al., 3 990), see Table
4.2.2.
Most studies have generally not considered the
possible interaction of VOCs with formaldehyde
and other indoor pollutants such as particles and
ozone. In one field study, in which a mobile
chamber was attached to a sick preschool, healthy
subjects were exposed to 170 pg/m3 formaldehyde,
while varying percentages of air from the sick build-
ing were added. A fourfold increase in perceived
odor intensity was observed when the “sick building
air” was increased fiom 10 to 100% (Ahlstrom et
al., 1986).
Recently, it was shown that dust particles carry a
large number of VOCs and SVOCs (Hirvonen et
al., 1994; Schlitt et al., 1993; Wolkoff and Wilkins,
1994). This leads to the hypothesis that particles,
though present in low concentrations, may be ad-
ditional important pollutants due to their adsorbed
chemistry (e.g., the combinations of surfactants and
VOCs/SVOCs) (see also Berglund and Lindvall,
1986).
Smoking is another important indoor pollutant.
It is well-known that smoking increases the com-
plaint rate (Hedge et al., 1989a; Jaakkola et al.,
1991; Robertson et al., 1988; Taylor et al., 1984)
and deteriorates the IAQ (Fanger et al., 1988; Gun-
narsen and Fanger, 1992).
Measurements, generally, do not represent the
VOC concentration in the breathing zone, but
rather the mean time-integrated concentration
measured over a certain duration (from less than
one hour to several hours/days) in the center of a
room. Concentration gradients may occur near the
breathing zone (Rodes et al., 1991). Hodgson et al.
(1991b) and Hodgson (1992) found that women
were exposed to higher mean concentration of both
TVOC (100% higher) and total particles (50%
higher) than men. This observation could be linked
to the general finding that women usually have
higher SBS symptom prevalence, disregarding their
job category (Burge et al., 1987; Espir et al., 1988;
Hedge et al., 1989b; Jaakkola et al., 1991; Lam et
al., 1987; Skov et al., 1989; Stenberg et al., 1993;
Stenberg and Wall, 1995). However, Hodgson et
al. (1991b) did not find any gender differences of
symptom reporting, despite the exposure differ-
ences, which agrees with a recent chamber exposure
study (Otto et al., 1993). Higher TVOC exposure
of women could be rationalized in terms of use of
personal care products including perfumes (Shields
and Fleischer, 1993; Wallace et al., 1991b), less of-
fice space and less mobility. Also, Berglund et al.
(1992) failed to find gender differences of impaired
performance in a sick building.

At present, it appears that the associations with
VOCs identified could also reflect the interaction of
other indoor parameters such as the occupant den-
sity and activities, concentration gradients and par-
ticles as VOC carriers. Hitherto unknown reactive
VOCs formed by atmospheric (indoor air) chemis-
try (Weschler et al., 1992), cf. Zhang et al.
(1994a,b), is another hypothesis (Sundell et al.,
1993), previously suggested by Sterling and Sterling
( 1983).
It should be clear fiom the literature that the as-
sociation between VOC exposure and SBS preva-
lence is not yet understood, but several hypotheses
have been proposed (see Conclusion). Few field
Peder Wolkoff. Volatile Organic Compounds 41
studies have carried out objective symptom meas-
ures (e.g. physiological measures) along with en-
vironmental measurements, e.g. VOCs. Future
analyses of field studies should focus on the possible
action of VOC patterns associated with reported
SBS prevalence and include objective (physiologi-
cal) measures. This should lead to identification of
chemical patterns and establish which VOCs could
be responsible for the perceived differences (cf.
Noma et al., 1988; Wilkins et al., 1993). Also, re-
cent findings related to indoor air chemical reac-
tions which form “reactive species” should be pur-
sued.
5. Emission Testing of Materials
5.1 Introduction
Development of healthier building materials and
products and product control has been prompted
by an ever increasing public interest in and demand
for more environmentally friendly indoor building
materials and office equipment. Improvement of the
IAQ by the use of healthy indoor materials (Wol-
koff, 1990a), i.e. materials with low and harmless
emission of VOCs, may be carried out by material
selection (Andersen et al., 1982) and source control
(Jayjock, 1994; Levin, 1992; Tucker, 1991; WHO,
1989a), in addition to adequate flush-out periods
or increased ventilation prior to occupancy of new
buildings.
Until now, the objective has been emission testing
of building materials and describing the VOCs and
their emission profiles (concentrations over time).
Furthermore, factors influencing the emission pro-
file have been investigated. The important goal
should be to relate these measurements to real
world scenarios by proper modeling. Emission test-
ing of building materials should be carried out
under controlled conditions, usually, in climatic
chambers. Technical guides thereof have already
been prepared (ASTM, 1990; ECA, 1991; Nord-
test, 1990; Tichenor, 1990). Only limited efforts
have focused on the intercomparability of climatic
test chambers (ECA, 1993; Gunnarsen et al.,
1994). The problem still remains to establish the
entire procedure from the choice of the “right”
chamber, the preconditioning of the test material,
the analysis, translate data to real scenarios and
comfort and health evaluation. In addition, predic-
tion of the emission profile should be possible to
evaluate the impact on IAQ over time. E.g., in a
recent study, M~lhaveet al. (1995) could predict
formaldehyde concentrations over time in a new
apartment, based on long-term emission testing of
major materials used in the same apartment.
There are several approaches to emission testing:
chemical and sensory tests, studies of the sorption
properties, bioassays and human exposure studies.
This chapter deals with chemical emission testing
and briefly the use of other methods, like a mouse
bioassay, while human exposure studies with se-
lected building materials and office machines are
presented in Chapter 6 .
The ultimate goal of emission testing is to evalu-
ate the impact of building materials on IAQ. Such
information can be used by building material manu-
facturers to produce better materials and also en-
able building designers and architects to select the
best indoor environmentally friendly materials. This
should reduce the probability of increased dis-
comfort problems, like SBS symptoms, in particular
in new or renovated buildings. Future evaluation of
the impact of VOCs on IAQ from building materials
should incorporate: 1) Emission characteristics, i.e.
VOC emission profiles as function of time under
controlled conditions, transferable to real scenarios;
2) Knowledge of the material emission processes
and models which can predict the short-term and
long-term behaviors; and 3) Principles for establish-
ing comfort and health criteria for ranking and
selection of indoor environmentally friendly ma-
terials. Additionally, the evaluation should consider
both short-term and long-term effects and it should
take into account other potential emitting sources.
A rating system for classification of the emission
from building materials has been suggested by Sei-
fert (1992). He rated the emissions from a material
according to their long-term effects caused by car-
cinogens, mutagens, teratogens and allergens, in ad-
dition to short-term effects as mucous membrane
irritation and odor annoyance, using a point system.
Previously, Person et al. (199 1) have applied TLVs
to evaluate the emission from household products.
The first national system for the combination of
emission testing with a health evaluation has ap-
peared recently (Dansk Standard, 1994; Nielsen et
al., 1994).
5.2 Chemical EmissionTesting
Table 5.2.1 lists the various methods used for emis-
sion testing of building materials and products and
some of their advantages and disadvantages. The
methods are extraction analysis, static and dynamic
headspace analysis, the latter using a climatic
chamber, dynamic emission testing with a climatic
chamber, dynamic large scale and full house testing
 Peder Wolkoff: Volatile Organic Compounds 43

Table 5.2.1 Emission source testing of VOCs from materials (modified from Tichenor, 1992)

Extraction analysis:
Provides information on material’s composition. It provides information of the total content of VOCs to be emitted. It does not,
however, provide emission raw data, i.e. the emission profile.
Static emission testing (headspace analysis):
Provides information about emissions’ composition. Static headspace analysis may reflect inadequate emission profiles (Colombo et
al., 1991).
Dynamic chamber emission testing:
Provides emission composition and emission profile data. Can provide data about the immediately perceived air quality.
Sorption properties of materials can be determined.
Animal bioassays can provide information about the effect of the pollutant load. In particular, the potential irritative effect can be
determined with a mouse bioassay.
Dynamic large chambers:
Provide composirion data and emission profile data. Human exposure studies provide information about subjective SBS symptoms
and objective clinical measures may establish dose-response relationships.
Test house studies:
Provide information about emission profile behavior under realistic conditions and the contribution of human activities. Realistic
sorption effects can be determined.
Field studies with a portable micro emission chamber (FLEC):
Non-destructive emission testing of suspected materials to identify and apportion emission sources in the field. Emission testing can
be carried out in the laboratorv.

and field emission analysis by use of a portable
micro chamber (FLEC), vide infra.
Extraction can provide better information than
normal headspace analysis, in particular if the ma-
terial contains large amounts of SVOCs (Pleil and
Whiton, 1990).
Static and dynamic headspace analysis can pro-
vide information of emitted VOCs. The former is
conveniently carried out by insertion of the sus-
pected material into a “non-emitting” bag filled
with clean air. The VOCs are identified by the com-
bination of headspace sampling on solid sorbent,
thermal desorption, followed by GC and MS tech-
niques and, when necessary, combined with sniffing
of eluted VOCs (Eustache et al., 1988). Using this
latter approach, malodorous sulfurous containing
VOCs emitted from a polysulfide based sealant, see
Fig. 5.2.1.A (Wolkoff, 1990a) and odorous alde-
hydes (hexanal) from a cured paint Cyoung, 1992),
respectively, have been identified. This technique
was later used to develop a more indoor environ-
mentally friendly odorless sealant (Wolkoff, 1990a),
see Fig. 5.2.1B. However, in static headspace analy-
sis, the emission profile may be dominated by non-
polar VOCs relative to higher boiling and polar
VOCs depending on the material matrix (Colombo
et al., 1991; Neil and Whiton, 1990). Static
headspace analysis has the advantage that the ma-
terial loading can be large increasing the analytical
sensitivity of VOCs emitted.
Good quality (chemical) emission testing is costly
(Knoppel, 1992a) and so are climatic chambers. The
need for a flexible, easy to use and relatively inexpen-
sive chamber prompted the development of a port-
able micro emission chamber (cell volume, 35 cm3)
(Wolkoff et al., 1991c, 1995).This Field andLabora-
tory Emission Cell (FLEC) has two purposes: it can
provide VOC emission data on suspected emitting
material surfaces in case of problem buildings for
source identification, be used for source strength de-
terminations, apportionment studies and it can also
be used in the laboratory as a climatic chamber. The
unique feature of the FLEC is that the source (ma-
terial surface) becomes an integral part of the micro
chamber, see Fig. 5.2.2. Because of its design, the
surface air velocity (which is proportional to the air
exchange rate) in the FLEC is under better control
than traditional climatic chambers with and without
fans. In addition, the time to reach chamber equilib-
rium has been reduced considerably for polar
SVOCs, due to the FLEC’s relatively small volume
compared to other small chambers and its high ex-
change rate. Both repeatability and reproducibility
have been shown to be satisfactory for selected ma-
terials (Roache et al., 1996; Wolkoff et al., 1991c,
1995).
5.3 Experimental Parameters
Influencin the Emission of VOCs
8
from Buil ing Materials
One of the goals of emission testing is transform-
ation of emission data to real senarios by modeling.
44 Peder Wolkoff Volatile Organic Compounds

A 31
. TOT. A6. 6500
,6500

4
15 I

f'

2 4 6 -6 10 12 14 16 16 20 22 24 26 26 30 32 34 mn

350000

1 Fig. 5.2.2 The Field and Laboratory Emission Cell "FLEC"

33

process of emission may also depend on the type of

VOCs emitted and the interactions which may oc-
cur between different VOCs (Sullivan, 1975). Evap-
oration is controlled by transfer (diffusion) of VOCs
I III
through the gas phase boundary layer. Usually, the
drying process of wet products is evaporation and
,mu7
such emission processes follow usually a first order
Fig. 5.2.1 Static headspace of building sealant from nylon bag, exponential decay (Dunn and Tichenor, 1988).
cryogenic sampling on Carbotrap B followed by microwavede- The emission can also be controlled by internal dif-
sorption and GC/MS analyses, and combined with sniffing. 50 fusion within the material itself, i.e. the diffusion is
m Sil 19CB capillary column 10 3 2 mm], GC program: 0" increas-
ing @C/rnin to 220°C. A] Sealant giving rise to complaints about slower than the evaporation process. The distinction
malodors, * =rnalodours ideiitified by GC/sniffing. B) Re- between the two processes should be reflected, to
developed formulation of sealant VOCs: 1 =acetaldehyde, 3 = some extent, in their dependence on the ventilation
carbon disulfide; 1 O=propanol; 1 2=divinyl sulfide; 16=acetyl-
acetone; 19=xylene; 24=undecane; 26=decamethyl cyclo- rate (or rather the surface air velocity in and above
hexasiloxane; 27=phenol, 28=naphthalene; 29=dodecamethyl the boundary layer). At high air velocities, limiting
cyclohexasiloxane; 3O=siloxane, 3 1 = 1,2,5-trithiacyciohep- evaporative transfer of VOCs may be reached.
tune; 3 2 = BHT; 33 =technical isododecane
Individual VOCs are released, usually, in quite
different amounts and with different time depend-
encies, i.e. different emission rates and different
Therefore, it is a prerequisite to know all salient and emission processes, the latter may even change dur-
controllable parameters influencing the outcome of ing the decay period.
an emission testing. In particular, the parameters Many parameters affect the emission profile of
which can affect the emission rate and which emis- VOCs from building materials (cf. ECA, 1991; Sei-
sion processes of primary pollutant sources both fert, 1992; Tichenor, 1992). Several of the par-
after short periods (hrs) and long periods (months). ameters are controllable in the laboratory and a few
For chambers with large wall area to volume ratios, are related to field conditions. Among these are
adsorption capacities, i.e. the chamber sink effect sample age, sample conditioning and sample prep-
may be important. In addition, ad- and desorption aration, atmospheric chemistry during testing, in
properties of a material itself are important material addition to the temperature, relative humidity, air
properties to determine. exchange rate and air velocity. One non-controllable
The emission of a VOC from a material surface parameter is the vapor pressure. Some of these par-
is controlled by physical processes, including evap- ameters are discussed below, including sample (in)-
oration and internal diffusion (Sullivan, 1975). The homogeneity.

Age. Knowledge of emission characteristics as a
function of age is important, because most materials
exhibit decaying emission profiles. This is particu-
larly relevant for wet products within a short time,
but some may continue emitting for several months,
such as waterborne paints (Berglund et al., 1982a;
Clausen et al., 1991; Wolkoff et al., 1991a; Wolkoff
and Nielsen, 1993). The age is also to some extent
associated with material storage time and handling
processes prior to testing and during analysis. The
age or history after building completion is also re-
lated to seasonal variation (temperature and venti-
lation) as found, e.g., in the Danish Twin Apart-
ment Study (Wolkoff et al., 1991a). It appears that
two of the most important parameters determining
the outcome of emission testing are the precon-
ditioning period and the handling of the material.
A i r exchange rate, air velocity and concentration gradi-
ent. The air exchange rate (AER) is an important
parameter, because it reflects the amount of dilution
and the fresh air supply to the climatic chamber.
Therefore, it has a major impact on the chamber
concentration. What is important in this context is
whether AER or the air velocity in the material’s
surface (boundary layer) has an influence on the
emission rate. The mean air velocity was measured
to be 7.2 c d s e c in six occupied homes (Matthews
et al., 1989). The frequency distribution maximized
at 0-2.5 c d s . In another study, Kovanen et al.
(1987) measured air velocities up to 9 c d s in
homes and offices, but velocities up to 20 c d s have
been reported (cf. Girman, 1993). The impact of
the air velocity may be strongly associated with the
type of emission process and the identification of
these is crucial for prediction of the long-term emis-
sion profile by modeling.
The emission rate of VOCs from wet materials
(paints and lacquers) which evaporate, before dry-
ing, is likely, but not necessarily, to be controlled by
evaporation (Clausen, 1993). Their emissions have
been found to be sensitive to the AER (Tichenor
and Guo, 1991; Tichenor et al., 1993; Wolkoff et
al., 1993b). Tichenor and Guo (1991) found that
the emission rate was proportional to the ratio of
the AER and the material loading (material surface/
chamber volume). This relationship was shown also
for formaldehyde (Matthews et al., 1987; Konopin-
ski, 1985; Reponen et al., 1991). In a study by Wol-
koff et al. (1993b) using the FLEC, it was shown
that the emission rates for selected VOCs emitted
from a waterborne paint, a thin film material, were
Peder Wolkoff Volatile Organic Compounds 45
strongly dependent on the AER (air velocity) and
almost proportional to the AER, using a first order
decay model including a sink effect. After the initial
film formation, the emission process may change to
be diffusion controlled within the fildmaterial. The
emission may also be a combination of evaporation
and internal diffusion, as suggested by Clausen et
al. (1991).
If the emission is controlled by internal diffusion,
change of the AER should have minor effect on the
emission rate. The emission profiles of thick layer
materials, e.g. carpet and sealant, could be de-
scribed satisfactorily by a recently developed expo-
nential diffusion model (Wolkoff et al., 1993b). This
was also the case for PVC flooring materials
(Clausen et al., 1993b) and linoleum (Jensen et al.,
1995a). It appeared that for carpet and sealant, the
emission constants showed less dependence on the
AERs which corresponded to air velocities from
0.3-1.4 c d s (Wolkoff et al., 1993b). Linoleum,
however, behaved differently, apparently because a
“stable” concentration gradient had not yet been es-
tablished within the material, in addition to the
possibility of oxidative degradation (Jensen et al.,
1996, 1995a).
A concentration gradient in the boundary layer
should increase the emission rate. During the early
stage of the emission testing of textile carpets, it has
been observed that increased AER resulted in an
enhanced emission rate (Sollinger et al., 1993;
Ullrich, 1990; Wolkoff et al., 1993b), in spite of a
supposed diffusion controlled emission. One ration-
ale could be the composition of textile carpets
(backing and fibers) and the fibers themselves form
a boundary layer.
The loading factor has also been shown not to
affect carpet emissions under static conditions (Sol-
linger et al., 1993). However, it must be realized
that the loading factor, per se, is only a practical
parameter, providing proper chamber concen-
trations by use of standardized loadings.
Atmospheric chemistry. The presence of air oxidants,
such as ozone, may influence the measurement of
the emission. This has been shown for carpets for
which the addition of ozone showed not only a
marked decrease of styrene and 4rphenylcyclohex-
ene (latex VOCs) emissions, but an enhancement
of aldehydes and TVOC (Weschler et al., 1992).
The ratio of measured aliphatic acids over their cor-
responding aldehydes from linoleum also appeared
to depend on oxidation, because the ratio decreased
46 Peder Wolkoff. Volotile Orqonic Compounds
under anaerobic conditions (nitrogen instead of air)
aensen et al., 1996). The observed increase of e.g.,
hexanal during the summer in an occupied apart-
ment could be rationalized by increased oxidation
and chain scission of fatty acids present in the lin-
oleum floor and other fatty acid residues (Wolkoff
et al., 1991a). Other studies point to ozone as a
cause of increased aldehyde and acid formation (cf.
Table 2.6.2) and deterioration of material surfaces
(Weschler et al., 1990b).
Materialfilm thickness. The importance of the film
thickness and structure has not been studied in de-
tail. The question is whether differences in the
thickness has any impact on the emission rate and
emission process. Clausen (1993) showed that the
emission rate decreased on increasing the film thick-
ness of a waterborne paint. He has also suggested
that variation of the thickness may provide infor-
mation about the emission process. It is anticipated
that a change fi-om a solid surface (e.g. steel) to a
porous surface will prolong the emission decay of
e.g. paints (Gehrig et al., 1994). The difference in
porosity to a more impermeable film structure in a
paint appeared also to prolong the emission profile
of Texanol considerably (Wolkoff and Nielsen,
1993).
Temperature and relative humidiq. The temperature
affects the vapor pressure and the diffusion coef-
ficients of the emitted VOCs. Therefore, the tem-
perature has a major impact on the emission rate of
VOCs fi-om building materials. This has been
shown in several bake-out studies where the VOC
concentration was enhanced by a temperature in-
crease (Girman, 1989). The temperature and hu-
midity dependence of formaldehyde release is well-
known (Van Netten et al., 1989). However, it is at
present difficult to generalize for VOCs, because
their emission may depend partly on the VOC po-
larity and the material's composition. The emission
of VOCs, with different volatility and polarity, from
a textile carpet showed dependence (increased
chamber concentrations) at elevated temperatures,
most pronounced for the high boiling benzothiazole
(Sollinger et al., 1994); this was found related to
decomposition of an added accelerator. Similarly,
both Seifert et al. (1989b) and Van der Wal et al.
(1994) have observed increased emission of 4-phe-
nylcyclohexene from textile carpets (latex backng)
and 2-ethylhexanol from PVC flooring materials,
respectively, by a temperature increase. In the car-
pet study by Sollinger et al. (1994), no significant
dependence on humidity was observed for 22 differ-
ent VOCs, except aniline which showed a weak in-
crease at elevated humidity, probably caused by de-
composition.
Vapor pressure. Vapor pressure effects would gen-
erally not be expected under dynamic emission test-
ing and indoor realistic concentrations. However, it
is possible during the initial burst of VOCs from wet
and un-conditioned materials that a vapor pressure
effect may be important, because high concen-
trations may be achieved in the boundary layer and
the chamber zone decelerating the evaporation.
Tichenor and Guo (1 99 1) observed a vapor press-
ure effect for woodstain and polyurethane some
hours after application. However, TVOC concen-
trations were 3-5 orders greater than normally en-
countered indoors. Very high material loadings may
also result in a buffer effect (Tichenor et al., 1990),
so increased ventilation may increase the emission
rate of VOCs controlled by evaporation (Jayjock,
1994). One study has not been able to verify vapor
pressure effects at realistic concentrations (Clausen
et al., 1990, 1991). The vapor pressure (chamber
concentration) can to some extent be controlled by
the loading factor and the AER in the climatic
chamber.
Sink effects. The impact of the sink effect is twofold.
The climatic chamber usually has a sink effect, i.e.
adsorption onto chamber walls (De Bortoli and
Colombo, 1992; Tichenor, 1992) and the materials
have adsorption (mass uptake) and desorption
(mass loss) properties. The chamber sink effect has
to be accounted for by necessary mathematical
modeling (Dunn and Tichenor, 1988). However,
certain competitive effects may possibly play a role.
For example, the emission of Texanol, a high boil-
ing VOC, from waterborne paints did not exhibit a
noticeable chamber sink effect in the FLEC (Wol-
koff and Nielsen, 1993) as anticipated from a pre-
vious study (Wolkoff et al., 1993b). A rationale
could be that the most abundant VOC (propylene
glycol), 2-3 orders of magnitude greater, competed
by adsorption onto the chamber wall. VOCs emit-
ted from one material may adsorb onto another ma-
terial and desorb depending on the climatic con-
ditions (Berglund et al., 1989); likewise dust par-
ticles act as a VOC reservoir (Wolkoff and Wilkins,
1994). The fleecy factor (area of the textile surfaces
over room volume) has been shown in Danish and
 Peder Wolkoff- Volatile Organic Compounds 47

Finish studies (Jaakkola et al., 1994; Nielsen, 1987)
to correlate with SBS symptom prevalence. How-
ever, this effect was not found in two other studies
(Sundell et al., 1994; Zweers et al., 1992). The sink
effect of materials has been measured, usually at
high concentrations (Borrazzo et al., 1993; Colom-
bo et al., 1993; Jmrgensen et al., 1993; Kjzr and
Nielsen, 1991; Levsen and Sollinger, 1993; Schmall
and Seifert, 1987).
Sink effects may be important and they could
have an influence on the emission decay, in particu-
lar for SVOC (Ligocki et al., 1992). The sink effect
may extend the residence time of VOCs and thereby
prolong the exposure period (Neremieks et al.,
1993; Sparks et al., 1993). In the case of evaluation
of suspected building materials the sink effect must
be considered (Berglund et al., 1989). However,
steady state indoor concentrations may not be

Table 5.4.1 Models applied to VOC emissions from building materials

~~~ ~

Materials Film type Models Time Comments

elapsed
thin thick First First order hternal hours
order decay+ diffusion
decay sink effect
Carpet + + +1 56 Emission rate enhanced by increased
+Z 170 AER.1'3
+3 96 Emission sensitive to temp., but not hu-
midity.

+4 3000 Determination to reach 50% indoor relevant

odor t h r e ~ h o l d . ~
~

Domestic products + +5 300 Emission decay related to TLVs.

Linoleum + +6 1000 Determination to reach 50% indoor relevant
odor threshold.
Paint i- +7 8400 Determination of time to reach emission rate
0.1 mg/(m2Xh).'
+ 3,s 350 Emission strongly depends on AER.3
t 4 3000 No sink effect because of competition with
dominating V O c 4
Paint-mercurv +9 2.5-order decav model fitted.'
Polyurethane + + '0 24 Vapor pressure effect observed.
PVC flooring + +I1 600 Model: diff. coefficient depends exponen-
tially on concentration gradient within ma-
terial.
Sandwich materials + 60-350 Double exponential model.12
Sealant + + 48 Emission rate enhanced with increasing
AER.'O
+3 192 Model accommodates nonpolar and polar
VOCs. Emission rel. insensitive to air ex-
change rate.3
+4 3000 Determination to reach 50% indoor relevant
odor t h r e ~ h o l d . ~
Wax, wet products + +10,13,14
24 Emission rate enhanced with increasing
+I5 14 AER."J
Emission data from two different chambers
compared.I3
Woodstain + + 10 150 Emission rate depends on AER.
Double exponential model.15
25 Mass transfer model."
~

References: 1) Sollinger et al., 1993. 2) Little et al., 1994. 3) Wolkoff et al., 1993b. 4) Wolkoff and Nielsen, 1993. 5) Person et
al., 1991. 6 ) Jensen et al., 1995a. Note: poor model fit was obtained for oxidative sensitive VOCs. 7) Clausen et al., 1991. 8)
Clausen, 1993. 9) Tichenor et al., 1991b. 10) Tichenor and Guo, 1991. 11) Clausen et al., 1993b. 12) Colombo et al., 1990.
13) Wolkoff et al., 1995. 14) Chang and Guo, 1992a. 15) Chang and Guo, 1992b. 16) Tichenor et al., 1993
48 Peder Wolkoff Volatile Organic Compounds
affected if completely reversible sorption occurs,
e.g. VOCs having vapor pressures greater than 1
torr (Ligocki et al., 1992).
Material Homogeneity. The measurements of the
emission rate of TVOC, 4-phenylcyclohexene, styr-
ene and toluene emitted from new latex based car-
pets at different manufacturing conditions, led to
the overall conclusion that evaluation of carpet
emission is complex (Hawkins et al., 1992). The
emission testing was carried out 1 and 24 hours
after unwrapping and placement in the chamber
and large variability within samples was revealed. It
is likely that a longer term testing would have re-
sulted in a clearer picture of the emission profile
behavior (cf. Wolkoff and Nielsen, 1993).
It was shown in an interlaboratory study that
sample inhomogeneity should be considered with
the use of, in particular, small chambers (ECA,
1993).
5.4 Models
Most of the studies carried out in climatic chambers
(Levin, 1992) have just measured the “supposed”,
steady state emission rate and characterized the
emitted VOCs under the supposition that the emis-
sion rate was constant after a certain time.
A prerequisite for prediction of the emission rate/
profile after a certain time is knowledge about the
emission process and models associated therewith.
If the emission testing is performed under “realistic”
and controllable conditions, mathematical modeling
should be able to predict the emission profile after
a certain time. If an incorrect model is applied, de-
termination of the time to reach a given emission
rate may be erroneous. For example, it was shown
using a first order decay model that the concen-
tration of two VOCs emitted from a vinyl floor
covering decreased faster than predicted. An expo-
nential diffusion model resulted in a better fit
(Clausen et al., 1993). This latter model is based on
Fick‘s First Law and incorporates that the diffusion
coefficient depends, exponentially, on the concen-
tration gradient within the material. Similarly, the
emission profile of styrene from processed paper
showed a better model fit using the exponential dif-
fusion model than a first order decay model (Wol-
koff et al., 1993a).
Table 5.4.1 lists some of the major findings re-
garding modeling of the emission profiles of VOCs
from various building materials. Ideally, the emis-
sion profiles and the associated emission constants
derived from the model should be independent of
the climatic chamber provided the air velocity,
chamber sink and chamber concentration all are
under control, cf. Girman (1993).
A majority of the studies so far have been carried
out within a rather short time duration (less than
one week). Generally, a first order exponential de-
cay model of the type, R=R, . ePk where R and
’
R, are the emission rate at time t and t=O, respec-
tively, and k=rate constant, has been applied (Dunn
and Tichenor, 1988). One major finding is that the
emission rate of some wet products, e.g. paints and
waxes, may be enhanced by increased AER under
the test conditions applied.
Mass transfer models have been applied to thin
films (coatings) within 25 hours after application, in
which time the transfer rate is assumed to be con-
trolled by transfer in the boundary layer. It is the
supposition that the transfer process is evaporation
controlled (Tichenor et al., 1993). Such a transfer
model has also been applied to a PVC flooring ma-
terial in a 21-compartment model (Neretnieks et
al., 1993). Finally, double exponential models have
been applied to obtain better model fits, however,
these models do not necessarily reflect the emission
process. It is important that the controlling emission
mechanism has been properly identfied. Therefore,
models should be evaluated at least at two air velo-
cities (Guo, 1993). Even if a proper model has been
identified there are many factors which may ob-
struct modeling of primary (and secondary) pol-
lutant source emissions, in particular after long
time. Some of these are:
The pre-conditioning (duration) may be very
critical.
Hardeningcuring process of applied material has
not yet finished at the start of emission testing.
A uniform concentration gradient has not yet
been established within the material.
Change of emission process may occur after a
certain duration.
Multiple emission processes may occur from the
same material.
Competing emission processes of critical VOCs.
One approach for emission testing could be evalu-
ation of the impact on the IAQ and coupling to the
time aspect of emission decay to be able to develop
more indoor environmentally .friendlymaterials and
products. This could secure occupants against high

exposures, in particular in new buildings and after
renovation. The first example using modeling to de-
termine the necessary time to reach a certain emis-
sion rate of waterborne paints was developed and
used for ranking purposes by Clausen et al. (1991).
Later, Wolkoff and Nielsen (1995) have suggested a
system which unifies chemical emission testing over
time with mathematical modeling, when necessary,
and comfort evaluation. The principle was to deter-
mine the time value, t(C,), necessary to reach the
relevant indoor air value, C,. This value was based
on odor andor airway irritation thresholds in a stan-
dard room of 17.4 m3 (Dansk Standard, 1994;
Nielsen et al., 1994). Coupling of emission testing
of some household products within the first 100-
150 hours with TLVs and compartment modeling
has been described by Person et al. (1991). Finally,
Black (1992) has proposed a method to rank car-
pets according to their TVOC emission rate meas-
ured 24 hours after chamber installation. The
method does not consider the possibility of different
emission profiles and it assumes that TVOC is a
health marker relevant for comparison.
Testing should ideally be performed under con-
ditions, such that emission data can be transformed
to real senarios. Air velocities, when relevant, and
specific ventilation rates (Us per m2) should be re-
alistic. It appears at present that the emission rate
of a particular VOC depends on the concentration
in the boundary layer above the material surface,
more so for evaporation than diffusion controlled
processes. However, there is still much more knowl-
edge required about the impact of the various par-
ameters discussed above before emission test data
can be properly compared.
-
5.5 Emission Testing Other Methods
One goal of emission testing is to evaluate the im-
pact of emitted VOCs on the IAQ over the time
span from the building completion or renovation
thereof. It is not unusual that comfort and health
data are unavailable from the literature (Nielsen et
al., 1996a). Furthermore, it is difficult to evaluate
the cumulative effects of emitted VOCs. One other
method may be to evaluate the irritative potential of
the emission. This is a bioassay based on modifi-
cation of the standard ASTM mouse bioassay
Peder Wolkoff- Volatile Oraanic Cornoounds 49
(ASTM, 1984). The method measures the sensory
irritation, based on analysis of the respiratory pat-
tern of mice, e.g. exposed to the emission of VOCs
from building materials. The decrease of the respir-
atory rate, mediated via a trigeminal or vagal reflex,
is a measure of the potential irritance. The method
can distinguish between sensory and pulmonary ir-
ritation. The F Q 0 , the concentration inducing a
50% reduction of the respiratory rate, has been pro-
posed for TLV assessment (Bos et al. (1992) have
discussed the limitations of this method).
The modified bioassay was applied to carbonless
copy paper forms (Wolkoff et al., 1988), later to
paints (Hansen et al., 1991) and building materials
(Nielsen et al., 1996b; Wolkoff et al., 1991b).
Formaldehyde was identified as a major causative
agent for the response in the first and third studies.
In the first study, it was found that a certain paper
which showed the greatest bioresponse also con-
tained several hundred ppm of free formaldehyde.
The bioresponse was compatible with a reported
outbreak of complaints in a post office during han-
dling of a new batch of copy forms. Similarly, a hu-
man exposure study on building materials showed
that eye and airway irritation reported in connection
with exposure to the emission from a particle board
coated with an acid-curing paint gave rise to a pro-
longed bioresponse compatible with a massive
formaldehyde emission (Johnsen et al., 1991; Wol-
koff et al., 1991b). The method requires high ma-
terial loadings, thus justifying its use for comparison
studies, screening purposes and selecting for de-
tailed chemical analysis and toxicological evaluation
(Tepper and Costa, 1992).
Study of the olfactory properties can also be
helpful for understanding the sensory emission of
building materials (Gunnarsen, Fanger, 1992). Re-
cently, Jensen et al. (1995b) have compared the
perceived (relative) odor intensities with chemical
emission data from 13 linoleum products. Multi-
variate analysis of the data revealed that two prin-
cipal factors could explain 68% of the odor inten-
sity variation. The factors were heavily weighted
for aliphatic C6-C8 acids and C5, C7 and C l o un-
saturated aldehydes, respectively. The GC/sni&g
analysis of emissions and the above approach ap-
pear to be a powerful combination to identify
odorous VOCs.
6, Chamber Exposure Studies with VOCs
6.1 Introduction
Human chamber exposure studies differ from field
studies in several ways. In chamber studies, environ-
mental measurements, both subjective and objective
can be performed simultaneously.In addition, some
climatic parameters, such as temperature, humidity,
exposure, air exchange rate can be controlled dur-
ing the exposure period. Chamber exposure studies
can provide information about dose-response re-
lationships, whereas field studies may only provide
information about associations between exposure
loads and e.g. SBS prevalence.
Some of the salient problems associated with
evaluation of chamber exposure studies are: 1) that
they do not normally mimic the source dynamics
encountered indoors and therefore it may be diffi-
cult to extrapolate the results obtained to real world
scenarios. Furthermore, 2) the choice of subjects
may be a problem with regard to representativeness,
3) the sensitivity of the selected subjects and 4)
power of the study (i.e. the number of subjects that
can be tested) is limited. Either the subjects are se-
lected as particularly sensitive to the indoor climate
or normal, healthy subjects are selected. Although
randomization is possible, it is difficult, in particular
with odorous VOC mixtures, to conduct the ex-
posure in a blind manner and overreporting of SBS
symptoms cannot always be excluded (recall bias,
cf. Knasko, 1993). In fact, two field studies indicate
that odor annoyance can be associated with in-
creased SBS symptom reporting of headache, eye
and throat irritation and nausea (Shusterman et al.,
1991; Wallace et al., 1993). One chamber exposure
study has shown that fewer SBS symptoms were re-
ported by persons exposed previously to a fresh
smell than by people who had been exposed to a
malodor (Knasko, 1992), i.e. one’s attitude to re-
port may depend on prior sensations or visual con-
tact. For example, Moschandreas and Relwani
(1992) observed that non-smokers reported a
higher odor intensity from ETS when smokers were
visible than non-visible.
There are subjective and objective effects to be
investigated in chamber exposure studies. The for-
mer includes perceived mucous membrane irri-
tation in eyes and the upper, lower airways, facial
skin effects, poor IAQ (odor annoyance) and other
SBS symptoms according to standardized ques-
tionnaires (Andersson et al., 1988; Lund and Rice,
1992). Objective measurements include i.a. changes
of the eye tear film physiology (Norn, 1983, 1992;
Kjzrgaard, 1992a,b). The tear film quality (Johnsen
et al., 1991) expressed as the pooled effect of re-
duced break-up time of the tear film (precorneal
film) (Franck, 1986), semiquantitative measure-
ment of reduced precorneal superficial (multi-lipid)
fatty layer (Franck, 1991), and reduced foam for-
mation at inner eye lid (Franck and Skov, 1989), in
addition to micro damage of the conjunctival epi-
thelium (Franck, 1986) have been used as measures
of effects of the eye. Another objective instrument
is the nose (Witek, Jr., 1993). Tests have dealt with
airway resistance (Morgan and Camp, 1986) and
the volume and cross-sectional area of the nose cav-
ity (Grymer et al. 1989; Rasmussen et al. 1990),
nasal lavage and analysis of biomarkers, such as
leukocytes, neutrophils and histamine release (Kor-
en et al., 1992). Other parameters are attention,
performance (Malhave et al., 1986) and lung func-
tion (Harving et al., 1991; Johnsen et al., 1991).
Entering the exposure chamber, a trained panel
can evaluate the immediately perceived air quality
on the decipol scale (Fanger et al., 1988).
Traditionally, subjects have been exposed to cer-
tain VOCs or mixture of VOCs, see 6.2. In some
exposure studies, subjects have been exposed to
ETS, human bioeffluents, in addition, the emission
of VOCs from building materials and a simulated
office environment, respectively, have been investi-
gated, see 6.3.
6.2 Chamber Exposure Studies with
VOCs and VOC Mixtures
In the classic work by Malhave et al. (1986b), 62
individual SBS sensitive subjects were exposed to a
mixture of 22 different VOCs at three different
levels for 2.75 hours, see Table 6.2.1. Malhave’s
mixture of 22 different VOCs was selected on the
basis of measurements in Danish buildings and
emission testing of building materials (M~lhave,

1982). The mixture contained two major VOCs,
butyl acetate and toluene in 1 : 1 ratio ( ~ 7 3 %
weight of total mixture). The total concentration of
VOCs were 0, 5, and 25 mg/m3 and the concen-
tration of the single VOCs were about 1/10 to 11’100
of their corresponding TLV value, but still higher
than those usually encountered indoors today in
non-industrial environments.
The effects studied by M~lhaveet al. were per-
ceived air quality, mucous membrane irritation
(dryness), odor annoyance and attention quality.
The study was later repeated by others with healthy
subjects (Hudnell et al., 1992; Otto et al., 1992,
1993), and in one study with both healthy and sen-
sitive subjects (Kjzrgaard et al., 1991). The major
findings of these studies for healthy subjects were a
dose-dependent increase of mucous membrane irri-
tation and deterioration of the air quality, both at 5
and 25 mg/m3 levels, an increased sensitivity was
observed among sensitive SBS subjects at the 25
mg/m3 level. However, the difference, among
healthy and sensitive subjects was not large
(Kjargaard et al., 1991). Decreased attention, in
the form of short-term memory deficiency, was ob-
served in the study with SBS sensitive subjects, but
not with healthy subjects. A major question is
whether the sensitivity is due to hypersensitivity.
The decane study by Kjzrgaard et al. (1989)
showed that the hitherto considered “inert” VOC
could provoke increased mucosal irritation and re-
duce the tear film break-up time; however, the con-
centration was about three orders of magnitude
higher than normally encountered indoors. In ad-
dition, deterioration of the air quality was reported.
So far, the majority of reported chamber exposure
studies have been performed at concentrations sub
TLV levels, but still higher than normally encoun-
tered indoors. One rationale for the observed effects
could be (hyper)addition of VOCs, because VOCs
may act by a common physical mechanism pro-
portional to their thermodynamic activity, rather
than by a chemical mechanism as proposed by
Cometto-Muiiiz and Cain (1991-1993).
Indicators for assumed inflammatory response,
e.g. significant increase of neutrophils has been ob-
served in nasal lavage of healthy men exposed to the
same 22 VOC mixture and the increase was ob-
served even 24 hours after the exposure (Koren et
al., 1992).
In one study, Mnlhave et al. (199 1) examined the
subjective reactions at nearly “realistic” indoor
TVOC concentrations of the 22 VOC mixture.
Peder Wolkoff Volatile Organic Compounds 5 1
Lowest reported dose-response effect levels were at
3 mg/m3 for odor intensity, i.e. significant change in
perceived intensity. The lowest reported level was 8
mg/m3 for changes in perceived air quality, need for
ventilation and perceived irritation in eyes, nose and
throat.
Chamber exposure studies should be able to ex-
plain the common result found in many field studies
that women report a higher complaint rate, when
compensating for bias and confounders, than men.
Whether this finding can be rationalized in terms of
different reporting attitudes or job characteristics
and therefore possibly different environmental con-
ditions (Hodgson et al., 1991b) is still an open
question. Odor annoyance (from ETS) and mucous
membrane irritation, have been reported to depend
to some extent on gender, women being more sensi-
tive than men (Cain et al., 1987; Cometto-Muiiiz
and Cain, 1992; Cometto-Muiiiz and Noriega,
1985; Winneke, 1992). E.g., it has been shown in
chamber exposure studies that in particular, young
non-smokmg women appear to be more sensitive to
ETS than men. On the other hand, M~lhaveet al.
(1991) found that smokers responded more
strongly than non-smokers to questions about air
quality and odor intensity. However, provocation
studies with carbon dioxide have only shown weak
indications that women had an increased sensitivity
(Kjzrgaard et al., 1992). Similarly, Otto et al.
(1993) did not find any gender difference in SBS
complaint rating during exposure to the 22 VOC
mixture. A possible explanation of the observed
gender difference could be that the two genders
have attached different values to the wording used
in the questionnaire, like “acceptability” (M~lhave
et al., 1991). However, Stenberg and Wall (1995)
concluded that the excess reporting prevalence is
real and not a reporting artefact.
The time scale and adaptation of perceived mu-
cous membrane irritation and odor annoyance are
two important aspects to be considered. Both con-
stitute important parts of the overall perception of
the IAQ. Knasko (1993) found that intermittent
bursts of odor (pleasant or unpleasant) did not in-
fluence the mood, performance and the perceived
health (headache and eye irritation) (cf. the field
study by Berglund et al., 1992). The subjects, how-
ever, reported that odors had a negative effect on all
factors. Time integrated response has revealed that
perceived eye and airway irritation, generally, in-
creases over time, but the time to reach the asymp-
totic level depends on the concentration, while the
Table6.2.2 Some human exposure studies with WOCs in climatic chambers

Study vocs Subjects/ Conc. (T)VOC Methods Major effects measured

(time hours) Design mg/m3
M W Subjective Objective
Melhave et al., 22 VOCs (2.75) 23 39l 0, 5, 25 questionnaire mucous membrane irritation - brain: performance 1
1986b 0, 2, 5, 15 digit span odor intensity 1'
acoustic rhinometry
1991b (50 min) 25 double 0, 1, 3, 8, 25 split lamp - tear film quality
blind
Melhave et al., 22 v o c s (1) 10 0, 10 questionnaire sensory effects t eye: tear film -
1993 (18, 22, 26°C) digit span nose: nasal cavity area, volume 1
acoustic rhinometry
split lamp - tear film quality
Iregren et al., Butyl acetate 24 35-1 400 questionnaire eye: break-up time -
1993 (20 min, 4 hrs) eye redness lipid layer -
-
split lamp tear film quality epithelial damage -
blinking frequency redness -
blink frequency (-)
Kjaergaard decane (6) 32 31 0, 54, 189, 540 questionnaire mucous membrane irritation in eye: break-up time 1
et al., 1989 double blind split lamp, tear film eye, nose, and throat '? PMN3 t
performance air quality 1 nose: P M N -
odor intensitv 1' brain: performance -
Kjzrgaard 22 VOCs (2.5) 352 5, 25 questionnaire air quality 1 eye: PMN t
et al., 1991 digit span odor intensity tear film -
nose: P M N -
brain: performance 1
Koren et al., 22VOCs (4) 14 0, 25 nasal lavage nose: P M N T
1992
Hudnell et al., 22 VOCs (2.75) 66 0, 25 questionnaire over time odor intensity 1,
1992 30% decrease over time
Hudnell et al., 22 VOCs mix. (4) 46 0, 6, 12, 24 Odor intensity 1 adoptation
1993 IAQ 1' improved
Mucous membrane irritation T'
(concentration dependent)
Otto et al., 0, 25 performance mucous membrane eye and throat brain: performance -
1992 irritation 1'
fatigue t
mental confusion t
IAQ, some adaptation, men and
women equal
Otto et al., 22VOCsmix(4) 26 15 odor intensity 1' performance -
1993 IAQ 1
 Peder Wolkoff Volatile Organic Compounds 53

odor intensity perception showed a marked adap-

tation for high concentration up to a certain level
(Hudnell et al., 1992, 1993; Kjargaard et al., 1991)
(cf. Cain and Murphy, 1980).

osure Studies with

6.3 Chamber
7
VOCs Generate from Building
Materialsand Office Equipment
The panel evaluation of the immediately perceived
air quality on exposure to body (odor) effluents,
ETS and the emission from building materials was
examined by Gunnarsen and Fanger (1992). They
found that adaptation to the air quality within 15
minutes was minimal for building material emis-
sions, pronounced for ETS and easily achieved for
bioeffluents. The reason could be that ETS con-
tains, in the gas phase, irritative aldehydes, cf. Table
2.3.1.1, while the building materials emitted a var-
iety of VOCs of which several could have had odor-
ous characteristics, whereas some could have had
irritative characteristics, cf. Table 2.2.1.
In two other studies, subjects have been exposed
to the emission from building materials ('Johnsen et
al., 1991; Wolkoff et al., 1991b and emissions from
office equipment (Wolkoff et al., 1992), respectively.
In the latter, the subjects (all women) carried out
typical office work including photocopying, word
processing with personal computers and laser print-
ing and paper handling, see Fig. 6.3.1. In both
studies, air measurements of VOCs, formaldehyde,
ozone and particles were carried out. Simul-
taneously, subjective evaluations of SBS symptoms
and panel evaluation of the IAQ in decipol were
carried out. In addition, objective clinical measures,
i.a. eye tear film quality and damage of conjunctival
epithelium, have been measured prior to and im-
mediately after the six hours exposure period. In the
simulated office study, measurements of biomarkers
in nasal lavage and acoustic rhinometry were in-
cluded.
The building material study (Wolkoff et al.,
1991b) has shown that subjective perception of SBS
symptoms and objective measurements, such as the
tear film quality, both could be affected by the dif-
ferent mixtures of VOCs emitted at speciated
TVOC concentrations ranging from 1100-2000 pg/
m3, as well as by formaldehyde. The concentration
of individual VOCs ranged from 8-846 pg/m3. In
the simulated office study, despite considerably
lower VOC concentrations increased SBS was re-
ported. However, formaldehyde, ozone and par-
54 Peder Wolkoff Volatile Organic Compounds
ticles were all present, but in sub TLV concen-
trations except for ozone, which reached levels close
to its odor threshold. The concentrations of ozone
and, in particular, formaldehyde were both greater
in the simulated office environment than in the non-
office environment. In this study, the tear film qual-
ity remained unaltered. However, damage of con-
junctival epithelium, despite the low pollutant con-
centrations encountered, was significantly greater in
subjects exposed to the simulated office environ-
ment relative to the non-office environment. The
low TVOC concentration and the relatively high
formaldehyde concentration close to that of a WHO
guideline (1989b) could be rationalized by reactions
between ozone emitted from the office machines
and VOCs emitted from the toner powder, the
paper (Wolkoff et al., 1993a) and from other VOCs
present in the chamber air. It is known that styrene,
a common VOC emitted from office machines, is
oxidized to formaldehyde and benzaldehyde by
ozone (cf. Table 2.5.2). Additionally, carpet emis-
sions exposed to ozone have resulted in an increase
of aldehyde concentrations, TVOC and a decrease
of major VOCs (Weschler et al., 1992). The results
are compatible with a recently proposed hypothesis
that ‘lost TVOC’ and subsequent increase of form-
aldehyde could be associated with increased SBS
prevalence (Sundell et al., 1993).
Both studies demonstrated that subjective evalu-
ation of SBS symptoms, in particular eye irritation,
was compatible with the observed objective biomic-
roscopic changes in the eye (Johnsen et al., 1991).
These results are compatible with findings from the
Danish town hall study which showed that SBS
symptom prevalence correlated with lower occur-
rence of foam in the eye lid (Franck and Skov,
1989) and reduced break-up time (Franck, 1986).
Later investigations also indicated that a thick outer
fatty layer (tear film) may protect against dry eyes
(irritation) (Franck, 1991).
The building material study showed that those
materials emitting VOCs with high odor thresholds
(i.e. “odorless” VOCs) resulted in the best immedi-
ately perceived IAQ (lowest decipol value). The
simulated office study resulted in a 2.6 decipol in-
crease (worse IAQ), while the subjects performed a
standard work routine. Continuous copying oper-
ation of a photocopying machine and a laser printer
resulted in a 8.2 decipol increase from 4.5 decipol
when machines were off.
A large formaldehyde emission from a particle
board (coated with an acid-curing paint) was not
Fig. 6.3.1 Chamber exposure study with a simulated office en-
vironment Thre personal computers, one laser printer and one
photocopying machine in a 30 m3 climatic chamber
reflected in the panel evaluation of the air quality
and neither was the tear film quality affected by a
concentration about 0.75 mg/m3. The later obser-
vation may indicate that the mechanism of the “re-
active” formaldehyde may be different from that of
VOCs in general. By contrast, the reported eye and
throat irritation was significant (‘Johnsen et al.,
1991) in essential agreement with a WHO report
(1989b). The findings of both studies suggest that
the evaluation of immediately perceived IAQ within
a time frame of one min is insensitive to an irritant
like formaldehyde at ca. 1 mg/m3 level. The findings
can be rationalized by the fact that odor perception
exhibits a steeper dose-dependence than irritation
and irritation has a latency (Cometto-MuiXz and
Cain, 1991, 1992). Furthermore, odorous VOCs
may mask perceived irritation at low concentrations
(Berglund and Lindvall, 1992; Engen, 1986),
whereas the reverse may be seen at high concen-
trations (Cain and Murphy, 1980).
A marked difference in the tear film quality
affected by the different building material emissions
led to the hypothesis that lipophilic VOCs more ef-
fectively destabilize the outer fatty layer of the tear
film than hydrophilic VOCs. Figure 6.3.2 shows
that at a level of high total lipophilicity of emitted
VOCs (Wolkoff et al., 1991b) the eye tear film qual-
ity was most deteriorated. This hypothesis is sup-
ported by the observation that, despite marked dif-
ferences of the measured tear film quality, the speci-
ated TVOC in molar concentrations (ppb) were
nearly the same, suggesting that the controlling step
may not be dose-dependent, but that destabilization
or dissolution of the fatty layer which constitutes
the outer fatty layer (Meibomian oil) (Holly, 1978)

0 - M22-
-11 *4
-2 - -1
-3 - shown to cause pronounced cytotoxic effects on cul-
-4 - 0-2
controls the process. This destabilization could lead
to a thinner fatty layer and cause a decrease of the
break-up time (Norn, 1992). This again could en-
hance the access to free nerve endings. Conse-
quently, irritation caused by pollutants would be ef-
fective at lower concentrations than for an intact
fatty layer (tear film). The proposed hypothesis is
compatible with the observed decrease of break-up
time in the decane study (Kjaergaard et al., 1989).
However, a decrease was neither found in the study
with the 22 VOC mixture (Kjaergaard et al., 1991)
nor with butyl acetate at supra TLV levels (Iregren
et al., 1993). The discrepancy may be partly ration-
alized by different measures of the tear film quality,
different concentrations and the total lipophilicity
of pollutants; e.g., the lipophilicity of butyl acetate,
expressed as the % , partition coefficient, is about
four orders lower than that of decane. In the decane
study, only break-up time was measured, while re-
sults for break-up time, foam formation and thick-
ness of the fatty layer were pooled together in the
material study (Johnsen et al., 1991; Wolkoff et al.,
1991b). It has been shown that pollutants such as
paraffin oils (alkanes), silicone emulsion (Gluud et
al., 1981; Norn and Opauszki, 1977), and white
spirit vapor (Stokholm et al., 1994) reduce the fatty
layer, as well as foam formation, break-up time, and
enhance damage of the conjunctival epithelium.
Likewise, it is known that the ionic and surface ac-
Peder Wolkoff. Volatile Organic Compounds 55
tive benzalkonium chloride reduces the surface ten-
sion and destabilizes the tear film (Holly, 1978; Wil-
son et al. 1975). Surface active species, such as ionic
surfactants are known to be eye and skin irritants,
and also to cause respiratory irritancy (Chiuchta
and Dodd, 1978; Kreiss et al., 1982). (A common
detergent, sodium dodecyl sulphate, has been
tures of oral mucosa epithelium (Arenholt-Bindslev
et al., 1992; Bleeg, 1990)).
So far, as pointed out by Franck and Skov
(1989), it is not known whether e.g. reduced foam
formation causes changes of the tear film or vice
versa. It is noteworthy that the tear film quality was
unaffected in the office environment study; only epi-
thelial damage was observed and vice versa in the
building material exposure study. The different ef-
fects could be rationalized in terms of different com-
binations of pollutant levels and user specific related
work requirements, e.g., VDT work in the simu-
lated office study.
6.4 The Association between Field
Studies and Chamber Exposure
Studies
The results of the ofice environment study are in
agreement with findings obtained in recent field
studies. Kjaergaard and Brandt (1993) found an as-
sociation between an increased concentration of
polymorphonuclear neutrophils in the eye and VDT
work (cf. Franck, 1986). VDT work has been as-
sociated with increased SBS prevalence (Nunes et
al., 1993; Skov et al., 1989; Stenberg et al., 1993;
Stenberg and Wall, 1995) and the same has been
reported for paper handling (Fisk et al., 1993). The
use of computers, however, was not found to be
significantly associated with SBS prevalence in the
study by Fisk et al. (1993), but use of photocopy
machines (Sundell et al., 1994) (see also Wallace et
al., 1993) and handling of carbonless copy paper,
have been found to be associated with increased
SBS (Fisk et al., 1993; Skov et al., 1989; Taylor et
al., 1984). In addition, Kjaergaard and Brandt
(1993) in their field study found that micro damage
of the conjunctival epithelium was weakly associated
with photocopying. The reactions of pollutants
emitted from office machines, i.e. formation of reac-
tive species by reaction with ozone (Eggert et al.,
1990; Schnell et al., 1992; Weschler et al., 1992;
Wolkoff et al, 1992, 1993a; Zhang et al., 1994a,b)
(cf. Tables 2.3.2.1 and 2.5.2), could be another
56 Peder Wolkoff. Volatile Organic Compounds
rationale for the observation of increased SBS
prevalence in the simulated office study. Menzies et
al. (1993) found that eye irritation was associated
with dust and outdoor pollutants (COYNO2 and
ozone). Dust particles have been shown to cause
eye redness (Kjaergaard and Pedersen, 1989) and
deposition of particles during VDT work could also
contribute to destabilization of the outer fatty layer
of the tear film (Schneider et al., 1994) (cf. Stock-
holm et al., 1982). In addition, the use of make-
up has been found to be an important confounder
regarding reported eye irritation (Franck, 1991;
Franck and Skov, 1989; Kjaergaard et al., 1993).
The overall results from the studies of building
materials and office environment suggest that evalu-
ation of the indoor climate should be cautious (Wol-
koff et al., 1991b, 1992). Neither VOCs or any
other indoor pollutant should be considered inde-
pendently. The cumulative exposure of pollutants
and user-related exposure, e.g. VDT work and the
amount of paper handling should be considered. In
addition, the impact of other exposure loads, e.g.
temperature, noise and cold draughts (Clausen et
al., 1993a; M0lhave et al., 1993; Wyon and Wyon,
1987).
Based on the combined results of reported field
investigations and the simulated office study, it is
proposed that eye irritation may be enhanced by at
least three types of exposure: chemical, physical
(e.g., particles and thermal climate including
draught) and specific activities (e.g. VDT work).
This is in agreement with the multi-pollutant ex-
posure approach applied by Menzies et al. (1993)
and the conclusion that the cause of indoor ocular
troubles are multifactorial (Norn, 1992). Further-
more, the relevance of considering the work situ-
ation, e.g. VDT work, is supported by the report
that the eye blink rate appears to be lower during
VDT work than under relaxed conditions (Shu-
Hung Wu et al., 1986; Tsubota and Nakamori,
1993) and, in general, when visual tasks become
difficult (Shu-Hung Wu et al., 1986). The combi-
nation of the observed decrease of the eye blink rate
and increased ocular surface (tear film) may in-
crease the rate of evaporation, thus promoting an
instability of the outer fatty layer (Tsubota and Nak-
amori, 1993). Although, one would expect an in-
crease of the blink rate as a result of eye irritation
(Prah et al., 1993; Prause and Norn, 1987), this is
probably not the case for VDT work. Once the tear
film has been ruptured by a surface active com-
pound(s), repeated eye blinking cannot restore the
film continuity within a short time (Burstein, 1985;
Holly, 1978).
Conclusion
This document is an overview and includes some
of the thesis work of the author without going into
experimental and technical details.
The thesis studies cover several disciplines: air
sampling and strategy, analysis of VOCs in air,
emission testing of VOCs from materials with a de-
veloped micro climatic chamber and use of models
describing the emission profile over time. In ad-
dition, two human exposure studies have been car-
ried out combining pollutant measurements with
both subjective and objective clinical measures of
the impact of the emission from selected building
materials and office equipment, respectively, and
also including the use of a bioassay.
Sources. There is a plethora of different emission
sources, each with its own emission characteristics,
which contribute to pollution of the indoor air. The
contribution of building material emissions relative
to all other sources was about 50% in a new occu-
pied Danish apartment and the time to reach a rela-
tively constant concentration level was in the order
of 100-140 days (Wolkoff et al., 1991a). On a long-
term basis, the emissions from new building ma-
terials will decline. Indeed, the etiological relevance
of some building material emissions in older build-
ings has been questioned (Sundell et al., 1994). The
contribution of secondary pollutant sources and hu-
man activity related emissions will dominate the in-
door air, in particular in older buildings. For ex-
ample, office machines, VDT use and paper han-
dling (e.g. carbonless copy paper) have been found
to be associated with increased SBS prevalence
(Fisk et al., 1993; Skov et al., 1990; Sundell et al.,
1994).
Measurements. The most common approach for
VOC air sampling indoors is preconcentration on a
solid porous sorbent (e.g. Tenax TA) followed by
thermal desorption and gas chromatography. This
approach allows air sampling with a high sampling
frequency (<60 min) and long-term sampling
(weeks). The former has revealed that the TVOC
levels may show considerable temporal variations
during the workday in offices (Wolkoff, 1990b) and
long-term air sampling has shown large seasonal
variations (Wolkoff et al., 1991a). Concentration
patterns also indicate that stationary field measure-
ments so far carried out (e.g. in offices) most likely
have underestimated the “real” exposure.
It is important to ask the right questions needed
to test a hypothesis about the impact of VOCs, in
order to plan a sampling strategy. In addition,
knowledge about the source dynamics, is required,
as well as the history and the building character-
istics. Also, sampling technique, transport, storage
and analysis, all with their own set of characteristics
for selection, should be carefully chosen. At present,
it appears that TVOC as a SBS marker should be
replaced with parameters better associated with
IAQ complaints and SBS prevalence or mechanism
of action (cf. Brown et al., 1994). This could be,
e.g., biological activity expressed as the sum of irri-
tant VOCs (TVOCi,it,,,y). The activity expressed
as partial pressure of each VOC relative to its satu-
rated vapor pressure (Ferguson principle) has also
been suggested (Cometto-Muiiiz and Cain, 1991,
1992, 1993; Mdhave and Nielsen, 1992). Physico-
chemical properties such as total lipophilicity could
be a measure for eye irritation (Wolkoff et al.,
1991b). Other suggestions are VOC group fiaction-
ation (Shields and Fleischer, 1993) and rank order
assessment (Morey and MacPhaul, 1990).
Field Studies. The VOC concentrations have been
measured with a variety of methods, sampling strat-
egies and different analysis methodologies and re-
porting. Large variations in TVOC concentrations
have been measured (Wolkoff, 1990b), which may
indicate that time-integrated mean concentrations
are inappropriate for evaluation of mucosal irri-
tation and odor annoyance. Generally, field studies
have failed to identi@ associations between VOC
concentrations and increased SBS prevalence. SBS
symptom reporting was carried out simultaneously
with measurements in one study and it was found
that TVOC, light and noise were associated with a
higher SBS prevalence (Hodgson et al., 1991b).
Some studies have reported associations between
TVOC and SBS reporting, but they are less clear
(cf. Berglund et al., 1992; Brown et al., 1994). Gen-
erally, symptom reporting has been retrospective
58 Peder Wolkoff. Volatile Organic Compounds
rather than reporting during sampling, thus possibly
resulted in a higher SBS rate, cf. Berglund (1992),
in addition to recall bias (Knasko, 1993) and the
bias of approach of the study applied (Berglund et
al., 1992). Other field studies have indicated that
VOCs as a pattern rather than as a concentration
may act on the sensory system. “Lost TVOC”
(ATVOC) (Berglund et al., 1993; Lundin, 1991,
1993) may reflect “reactive” indoor air chemistry
and may follow increased SBS reporting (cf. Sund-
ell, 1994). This hypothesis, first proposed by Ster-
ling and Sterling (1983), is supported by other
studies which have shown increased aldehyde and
TVOC emissions upon exposure of textile carpets
in the emission to ozone (Weschler et al., 1992),
increased formaldehyde formation during operation
of office machines (Wolkoff et al., 1992), in ad-
dition, to increased aldehyde concentrations indoors
(Zhang et al., 1994a,b).
Material Emission Testing. Emission testing of build-
ing materials may provide dormation about VOCs
by the use of static or dynamic headspace analysis,
the latter using a climatic chamber. Some unstable
VOCs can be identified using the combination of
preconcentration of a headspace sample, thermal
desorption and GC-port sniffing technique (Wol-
koff, 1990a). Static headspace may also be used to
compare the emissions from photoprocessed paper
from office machines (Wolkoff et al., 1993a). In
complaint cases, suspected emitting sources can be
taken to the laboratory for determination of their
headspace emission profiles (Wolkoff, 1990a). Al-
ternatively, the portable micro emission chamber
(FLEC) can be applied in the field (non-destructive
testing) for source identification and in a laboratory
for emission testing (Wolkoff et al., 1991c). The irri-
tative potential of VOC mixtures emitted from ma-
terials can also be screened by bioassays (Tucker,
1993), e.g., the mouse bioassay (Wolkoff et al.,
1988, 1991b), and the active agent(s) may then be
identified by chemical analysis.
Emission testing of waterbased paints has shown
that the emission profile of high boiling VOCs may
continue for more than a year (Clausen et al.,
1991). Emission testing at different air velocities can
be used to validate models which reflect the emis-
sion process (Wolkoff et al., 1993b). Emission test-
ing of VOCs from building materials should result
in an evaluation of the materials’ impact on the L4Q
(comfort and health) on both a short-term and a
long-term basis. Although, an approach already has
been developed for labeling building materials’
emissions according to their possible impact on the
IAQ using comfort endpoints (Wolkoff and Nielsen,
1996), standardized methods are required to com-
pare emission data. Modeling can also be used to
estimate the relative contribution of a particular
source, e.g., the emission profile of styrene from
photocopied paper can be used to estimate the styr-
ene in a standard room (Wolkoff et al., 1993a).
Human Exposure Studies. Human chamber exposure
studies with single VOCs, mixtures of VOCs and
mixtures of VOC emissions from building materials
and office equipment have indicated that VOCs
may contribute to deterioration of the IAQ, in the
form of odor annoyance and mucous membrane ir-
ritation at or close to concentrations relevant for in-
door settings, i.e. about two orders of magnitude
below TLVs. Subjective perceptions of SBS symp-
toms have been found to be compatible with objec-
tive measures of the tear film quality in some
studies. Studies of the tear film quality (expressed
as break-up time, semiquantitative measurement of
precorneal fatty layer, appearance of foam at eye lid)
have indicated that it can be affected at 1-2 mgl
m3 speciated TVOC levels from building materials
(Wolkoff et al., 1991b). Also, that the total lipophil-
icity of the VOCs present could be one physico-
chemical property reflecting for destabilization of
the eye tear film. However, the action on airway
mucous membranes may be different. The immedi-
ately perceived air quality as a measure of the IAQ
and SBS marker should be used cautiously in case
of irritants, like formaldehyde (Wolkoff et al.,
1991b), because of the latency of mucous mem-
brane irritation, but also due to the fact that odor
perception before adaptation may mask irritative
perception.
Both subjective and objective effects (micro dam-
age of conjunctival epithelium) observed at indoor
relevant concentrations suggest the relevance of
considering all potential pollutants in concert (i.e.
VOCs, formaldehyde, ozone, particles), compatible
with the multi-pollutant exposure model (Menzies
et al., 1993; Wolkoff et al., 1992), rather than look-
ing at VOCs as a single pollutant entity. An inte-
grated evaluation of exposure loads should be con-
sidered including the physical exposure (e.g. particle
exposure and thermal climate), in addition to the
worker’s situation, e.g. VDT work and paper han-
dling.
The role of VOCs as causative agents leading

to increased IAQ complaints and SBS prevalence
appears to be multi-faceted and it is still not yet
clear how VOCs alone may cause SBS. Several
hypotheses have been proposed which could ra-
tionalize the possible impact of VOCs on the IAQ
and explain SBS: a) The total exposure approach,
where VOCs will exhibit a considerable additivity
despite sub-TLV levels through a nonspecific pro-
cess; b) the action of specific irritants, such as
formaldehyde or acrolein in ETS; c) the multi-pol-
lutant exposure approach (Menzies et al., 1993;
Wolkoff et al., 1992), including also the work situ-
ation (VDT) and deposition of particles (Schneid-
er et al., 1994); d) spatial variations, e.g. concen-
tration gradients (Noma et al., 1988); e) physico-
chemical properties, such as concentrations ex-
pressed as the chemical activity (Cometto-Muiiiz
and Cain, 1991, 1992, 1993; M~lhaveand Niel-
sen, 1992), lipophilicity, or reduction of the sur-
face tension of the eye tear film by surface active
substances (Franck, 1991; Wolkoff et al., 1991b);
f) the possibility of odors triggering certain symp-
toms, in addition to noise, lighting and tempera-
ture (Clausen et al., 1993a); g) reactive species,
e.g., formed by indoor air chemistry (Sundell et
al., 1993). In addition, VOCs adsorbed on par-
ticles have been suggested to form an efficient sen-
sory stimuli (Berglund and Lindvall, 1986).
Research Implications. So far, the research has fo-
cused on VOCs and the reactive formaldehyde and
has tried to rationalize the health impact accord-
ingly. Future research activities on VOCs and other
indoor pollutants are still needed, in order to ident-
ify the etiology of deteriorated IAQ and SBS. It ap-
pears from this overview that the following research
topics would be necessary and fi-uitful:
The etiological fraction of SBS prevalence from
indoor sources, e.g. building materials’ emission
relative to daily activity related and other salient
Peder Wolkoff: Volatile Organic Compounds 59
sources, including human bioeffluents should be
studied. The identified associations of SBS
prevalence with the use of office equipment and
paper (Fisk et al., 1993; Skov et al., 1989; Lden
and Karlberg, 1992; Sundell et al., 1994), daily
activity related contributions, such as use of of-
fice equipment, paper, maintenance, VDT use
and particle deposition all should be incorpor-
ated in models for evaluation. In addition, the
relatively large surface area of furniture should
prompt more studies regarding emission testing
and evaluation thereof.
Considering the huge amount of cleaning agents
used on a daily and yearly basis, it appears that
VOCs from residues and the ionic surfactants
should be important indoor pollutants to measure
in the air and particles.
There is a strong need to identify mechanisms of
mucous membrane irritation (eye and airways).
Further, the identification of reactive causative
agents and using multi-exposure approaches
should be a new way of exploring and under-
standing the etiology of SBS.
Quantification of the impact of odor sensation
on other SBS symptoms, in particular the link
between chemical emission testing of building
materials and sensory evaluation should be iden-
tified.
Field studies which combine symptom reporting
with simultaneous IAQ measurements, i.a.
VOCs and other indoor pollutants should be car-
ried out. Data should be analyzed with the use of
multivariate analysis techniques to identlfy which
VOCs and other pollutants are associated with
SBS symptom prevalence and in what context
they do so.
Field studies should, in addition to personal ex-
posure measurements, incorporate objective
(physiological) measures, e.g. deterioration of the
eye tear film (Franck, 1986, 1991; Franck and
Skov, 1989; Kjargaard and Brandt, 1993).
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