Professional Documents
Culture Documents
by
Arbejdstilsynet
Arbejdsmiljøinstituttet
This thesis has been submined as partial fulfiltment 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*
l. P. Wolkoff, L.F. Hansen, G.D. Nielsen (1988) ganic Compounds from Waterbome Paints.
"Airway-lrritating Effect of CarbonJess Copy Methods of Comparison", Indoor Air, l, 562-
Paper Examined by the Sensory Irritation Test 576.
in Mice", Envirommmt Imernational, 14, 43-48. 7. P. Wolkoff, P.A. Clausen, P.A. Nielsen, H . Gus-
2. P. Wolkoff (1990a) "Proposal of Methods for tafsson, B. Jonsson, E . Rasmusen (1991c)
Developing Healthy Building Materials - Lab- "Field and Labaratory Emission Cell: FLEC",
aratory and Field Experiments", Enviromnemal IAQ '91 Healzhy Buildings, ASHRAE, pp. 160-
Technology, 11, 327- 338. 165.
3. P. Wolkoff (1990b) "Some Guides for Measure- 8. P. Wolkoff, C.R johnsen, C . Franck, P. Wil-
ments ofVolatile Organic Compounds lndoors", hardt, O. Albrechtsen (1992) "A Srudy of Hu-
Environmemal Technology, 11, 339- 344. man Reactions to Office Machines in a Cli-
4 . P. Wolkoff, P.A. Clausen, P.A. Nielsen, L. matic Chamber", Journal of Exposure Aualysis
Mølhave (1991 a) "The Danish Twin Apartment and Enviromuemal Epidemiology, Suppl. l, 71-
Srudy. Part 1: Formaldehyde and Long-Term 96.
Measurements of VOC", Indoor Air, 1, 478- 9. P. Wolkoff, C. Wilkins, P.A. Clausen, K. Larsen
490. (1993a) "Comparison of Volatile Organic
5. P. Wolkoff, G.D. Nielsen, L.F. Hansen, O. Al- Compounds from Processed Paper and Toners
brechtsen, C.R Johnsen, J. Heinig, C. Franck, from Office Copiers and Printers: Methods,
P.A. Nielsen (1991b) "A Srudy ofHuman Reac- Emission Rates, and Modeled Concen-
tions to Emissions from Building Materials in trations", Indoor Air, 3 113- 123.
Climatic Chambers. Part II: VOC Measure- l O. P. Wolkoff, P.A. Clausen, P.A. Nielsen and L.
ments, Mouse Bioassay, and Decipol Evaluation Gunnarsen (1993b) "Documentation of Field
in the 1- 2 mglm3 TVOC Range", Indoor Air, 1, and Labaratory Emission Cell "FLEC" -
389-403. ldentification o f Emission Processes from Car-
6. P.A. Clausen, P. Wolkoff, E. Holst, P.A. Nielsen pet, Linoleum, Paint, and Sealant", Indoor Air,
( 1991) "Lon g Term Emission o f Volatile O r- 3, 291 - 297.
Contents
Ust of Studies 4
Abbreviations and Terminology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
Units . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Preface . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Chapter l - Introduetion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.1 Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.2 Volatile Organic Compounds (VOCs) . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.3 The Office Environment - The Future Occupational Environment . . . 13
1.4 Determination and Evaluation of lndoor VOC Exposure . . . . . . . . . . . . 14
1.5 Summary ofThesis Work . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
Chapter 2 - Sources of VOC in the Indoor Environment . . . . . . . . . . . . . . . 17
2.1 Introduetion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.2 Building Materials (interior use) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.3 Human Activity (2.3.1 General Aetivity, 2.3.2 Activities in the Office
environment) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
2.4 Mieroorganisms (MVOCs) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
2.5 Outdoor Air and lndoor Air Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
2.6 VOCs Reported to Have Caused IAQ Problems . . . . . . . . . . . . . . . . . . . 22
2.7 Emission Rate ......... ..... . ... ................ . ... . . ........ 23
2.8 Pollutant Source Dynamics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
Chapter 3 - Sampling Strategy and Methods of Sampling, Analysis and
Source Identification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
3.1 Sampling Overview . .. . . . . . . ...... . . . . . . .. . .......... .. ....... . 26
3.2 Sampling Strategy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
3.3 Sampling Methods ..... ... . .. . ... . ..... ....... ..... . .. . ....... 29
3.4 Analysis, Reporting, Validation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
3.5 Methods of Potential VOC Source ldentifieation . . . . . . . . . . . . . . . . . . . 34
3.6 Future Need for Sampling and Analysis .... . ... . . .. . .. ... . . . . . . .. 35
Chapter 4 - VOC Field Investigations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
4.1 VOC Field Measurements . . ...... . . . . .... . ... .. .. . .. .. .. . .. . ... 36
4.2 Association Between VOC Exposure and SBS . .. ... . . .. .. .. . .. . ... 37
Chapter 5 - Emission Testing of Materials . . . . . . . . . . . . . . . . . . . . . . . . . . . 42
5.1 Introduetion . . ............ . .. ... ........ . ........ . . .... . . .. . . . 42
5.2 Chemieal Emission Testing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42
5.3 Experimental Parameters Influencing the Emission of VOCs from
Building Materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43
5.4 Models .... . ..... ..... . .. . ........ . . . . .. . . . ......... . ..... . .. 48
5.5 Emission Testing - Other Methods . . . . ... . .. ..... . .. .. . .. .. . . . .. 49
Chapter 6 - Chamber Exposure Studies with VOCs . . . . . . . . . . . . . . . . . . . 50
6.1 Introduetion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
6.2 Chamber Exposure Studies with VOCs and VOC Mixtures . . . . . . . . . 50
6.3 Chamber Exposure Studies with Materials and Offiee Equipment . . . . 53
6.4 The Association between Field Studies and Chamber Exposure Studies 55
Conelusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 60
7
Units
Preface
Indoor air research is a multidisciplinary science. It chamber exposure studies and carrying out the
became clear to me that an understanding of the clinical investigations. Discussions with Dr. C.
possible impact of volatile organic compounds Franck about the tear film have been much appreci-
(VOCs) on the indoor air quality in non-industrial ated.
buildings would inelude several disciplines. This in- I am grateful to associate professor Ole Albrechtsen
cludes methodologies of how to sample and ana- and his staffat The Danish Technical University
lyze, knowledge of sources and their emission (Lyngby) for his help with conducting the chamber
characteristics, and methods for field investigation, studies.
in addition to climatic chamber exposure studies. I am indebted specially to senior scientise Peter A.
And finally, methodologies for evaluation of the im- Nielsen for Iong-term collaboration and many fruir-
pact o n man of the emission from building materiais ful discussions and to senior scientist, Ph. D. L. Gun-
and office equipment. uarselt for collaboration, both at The Danish Build-
The aim of this thesis is to provide an overview, ing Research Institute.
from a chernist's point of view, of the various A Danish-Swedish joint project resulted in devel-
sources of volatile organics encountered in the in- opmem and documentation of the Field and Laba-
door environment. I intend the thesis to be an inspi- ratory Emission Cell (FLEC). I am indebted to
ration for researchers to perform research about the M.Sc. Hans Gustaftson and B.Sc. B. Jonsson at The
role ofVOCs in cernbination with other indoor pol- Swectish National Testing and Research Iostitute for
lutants on indoor air quality and the impact on their contribution.
man. I thank associate professor, D.Med.Sc. Lars
This work would not have been possible without Mølhave at the Institute of Environmental and Oc-
the langstanding interest and eneauragement from cupational Medieine (Universicy of Aarhus) for col-
director-general, D.Med.Sc. Ib Andersen of this insti- laboration in the Danish Twin Aparonent Study.
tute, who initiated me into this research field. I wish to express my gratitude to Mrs. Inger
Most of the work presented in this thesis has been Johausen, Mrs. Birthe Kvamm, and B.Sc. Elke
based on team work. It is with great pleasure that I Rasmusen for carrying out the GC work, and spedal
thank all my co-authors for fruitful collaboration. thanks to Mr. Kjeld Larsen for technical support and
I am indebted to my Iong-term co-worker, M.Sc. performing the GC/MS work.
Per A. Clausen, who did a great deal of the modeling Mrs. Kirsten Selmer Pedersen and Mrs. Lisbeth Ro-
work. Also, I thank statistician, Ph.D. E. Holst for senmejer are thanked for their secretarial assistance.
statistical advice and assistance. The valuable linguistic assistance by Mrs. bzge Frisch
The mouse bioassay tests were carried out by is much appreciated.
Ph.D. Lea E Hansen and my senior colleague, D.Sc. Several of the studies have been financially sup-
(Phamz.) Gwmar Damgaard Nielsen whom I sin- ported by The Natimtal Hottsing and Bui/ding Agency,
cerely thank for many stimutating discussions and The National Agency for Trade and bzduscry (now
support over the years. Danish Agency for Development of T rade and In-
I would like to thank M. Sc. Peter Wilhardt for per- dustry), and The Danish Wbrkiug Environmem Fund.
forming some of the hygiene measurements and Finally, I would like to thank all subjects who volun-
senior scientist, Ph.D. C. K Wi1kins for valuable as- teered in the chamber exposure studies.
sistance and input. Computational assistance was
given by Ph.D. P.A. Lund. Peder Wblkoff
I am indebted to Dr. Claus R. Johnsen (National National Institute of Occupational Health
University Hospital) and Dr. Carsten Frank (Glo- Denmark
strup University Hospital, now Chief physician, Sla- Capenhagen
gelse Central Hospital) for assisting with the May 1995
l. Introduetion
environment where a few pollutants generally are
1.1 Background dominant.
The energy erisis of the 1970s resulted in energy • Concentration levels are generally lower than
conservation measures such as tigluer buildings and threshold limit values (fLVs) (Arbejdstilsynet,
reduced ventilation requirements (Mage and 1994) up to three orders of magnitude.
Gamrnage, 1985; Esmen, 1985). New building • The number and variation of potential pollutant
scyles accelerated the use of synthetic buHding ma- sources are great.
terials, and there was a rapid increase in use of mo-
dem office technology, such as photocopying ma- The pollutants may be categorized into the foliow-
chines, computers, video display terminals, printers, ing three types:
carbonless copy paper, etc. It is generally believed
that these changes resulted in a large number of new ,l' Volatile lnorganic Compounds
and (possibly) higher concentrations of organic in- 1. Gases and vapors '\,
door air pollutants, in particular in new buildings Volatile Organic Compounds•
2. Particulnle maner, including radianerive parricles and cn-
(Brown et al., 1994; Lebret et al., 1986; Van der vironmcnlal lobacco smoke (ETS)
Wal et al., 1991). 3. BiologicaJ air contaminants (bactcria, microfungi, clc)
The widespread discontent with perceived de- • - WOCs, VOCs, SVOCs (scc Tablc 1.2.1)
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 1.2 Volatile Organic Compounds
1989a). The SBS term denates a camplex of non- Volatile organics are a broad range of compounds
specific symptoms in more than 20% of the work with boiling points from Jess than ooc to about
force . The symptoms are irritation of mucous mem- 400°C, WHO ( 1989a) has classified these into four
branes of the eye, the nose and the throat, and CNS categories, see Table 1.2.1. The classifkation was
related, such as headache, fatigue and difficulties of based on compound volatility. This overview deals
concentration. Relief of the symptoms usually oc- in particular with volatile organic compounds
curs upon leaving a building. The most commonly (VOCs), i.e. those having boiling points from 50-
reported IAQ and SBS complaints are stuffy air, l 00°C to 240-260°C. The molecular weight range
odor annoyance, and mucous irritation. It is aften is from 50-70 to about 300 dalton. VOCs exist
hypothesized that increased SBS prevalence has a mainly in the gas phase in the temperature and hu-
multifactorlal etiology (Mendell, 1993: Mølhave, midity ranges encountered indoors. SVOCs and
1991) andmayarise from different exposure loads, VOCs overlap to same extent and there is no clear
e.g. pollution, thermal, and psychosocial loads. In- dislinetion except boiling point and vapor pressure.
creased ventilation does not appear to be a panacea Aldehydes, in general, are also considered in this
for improving IAQ Gayjock, 1994), since ventilation overvtew.
systems have been found to be responsible for re- VOCs are ubiquitous in the indoor air. Several
duced acceptability among a panel o f judges (Fan- hundred organic compounds have been found in
ger et al., 1988). the indoor environment (Brown et al., 1994; WHO,
The IAQ is i. a. influenced by the universe of in- 1989a). The major classes are shown in Table 1.2.2.
door air pollutants. These are characterized by the They are further characterized by their indoor/out-
following: door concentration ratios. For typical indoor related
VOCs, the ratio is larger than one (Daisey et al.,
• They represent a camplex mixture of pollutants. 1994; De Bortoli et al., 1986; Cohen et al., 1989;
The number of pollutants encountered aften is Lebret et al., 1986; Lewis, 1991; Wallace et al.,
greater than found in the traditional occupational 1991). In addition, VOC concentrations are cha-
12 Peder Wolkoff Vololt'e Orgonic Compounds
racterized by great variation both in time and space concentrations are found in major national studies
characterized by the source dynamics (see 2.8) and from Canada (Otson et al., 1992a), Germany
the building characteristics (Harrje, 1991). The lat- (Krause et al., 1991; Seifert et al., 1989a), The
ter is expressed by e.g. the great number of different Netherlands (Lebret et al., 1986; Van der Wal et
building types and ventilation systems applied. al., 1991), Italy (De Bortoli et al., 1989), European
The concentrations encoumered indoors usually Parliament (De Bortoli et al., 1990), France (Bar-
are sub TLV levels, below airway irritation chres- guil et al., 1990) and United States (Shah and
holds, but they may be above odor thresholds. Singh, 1988; Wallace et al., 1987a). The individual
VOCs measured indoors, therefore, are generally VOC concentrations range from nglm 3 to mglm3 •
considered "non-reactive" as single substances, ex- An Arnerlean database showed that the majority of
cept for formaldehyde and acrolein. An association 66 indoor VOCs ranged from 0.4 to 4 ~glm3 as-
between VOC concentrations and increased SBS suming an average molecular weight of l 00 (Shah
prevalence is not straightforward, probably due to and Singh, 1988). This agrees with the Australian
the hypothesized multifactorlal etiology of SBS. review in which the mean concentration of single
Particles, in particular floor dust, can aet as carriers VOCs, generally was found to be below 50 ~glm3 ,
ofVOCs and SVOCs (Gebefiigi, 1989; Wolkoff and with most below 5 ~glm 3 (Brown et al., 1994). Peak
Wilkins, 1994) thus making resuspension of de- concentrations, however, will depend on the dy-
posited dust on the skin an alternative exposure namics of the indoor environment and the sampling
pathway to inhalation. Water soluble WOCs like strategy.
formaldehyde may also be carried by dust Qualitarive studies o f white collar workplaces by
(Kirchherr et al., 1992; Roehenberg et al., 1989), in north Arnerlean govemment agendes have indi-
addition to surfactants (Kreiss et al., 1982). cared that indoor contaminants and building fabric
A listing of VOC concentrations measured in- consrirute about 12- 25% of eauses of IAQ pro-
doors has been compiled by WHO (1989a) and re- blems (Kirkbridge et al., 1990; Wallingford, 1988).
cently by Brown et al. (I 994). listings of measured This was based on identified problems by health
officers. A major cause appeared to be inadequate holds does not exist for airway irritation for VOCs.
ventilation, less important appeared to be outdoor Bos et al. (1992) and Schaper (1993) have reviewed
sources, and microbiological sources, see Tabte and compiled about 154 RD50 values based on a
1.2.3. The results may not be directly comparable standard mouse bioassay (ASTM, 1984). The
to European buildings due to different building RD50, the concentration inducing a 50% reduction
scyles and ventilation systems. However, when inter- of the respiratory rate in mice, has been proposed
preting these results, one should be aware of the for occupational 11..V assessment by 11..V=
srudy design, the division of causes, the possible 0.03XRD 50 (see Bos et al. (1992) for !imitations of
disciplinary bias of investigator and Jack of inter- this approach). A substantial number of 11..Vs of
vention. VOCs retleet airway irritation to a large extent
Many of the VOCs found indoors may deterio- (Comeno-Muiiiz and Cain, 1991). The difference
rate the IAQ in terms of sensory reactions such as between 8 normal working hours 5 days a week and
odor annoyance and eye and airway irritation (Berg- 24 hours spent indoors 7 days a week (continuous
lund and Iindvall, 1992: Burge and Hoyer, 1990; exposure) may lead to indoor relevant irritative
WHO, 1989a). Another important aspect is the thresholds24 h equal to about l /4X11...V. Such a
possible loss of productivicy by deteriorated IAQ value should proteet against mucous membrane ir-
caused by VOC exposure. However, productivicy is ritation because irritative effects generally have steep
difficult to measure and no clear indkation of the dose-effect relationsbips (Commeno-Muftiz and
importance of VOCs is available today (Nunes et Cain, 1991). IAQ evaluations based on ll...Vs have
al., 1993; Stolwijk and Zyla-Wisensale, 1992). been criticized (Hodgson et al., 1994; Pierson et al.,
WHO (1989a) has recognized SBS and the po- 1991 ), but this may be avoided by use of an ad-
tential role of VOCs and proposed recomrnenda- ditional common safecy factor of l O (Shoaf, 1991).
tions which included: This would result in a pragmatic "indoor 11..V24h"
of l/40 X11..V (Nielsen et al., 1995), provieled the
• Irritants should not exceed ED 10• ll...V is basedon scientific criteria (Peterson, 1992).
• Odors must not exceed ED50 • A safety factor of about 35 of Dutch 11..Vs was sug-
• Emission of VOCs from building materiais gesteet by Verhoeff et al. (1988) for indoor evalu-
should be evaluated. ation of VOC exposure.
• Source control of emissions of VOCs should be
developed.
• Methods of biological burden assessment should 1.3 The Office Environment- the
be developed. Future Occupational Environment
• Total personal exposure assessment should be North Europeans and north Americans, especially
carried out. in urban environments, spend more than 90 percent
of their time indoors, at home, at work or during
Odor (detection) thresholds of 529 VOCs have re- transport (Letz, 1990). This amount of time is even
cently been evatuateet (Devos et al., 1990). The greater for children, elderly and sick people. The
odor thresholds vary across 12 orders of magnirude, more time spent indoors the greater is the total ex-
from grams to picograms per m 3 . The majoricy of posure to indoor pollutants. It appears that more
the thresholds range from mg to J.tg per m3 • How- than 60% of the workforce work in offices or office-
ever, this does not exelude the possibility that some like environments (Wahlberg and Stenberg, 1991).
indoor VOCs not yet measureel may have thresholds This proportion of people is anticipated to increase
in the nano to picogram per m 3 range, e.g. unsatu- during the next decades because of modem tech-
rated aliphatic aldehydes (Von Ranson and Belitz, nology, e.g. the use ofVDTs and encapsulated ma-
1992). In addition, the individual sensitivity also has chinery. An increase of people working at home is
a wide variation. While odor complaints may not be also anticipated (Mage and Gammage, 1985).
directly responsible for serious health effects, they Woods (1989) has estimated that about 20% of
are still considered unacceptable in the industria- all office workers who are exposed to an office eli-
lized world (poor IAQ) and may result in reduced mate would have adverse health effects like SBS
produetion and low morale (McJilton et al., symptoms. The symptom prevalence of eye and air-
1990). way irritation and CNS related symptoms in the
A list as comprebensive as that for odor thres- Danish town hall srudy was 26% and 23%, respec-
14 Peder Wo lkoff Volot e Orgonic Compounds
tively (Skov et al., 1989). Similar ratings have been partant and their impact on the IAQ may be greater
found in other studies (Mendell, 1993). Norback than that of bioeflluents from humans (Gunnarsen
and Edling ( 1991) fo und that in a normal Swedish and Fanger, 1992).
population 16% reported eye irritation experienced
during the last three months, nose and throat irri-
tation 19% and 13%, respectively, l 0% had experi- 1.4 Determination and Evaluation of
enced headache, and 30% fatigue. Complaint lncloor VOC Exposure
symptoms have been reported up to 50-60% We experience in the office environment a variety of
(Kreiss, 1989). different exposures. These are chemical, physical,
Four out of 50 patients, examined by a medical biological, and psychosocial. The removal rate of
doctor, indicated office machines as the cause of VOCs is determined by the nature of ventilation
complaint (Terr, 1986). In a tater review, including and ad- and desorption characterisnes of materiais
additional 40 patients which also claimed "environ- within a room and in addition to cleaning. Basically,
mental illness", 19 had the office environment as there are two major approaches for evaluation of the
their workplace (Terr, 1989). lt is striking that air- exposure to chernicais in indoor air. These are l)
way irritation and skin problems are more frequent measurements of VOCs in the indoor environment
in the office environment (Wahlberg and Stenberg, combined with epidemiology, 2) human exposure
1991) relative to other non-industrial environments. studies with VOCs, emissions from materiais and
One ubiquitous symptom is the perception of dry machilles in climatic chambers, and in addition to
air despite relative humidicy in the accepted range chemical, physical, sensory and biological emission
20-60% (Eide et al., 1992). Sundell and lindvall testing of building materials, produets and equip-
(1993) considered this perception an importane in- ment in the laboratory.
dicator of increased risk of SBS prevalence. lt is importane in this context to distinguish be-
The Danish town hall study showed that the use tween the different purposes of indoor air sampling
of office machines, VDT work and handling of and occupational hygiene sampling, respectively.
paper was associated with eye and airway irritation The latter should proteet against adverse health ef-
as well as with CNS related symptoms (Skov et al., feers. The purpose of indoor air sampling has ex-
1989} and in agreement with Sundeli et al. (1994), panded to inelude emission testing for control of
in particular with regard to photocopy machines as IAQ and prevention of discomfort problems, such
a pollutane source. Similarly, other research groups as odor annoyance including eye and airway irri-
have found that handling of copying paper was as- tation, in order to minimize SBS prevalence, in ad-
sociated with reported symptoms (Fisk et al., 1993; dition to exposure assessment, see Tabte 1.4.1.
Taylor et al., 1984) and Kjærgaard and Brandt
(1993) found a weak association between photo-
copying and micro damage of the conjunerival epi- 1.5 Summary of Thesis Work
thelium. There are only a few cases reporting symp- In view o f the need for multidisciplinarity in indoor
toms related to the use of office equipment, like a air research, and in particular in the evaluation of
laser printer (Skoner et al., 1990), a photocopying the possible link between VOC exposure and SBS
machine (Gallardo et al., 1994; Selner and Stau- prevalence and deteriorated IAQ, the studies pre-
denmayer, 1985) and heat sensitive paper (Tencati sented in this thesis had several goals.
and Novey, 1983). The use of carbonless copy These were:
paper (Buring and Hennekens, 1991) and VDT
work (Scansetti, 1984; Stenberg et al., 1993; • To obtain information about VOC sources and
Wahlberg and Stenberg, 1991) have also been of their emission characteristics (Chapter 2 and
concern in some cases. studies 2, 3, 4, 5, l 0) .
Fanger and his group (1988) found that the im- • To develop a method for VOC sampling and
mediately perceived air quality was decreased, 25% analysis, to define sampling objectives and strate-
by ETS and various activities, 13% by the users gies and to develop methods for identifying ernit-
themselves (bioefiluents}, 42% by the building ma- ting VOC sources in the field in relation to alter-
terials and 20% by the ventilation system. This im- native methods available (Chapter 3, studies 2
plied that the emission of pollutants from both the and 3).
building materiais and the ventilation system is im- • To measure VOCs in city halls with a high samp-
Peder Wolkofl: Volatile Orgonic Compounds 15
Table 1.4.1 Objectives ol indoor o ir sampling versus occupotional hygiene air sampling
Objective Purpose
lndoor air sampling 1 Control of IAQ and exposure assessment. Prevention of discomfort (e.g. odor an-
noyance) and eye and airway irritation (i.e. incrcased SBS prevalence)
Proteetion against adverse hcalth cffccts
Matcrial/cquipmcnt emission testing Dcvclopment of hcalthier materials, better equipmcnt and produet control.
Exposurc asscssment by quantification of sourcc strengths
Occupational hygiene air sampling Proteetion against adversc health effccts, cxposurc asscssmcnt
l ) Sec also Tabte 3.3.2.
Jing frequency and to review and relate the results Some guides for indoor VOC sampling are pre-
to other field studies (Chapter 4, study 3). sented (Wolkoff, 1990b).
• To develop methods for measuring the emission
of VOCs from building materiais and office Study 4. VOCs and formaldehyde were monitored
equipment, to develop models describing the in two new twin apartments (one vacant during the
emission rate over time, and to explore the use of measuring period) were monitored over a one year
a bioassay as a potential emission test for airway period. VOC and formaldehyde concentrations are
irritation. Finally, to relate chemical studies to discussed in terms of the influence of occupancy,
other methods of materlal testing (Chapter 5, age, activity, and season. A guide for a "flushing
studies l, 2, 5- 7, 9, 10). out" period prior to occupancy is proposed (Wol-
• To study the impact of VOC emissions from koff et al., 199la).
building materiais and office equipmem on per-
ceived IAQ. Additionally, to anempt to link VOC Study 5. A combined multidisciplinary study with
exposure to physiological measures such as the subjects exposed to the emission of VOCs from
tear film quality and finally to relate these results building materials. The VOC emission results are
to other chamber studies including field studies discussed in terms of the immediate perceived air
(Chapter 6, studies 5 and 8). qualicy in decipol, the tear film quality, and a mouse
bioassay. A proposed mechanism for eye irritation
The major findings of the ten studies l to l O are is presented (Wolkoff et al., 199lb).
shown below:
Study 6. The emission of VOCs from waterborne
Study J. First example of an animal bioassay applied paints has been measured in climatic chambers and
to a materlal used indoors: carbonless copy paper. monitored over a one year period. A general prin-
The results were comparible with reported symp- ciple has been developed for ranking of building
toms and a large formaldehyde content of the copy materiais with regard to their emission into the in-
forms (Wolkoff et al., 1988). door air environment (Clausen et al., 1991).
Study 2. Approaches for developing "healthy build- Study 7. A portable, handy, and inexpensive field
ing materiais" are presented and discussed. Three and laboratory emission cell (FLEC) for the mea-
cases are presented and discussed. Gas chromato- surement of VOC emissions from pianar building
graphy has been combined with a snifting technique materiais has been developed, tested and compared
to identify malodorous VOCs ernined from a build- with a small clirnatic chamber for repeatability and
ing sealant. An example of comparing emission pro- reproducibility. The FLEC has been used in the
files of selected building materiais with measured field on different sunaces and the results compared
room air (Wolkoff, 1990a). with room air sampling (Wolkoff et al., 199lc).
Sntdy 3. The experience of room air sampling of Study 8. Subjects have been exposed to a sirnulated
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 Orgonic Compounds
The results showed that the subjects' perception of processed paper and modeling carried out (Wolkoff
SBS symptoms was comparible with the decipol et al., 1993a).
evaluation and damage of the conjunerival epithe-
lium as the only clinical objective measure, despite Smdy 1O. Using the Field and Labaratory Emis-
overall very low exposures (Wolkoff et al., 1992). sion Cell (FLEC) the emission processes of se-
lected VOCs from three pre-conditioned building
Srudy 9. To investigate the emission of VOCs from materials: a carpet, a waterbome paint, and a seal-
office machines, their toner powders, and the pro- ant, have been identified by modeling of the emis-
cessed paper. It shows that processed paper emits sion profiles over time. One material, linoleum,
many different VOCs, due to toner pawder emis- apparently had not reached a stable concentration
sion, persistently for several days. The emissions gradient in the materlal or oxidation may have oc-
have been measured quantitatively and compared. curred to give good modeling (Wolkoff et al.,
The emission profile has been determined for one 1993b).
2. Sources ofVOCs in the lndoor Environment
Tab le 2.2.1 Selecled exomples ol VOC sources- Building re lo led moleriels !for indoor use)
la ble 2.3.1. 1 Selected examples of VOC sources- human aclivily re ated emissions
Source References
Emission testing Ficld mensurement Typical VOCs cmined/measurcd
copying work (Grot et al., 1991), including smoking emission ofVOCs from wet photocopying machines
which occurs within minutes. Some aerlvities may is encountered only in North Arnerica (Daisey et
result in a Jong-term emission like painting al., 1994; Grot et al., 1991; Tsuchiya, 1988; Tsu-
(Clausen et al., 1991; Wolkoff et al., 1991a). The chiya and Stewart, 1990; Walkinshaw et al., 1987).
emission of siloxanes from the use of personal care Thirty-one VOCs withawide range ofvolatility and
produets (Shields and Weschler, 1992) may also persistence were identified from processed paper
add considerably and so does the use of fragrances from photocopying machines, laser and matrix
(Wolkoff, 1992b; Wolkoff et al., 1992). Even if the printers (Wolkoff et al., 1993a). Several of the ernit-
activity is brief, the VOCs ernined can be adsorbed red VOCs can be characterized as odarous (e.g.,
to other materiais (fleecy surfaces) (Tichenor, styrene and acrylates) or contact allergens (e.g.,
1992) and dust particles (Wolkoff and Wilkins, acrylates and azo-bis-isobucyronitrile). The emis-
1994) and be reemitted at later stages depending sion of other pollutants, from photocopying and
on the climatic conditions (Nielsen, 1988). Delayed laser printer equipment, such as ozone and par-
peak concentrations have been shown to occur after rides, however, has received much more attention
cleaning aerlvities (Gibson et al., 1991; Vejrup and (Allen et al., 1978; Eggert et al., 1990; Bruun-
Wolkoff, 1994). An alternative exposure pathway Hansen and Andersen, 1986; Olander, 1992). One
could be skin adsorption, e.g. halogenared hydro- study has indicated that the formation of formalde-
carbons from showering (Szejnwald Brown et al., byde from office machines may be significant (Wol-
1984). koff et al., 1992) and is possibly formed by reactions
of VOCs with ozone (see Table 2.5.2). The han-
2.3.2 Activities in the Office Environment dling of carbonless copy paper is another potential
Only limited information is available on VOCs VOC source (Norback et al., 1988; Wolkoff et al.,
ernined from office machines (Brooks and Davis, 1988) which has been found to be associated with
1992; Miksch et al., 1982; Sonnino et al., 1983; SBS symptoms jointly with photocopying and VDT
Wolkoff et al., 1992, 1993a), see Table 2.3.2.1. The work (Skov et al., 1989; see also Fisk et al., 1993;
Toble 2.3.2.1 l si of pollutanis emilled from office mochines ond other office equipment
Stenberg et al., 1993; Sundeli et al., 1994; Taylor fungal VOCs. Norback et al. ( 1993) detected 2-
et al., 1984). ethylhexanol and 1-octen-3-ol, respectively, in
Building materials in new buildings appear to be about 33% of bedreoms and in personal samples in
the dominating primary pollutant sources for up to 39 homes. Strom et al. (1994) found elevated total
about 12 months, see seerion 2.2, relative to other concentrations of MVOCs in buildings with odor
sources. The emission deeline depends on their problems compared with reference buildings.
emission characteristics (Seifert and Ullrich, 1987). Cultivation studies of indoor microorganisms in-
The use of office equipment, such as printers, pho- dicate that the VOC formation i.a. depends on the
tocopying machines, in addition to the emission microbial strain, but the substrate composition ap-
from processed paper (Wolkoff et al., 1993a) and pears to be even more important than incubation
cleaning and maintenance provide daily comri- time and microbial growth rates (Bjurman, 1993;
butions of pollutants. These daily periodic sources Rivers et al., 1992). The water activity within the
have been proposed to cause malfunctioning of attacked object, rather than the relative humidity, is
electronic equipment (Shields and Weschler, 1992). anether important factor determining the growth
rate (Flannigan, 1992).
Table 2.4.1 Some exomples of VOCs {MVOCs) ol m·crobrolog co erigin in indoor o 'r
Table 2.5.1 Selected exomp·es ol outdoer reloted VOC contri· Table 2.5.2 Same exomples ol secondory VOCs formed by oxi·
butions dotion
References: l, 2) Verhoeff et al., 1987, 1988. 3) Schercr et al., Styrene Formaldehyde, benznldchydc~b.~
1993. 4) Kliest et al., 1989. 5) Kuliman nnd Hill, 1990. 6) Un- and sat. hydro- Aldehydes~•
Cohcn et al., 1989. 7) Garnmage and Matthews, 1988. 8) carbons, fatty acids
Hawthorne et al., 1986. 9) Weisel and Lawryk, 1993. IO)
Hodgson et al., 1991a. 11) Wolkoff et al., 1991a. 12) Wcschler Vinyl cyclohexenc Formaldchydc and formic acid~b
et al. 1990b. 13) Pleil et al., 1989. 14) Daisey et nl., 1994. 15)
Lewis, 1991 References: l ) Grosjean et al., 1993. 2a, b) Zhnng et al.,
1994a, b. 3) Cicclioli et al., 1992. 4) Tuazoo et al., 1993
found an increase of benzene and toluene with the equivalents (Zhang et al., 1994b). The reported for-
ventilation on, while the concentration of halocar- mation of 6~methyl-5-heptene-2-one identified in
bons increased, when the ventilation was off indi- vacuum cleaner dust (Wolkoff and Wilkins, 1994;
cating local sources. Similarly, Nagda et aL (1991) Wilkins et al., 1993) is comparible with oxidation of
found that 1VOC was substantially higher at high a-pinene (Ciccioli et al., 1992).
ventilation rate during summer time (the outdoor Reactions of other terpenes with ozone result in
level was also high). formaldehyde and various ketones, see Tabte 2.5.2.
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 2.6 VOCs Repor1ed to Have Caused
other aliphatic aldehydes have been reported to be IAQ Problems
ernined from paints and paint resins after curing Tabte 2.6.1 summarizes selected cases where VOCs
(De Bonoli et al., 1985; Ullrich et al., 1982; Young, have been suspected to partially have caused some
1992). These aldehydes are very likely formed by discomfort, however, questionnaires have rarely
autoxidation processes. The exposure of carpet been used. The dominant symptoms reported have
emissions to ozone showed an increase of aldehyde been mucous membrane irritation and odor anno-
formation and TVOC (Weshler and Hodgson, yance. A classical example is the emission of ali-
1992), while a marked increase offormaldehyde has phatic amines, diamines and sulfides, including am-
been found in a simulated office environment study monia from casein containing self-leveling monar
with ozone emitting machines (Wolkoff et al., on wet concrete (Karlsson et al., 1989; Lundholm
1992). The aldehyde formation may arise, i.a., from et al., 1990). Some VOCs have low irritation thresh-
degradation of long-chain fany acids in resins and olds such as aliphatic acids and amines, or may be
linolewn Gensen et al., 1994, 1995a). Wolkoff et allergerne like shampoo constituents (Taylor and
al. (1991 a) observed an increase of hexanal in an Hindson, 1982). The VOCs may be (mal)odorous
inhabited apartment during the warm season. Some with low odor thresholds, like sulphur containing
VOCs formed by oxidative processes are Iisted in VOCs from polysulfide based sealants (Wolkoff,
Tabte 2.5.2. There are indkations that atmospheric l 990a) and 4-phenylcyclohexene from latex based
(indoor air) chemistry, e.g. reflected in an increase carpets (Hodgson et al., 1993). The VOCs ernined
of aldehydes (Zhang et al., 1994a,b), may be im- are solvent residues, additives, and reactants from
portant for understanding increased SBS prevalence the raw materials, deearnposition products, which
and loss of 1VOC from intake to exhaust air (Sun- are formed during the hardening processes and fi-
dell et al., 1993). The formaldehyde yield from re- nally secondary pollutants caused by hydrolysis reac-
actions of lirnonene and styrene, respectively, with tions (e.g. plasticizers) or by microbiological action.
ozone was found to be from 125 to 150% molar There are few intervention studies direcdy related
Peder W olkoll· Vololtle Orgonic Compounds 23
Table 2.6.1 Selecled exomples ol VOC sources reporled lo hove coused IAQ problems
to building materiais and their emission of VOCs. dard room (Wolkoff and Nielsen, 1995). Reported
In a longitudinal intervention srudy, the removal of emission rates, usually obtained from "steady state"
wall-to-wall carpets in schools resulted in a decrease measurements, are in the order of a few ._.g/(m2 Xh)
of reported SBS symptoms relative to a group not to mg/(m2 Xh) (Biack et al., 1991; Colombo et al.,
exposed to carpets (Norbiick and Torgen, 1989). 1990; Davidson et al., 1991; Miksch et al., 1982;
The carpets were 8-1 O years old, any VOC emis- Mølhave, 1982; Saarela and Sandell, 1991; Strob-
sion should have been low (decomposition or ridge and Black, 1991; Wallace et al., 1987b). The
MVOCs), and other pollutants, e.g. mites and source strength in a room is obtained by multiplying
mold, may have been removed also. the materlal area with its emission rate. Many fac-
tors can influence the emission rate, like tempera-
ture, to a less extent the relative humidicy and the
2.7 Emission Rate materlal age, for further discussion, see Chapter 5.
Most reported VOC emission rates (mass ernined Body eftluent emissions have been determined to
per area and time)) arebasedon one measurement, be about 0.2-Q.3 mg/h per kg body weight
usually the supposed "steady state" concentration (Mølhave et al., 1995), in agreement with the clas-
(Levin, 1992). From a practical viewpoint, emission sic study by Wang (1975). Isoprene appears to be a
rate constants are preferable for purposes of major body VOC with an emission ca. 30()-400 ._.g1
modeling emission profiles over time, e.g. in a stan- h (Ellin et al., 1974). Lewis and Zweidinger (1992)
24 Peder Wolkoff: Volatile Orgonic Compounds
estirnated aldehyde emission rates to 9.4 mg/h and (1982) presented a simple model with three emis-
other non-methane TVOC to l 00 mg/h in resi- sion types such as constant generation, workday
dences. generation and episodic generation. By combining
the temporal patteros with the sparlal patteros Levin
( 1992) ended up with a two-by-three matrix, see
2.8 Pollutant Source Dynamics Scheme 2.8.2, in which he distinguished between
The total indoor air pollution of VOCs comprises point sources and distributed sources each having
the combined contributions from the building re- constant, periodic (occupational) and episodic time
lated, human activity related and outdoor sources. pattems.
Each pollutant source has its own emission charac-
teristic, i.e. temporal emission and spatial patterns. The concentration-time pattern of VOCs in the of-
Figure 2.8.1 shows the deeline of the coatescent fice environment with aetlvities may vary signifi-
agent Texanol, used in a waterbome paint, in a new cantly during the working hours and depends upon
apartment over a one year period from the time of a series of imerrelated factors such as location, oc-
completion (Wolkoff et al., 1991 a). Several research cupant density and user related activity (Crump and
groups have suggesred schemes to describe the vari- Madany, 1993; Ekberg, 1994; Hodgson, 1992;
ability of di.fferent emission sources. Seifert and Johansson, 1978; Wolkoff, 1990b). This also in-
Ullrich (1987) distinguished between continuous cludes photocopying (Daisey et al., 1994; Grot et
and discontinuous emission sources. These emis- al., 1989; Hodgson et al., 1991 a) and the use of
sions may further be subdivided into those behaving personal care produets (Shields and Fleischer,
in a regular or irregular mode as shown below in 1993). The temperature, humidity, ad- and desorp-
Scheme 2.8.1. The time scale of the continuous tion processes (Borrazzo et al., 1993) and outside
type was in the arder of months or weeks while it aerlvities (Ekberg, 1994; Pleil et al., 1989) can also
proceeded within hours or minutes for the discon- contribute. On a Iong-term basis, the primary
tinuous type. Others distinguish between short and VOCs from building materiais will dominate during
long term temporal variations including spatial vari- the first year in a new building. The contribution
ations (Otson and Fellin, 1992) while Miksch et al., from daily aetlvities (e.g. office machines and other
human activities) and secondary pollutant sources
will progressively dominate the indoor air. This
JlQ·m" could be one explanation for the identified associa-
4oco~~---r--~--~~----~----~--~-. tion between use of photocopying machines and
- - Texanol
3500
•••••••• Texanol"
SBS prevalence (e.g., Sundeli et al., 1994). How-
3000. - - Ethanol' ever, SBS has not been found to be associated with
2500 : -·-Acetone
2000 --- · Acetone• the use of computers (Fisk et al., 1993).
1500 The impact of the ad- and desorption processes
1000 could be reflected in a typical office in which emit-
500 ted pollutants from human aerlvities during the
0~~~~--~~~~==~------~--
workday are adsorbed on fleecy surfaces (textiles)
"500 L..-~50"..--:-1~00"..-~15~0~2~00:-=-1'~2~50~~300=-=-~3~5~0~4~0~0~450
and shelves (paper). During the night, while the
Days
ventilation system is turned off, and over time, the
Fig. 2.8.1 Average time/ concentralion profiles ol Iong-term VOC
sampling (7 - 14 doysl ol acetone, ethanol, and Texanal in Danish equilibrium between VOCs in the air and sorbed
Twin Apartments (occupied and vacant)_ Date O(date ol building VOCs is reestablished, with a resulting increase in
completion) .. 1 November 1987. • =occupied . .!.=Date ol oc· air concentration which the occupants will be ex-
cupancy. i 20 June 1988 _{Wolkoff et ol., 1991 ol
posed to the next morning. Conversely, if the
HVAC system is rurned on ovemight with heating reduced (e.g., Grot et at., 1991; Shields and
the VOCs could be removed (Nielsen, 1988). The Weschler, 1992; Turiel et al., 1983). It was shown
association between the fleece factor (Nielsen, in the Danish town hall study that the office size
1987) and increased SBS prevalence Oaakkola et and occupant density were important parameters
al., 1994), however, has not been found in two associated with increased SBS prevalence (Skov et
other studies (Zweers et al., 1992; Sundeli et al., al., 1990). This may lead to the condusion that lo-
1994). cal pollutant sources (e.g. work stations, human ac-
The building characteristics (Harrje, 1991 ), i. e. tivities including bioeffiuents) may play a more im-
different ventilation conditions and wind direction portant role than ventilation (Farant et at., 1992;
may also play an important role and add to the vari- Hodgson, 1992; Nagda et at., 1991).
ability and temporality of indoor pollurants. Wesch- The overall source dynamics of VOCs indoors
ler et al. (1990a, 1992) found that indoor ozone are reflected in the variabilicy expressed by the fol-
concentrations may vary greatly with the time of the lowing: the plethorn of source types and their
day and this may affect the types and concentrations emission characteristics as temporal and spatial
of VOCs found indoors (Weschler and Hodgson, panems; the concentration ranges eneouncered in-
1992). Generally, TVOC levels have been found to doors. lt is important to realize that the sampling
be inversely proportional to the air exchange rate, strategies should be related to these dynamics (cf.
i.e. concentrations increased when ventilation was Chapter 3).
3. Sampling Strategy and Methods ofSampling,
Analysis and Source ldentification
Sarbent reusable
Solvent desorption 1 • 10·~ 5 Rcpeated analysis Lower scnsitivity, >4 h Solvent elurion and HRGC/ mc:~n
"
28 Peder Wolkoff: Volatile Organic Compounds
Table 3 . 3.2 Importani steps from sampling to onalysis, ond idenlilicolion ol VOCs indoors b y use ol precancenlrolion lechniques
There are six different sampling objectives as It is advisable to start an indoor complaint case
shown in Table 3.3.2. Furthermore, this Table sum- with a walk-through inspection (ECA, 1989a;
marizes sampling criteria, strategy criteria, sampling Garnmage et aL, 1989; McCharty et al., 1991) and
media criteria, storage criteria and criteria for the gather as much information about aerlvities and
analysis. evems as possible. The recognition of odors or irri-
The quality of VOC measurements is a fimetion tants may help to identify potential emitting sources
of the labaratory which is executing the methodo- and to plan the sampling strategy accordingly.
logy and its skill, competence and experience of If the sampling objective is a complaint case,
field air sampling. Sampling and analysis are expen- VOC sampling, usually, should be one of the last
sive tools and the personnel resources cover the steps of the investigation. The cost of VOC meas-
major part of the total cost (Knoppel, 1992a). urements limits the number of samples, thus the
Peder Wolkolf : Volatile Orgonic Compounds 29
selection of spaces is restricted, thus requiring a de- the ~glm 3 range thus necessitating a preconcen-
tailed sampling design. tration step. The most widely used method is sam-
The sampling methods Iisted in Table 3.3.1 have pling on a solid sorbem (porous organie polymer
different time resolutions of sampling, which pro- or carbonaceous) either actively with the use of
vides the choice of obtaining short-term and Iong- a calibrated pump or in the passive mode (diffu-
term time-integrated coneemrations. These sion) with the use of a well defined sorbent bed.
methods should be adapted according to the sam- Subsequently, the preconcentrated pollutants are
pling objectives Iisted in Tabte 3.3.2. lt is important eluted prior to a gas chromatographic analysis.
to remember that the sampling duration and the Generally, thermal desorption has been applied to
analytical sensitivity are interlinked. In principle, it porous organic polymers, such as Tenax TA, while
should be possible to distinguish between different solvent elurion has been applied to carbonaceous
emission source types in the field. Seifert and sorbents, but the use of thermal desorption is in-
Ullrich (1987) classifled sampling procedures into creasing.
five elifferen t categories of sampling duration. These The major difference between solvent and ther-
were one week, 8- 24 hours, 6Q-180 min, 5- 30 min mal elurion is the loss in sensitivity by solvent di-
and continuous monitering. Both active and passive lution of the pollutants followed by GC injection
sampling are available with the two first categories, of a small fraction of the original sample (typically
i.e., Iong-term sampling. While Iong-term sampling 0.1- 1%). The major advantage of active sampling
provides information of Iong-term time integrated combined with thermal desorption is the flexibility
mean concentrations, multiple, sequential short- in time resolution of sampling, in particular when
term samples can provide information about short- monitering short-term peak concemrations. Active
term peak eoncentrations. It should be possible to sampiers are also typically used to calleet tirne-in-
obtain information about short-term, discontinuous tegrated samples and so do not capture peak con-
(periodic) exposure events, such as activity related centrations. With thermal elution, however, only
events, traffic contribution or the effeet of a tem- one sample run is normally available. The loss of
perature increase by multiple sequential short-term WOCs and solvent overlap during chromatogra-
sampling together with a high sampling frequency. phy when using solvent desorption, e.g. carbon di-
Integrated sampling of VOCs with real-time non- sulfide, may be overeorne by use of dimethylform-
specific and semi-specific deteecion is also possible amide Gohansen and Wendelboe, 1981). An alter-
(Clobes et al., 1992; Ekberg, 1994; Garnmage and native to thermal desorption is microwave
Matthews, 1988; Wolkoff, 1987). desorption of carbonaceous sorbents in ceramic
The selection of spaces within a room for sam- tubes (Neu et al., 1982; Rektorik, 1985,; Vu Duc
pling is another important issue. Rodes et al. (1991) and Huynh, 1991; Wolkoff, 1986). Multiple analy-
have discussed the implications of concentration ses of the same sample can be achieved by ther-
gradients due to sparlal variations, in particular near mal desorption, followed by micro-concentration
point sources. Prior to selection of sampling Joea- of VOCs on activated carbon and subsequent sol-
tion it is important, depending on the sampling ob- vent microextraction at the cost of some sensitivity
jective, to consider the history, ongoing activities, (Atlas et al., 1985).
and the clirnatic conditions and sample accordingly. The choice of sampling technique depends pri-
An understanding of these parameters will also be marily on the sampling strategy required. The
a prerequisite for evaluation of the results. For ex- sampling and sorbent criteria are interlinked with
ample, it was shown that benzene and toluene from the breakthrough valurne (BTV) and required
motor bike parts migrated from crawl space under sampling volume, blank value of clean sorbent, de-
one apartmem into a neighboring apartmem during sorption effidency, analytical sensitivity and ther-
a time span of about one month which resulted in mostability of the sorbent. One sorbent eannot
delayed peak concentrations (Wolkoff et al., 1991a). fully aecommodate a complete range of VOCs
with different volatilities and polarities. The pre-
ferred sorbent should reJease the VOCs at tero-
3.3 Sampling Methods peratures below degradation of the sorbem and
Active Sampling on Sorbent should not be susceptible to artifact formation .
Themtal desorption vs. Solvent desorption. The VOC Carbonaeeous sorbents can reJease most WOCs
concentrations encountered indoors are usually in at reasonable temperatures, however to reJease
30 Peder Wolkoff· Vololo1e Organ c Compounds
VOCs and SVOCs higher temperatures are re- DiHusive Sampling on Sorbent
quired with the possibility of artifact fonnation Diffusive (passive) sampling (Brown, 1993) with
(vide infra). carbonaceous sorbents has been used extensively for
The sorbent Tenax TA has been used for more Iong-term sampling (Brown et al., 1992; Cohen et
than 20 years, the first time for detecting mari- al., 1989; De Bortoli et al., 1989; Lebret et al.,
juana smoke indoors (Novomy and Lee, 1973). lt 1986; Seifert and Abraham 1982, 1983; Seifert et
appears to be the most versatile, thennostable, and al., 1989a; Shields and Weschler, 1987, 1992; Wol-
hydrophobic sorbent for indoor measuremenes koff et al., 1991a). The main advantage of passive
available (today) for monitoring VOCs (in the sampiers is that they do not require a pump, are low
range of CrC 6 to ;o:C 18) (Health & Safety Execu- in cost, quiet, easy to use and to mail. They are
tive, 1993; Knoppet, 1992a,b; Rothweiler et al., generally used for Iong-term sampling, where peak
1991). l t fulfills many of the sorbent criteria. The concentrations eannot be monitored. Diffusion co-
range may be extended to (Cr C 5) using certain efficients o f VOCs are limited, but they can be esti-
precautions depending on the VOC polarity and mated by calculation (Nordstrand and Kristensson,
BTV. Other sorbents have been used, such as Por- 1994).
apak Q and Carbotrap Gohansson, 1978; The reported sampling duration is from about
Rothweiler et al., 1991; Wallace, 1991), but these one to six weeks, see Tables 3.3.1 and 4.1.1. Lewis
have Jimited thermal stability or high background et al. (1985) have developed a thermally desorbable
buiid-up (high blank values) during storage (Cao diffusive sample device with Tenax to overeorne the
and Hewin, 1993a, 1994a; De Bortoli et al., long sampling duration required and increase the
1992). Sarbents like Porapak Q, however, may be sensitivity. The sampling rate was camparable with
bener suited for polar WOCs (cf. Bayer, 1994). pump sampling and ppb levels were measursble
Varlous forms of carbonaceous sorbents (Bertoni within one hour. Recently, Tenax TA has been ap-
et al., 1981; Fabbri et al., 1987; Mangani et al., plied for Jong-term diffusive sampling (Brown et al.,
1982) have been investigated and multibed tubes 1992, 1993).
(e.g. glass beads, Tenax TA and Ambersorb XE- For weak sorbents, such as Tenax TA, WOCs
340) have been used (Bianchi and Varney, 1993; like benzene may be underestimated, because of
Grot et al., 1991; Tsuchiya, 1988). The advantage their relatively higher diffusion coefficients, and
of multisorbents is that a wider range of VOCs back diffusion eannot be ruled out, in particular for
can be simultaneously sampled. However, the long sampling periods (Brown et al., 1992). Al-
most therrno-sensitive sorbent deterrnines the though ideal uptake rates can be estimated with
upper desorption temperature. good accuracy, it has been shown that they change
A new Tenax version, Tenax GR (Tenax matrix to lower values over time (Brown et al., 1993; De
with 23% graphitized carbon), has recently been Bortoli et al., 1989). This implies that the uptake
introduced. This sorbent appears not to be bener rates should be determined for the required sarn-
than Tenax TA with regard to BTV in comparison plielg period (Bradshaw and Ballantine, 1995).
of B1V data from Ventura et al. (1993) with Ten- VOCs sarnpled on carbonaceous sorbents are hy-
ax TA data from Health & Safety Executive drocarbons and only a few polar VOCs have been
(1993), see also Cao and Hewin (1994a). lt has reported. This is partly due to the incomplete de-
high thennal stability, low hydrophobicicy (BTV sorption of these compounds by solvent elurion
for water, however, has doubled), but the back- using solvents of low polarity.
ground buiid-up is higher (Cao and Hewin, Another major caveat is the possibility of under-
1993a) and the recovery of e.g., p-pinene is low esrimared concentrations due to low air face velo-
(Cao and Hewin, 1993c). dties encountered in indoor environments (Gir-
Sampling of ambient air on Tenax at subambient man, 1993) which may reduce the sampling rate
temperatures has been reported (Ullrich and Sei- substantially. In addition, high humidity can reduce
fert, l 978), but water removal is required, thus in- the sampling rates (Lewis et al., 1985).
creasing the chance of retention of polar VOCs. Re-
cendy, Yokouchi et al. (1993) have reported quanti- Pitfalls (active sampling on sorbent)
tative sampling of isoprene and dimethyl sultide on Pitfalls are possible in all steps from definition o f the
Tenax TA at I5°C and they found a doubling of sampling objective to the final analysis. The major
BTV going from 20 to l0°C. pitfalls with regard to air sampling and preconcen-
Peder Wolkolf: Volot e Orgonic Compounds 31
tration on solid sorbents, not considering the as- longer (Health and Safety Executive, 1993). How-
pects of the indoor dynamics (temporal and spatial ever, sample Iass of, in particular, WOCs is poss-
variability), are the BTV, stability ofsorbent, artifact ible, if the tubes are not properly sealed (Brown et
formation (e.g. oxidative reactions) befare, during al., 1992; De Bortoli et al., 1989). Special pre-
and after sampling and dispiacement (competitive cautions to produce very low blanks, for measuring
adsorption effects of different VOCs). Finally, the in the nglm3 range have been reparted by Schmid-
method of analysis and reporting may also become bauer and Oehme (1988). However, blank values
potential errors. Tabte 3.3.2 surnmarizes potential are built up depending on storage conditions and
pitfalls associated with air sampling indoors. lang sampling durations (Cao and Hewin,
1993a,1994a). De Bortoli et al. (1992) showed that
Breakthrough volume. BTVs or safe sampling val- Carbotrap had more background buiid-up than
urnes are available for same VOCs (Brown and Pur- Tenax TA and the same was found for Tenax GR
nell, 1979; Clark et al., 1982; Figge et al., 1987; (Cao and Hewin, 1993a, 1994a).
Health and Safety Executive, 1993; Krast et al., Same sorbents, in particular the carbonaceous
1982). Recent studies have shown that BTVs may anes, retain large amounts of water, which may not
be greatly overestimated at TLV levels by use of the only reduce BTY, but also can cause degradation
indirect method (Harper, 1993). It has been recom- of the chromatographic resolution, dog the column
mended to secure a safe sampling volume, that sam- with water and may affect split ratios (Knoppet,
pling valurnes should not exceed 70% of BTV 1992b; Health and Safety Executive, 1993). Tbe
(Health and Safety Executive, 1993). lt is also choice of analytical column and GC temperature
known that BTVs are reduced by a factor of ca. programming may therefore be critical. Proper pro-
two by a l0°C increase (Brown and Pumell, 1979; gramrning starting at subambient temperature and
Harper, 1994). Reduction ofthe BTV (e.g. Porapak using several temperature ramps makes it feasible to
and Carbotrap) at increased humidity is also known identify and quantify a large range of WOCs and
(Harper, 1993, 1994; Cooper and Pellizzari, 1990) VOCs using Tenax TA as sorbent (Bianchi et al.,
and the sorbents are therefore, in same cases, Jess 1989).
suited than Tenax. It has been noted that high hu-
midity resulted in increased adsorbent resistance Artifact Formatio11. The formation of artifacts on
(Fabbri et al., 1987), causing a reduction of the Tenax by reactive air pollutants (e.g ozone and ni-
sampling valurne if the sampling flow eannot .b e trogen oxides) has been documented and may be
controlled. Measurements by the indirect method overeorne for nonpolar VOCs by a scavenging so-
at high relative humidities have indicated that BTVs dium thiosulfate irnpregnated glass fiber filter (Pel-
are about halved for organic polymer sorbents, but lizzari et al., 1984). Caution should therefore be
reduced to ane tenth for carbonaceous sorbents taken using Tenax TA inozone enriched environ-
(Health and Safety Executive, 1993; see also Clark ments (Knoppet, 1992b). The two most common
et al., 1982). Recent studies have indicated that the artifacts are benzaldehyde and acetophenone, if
indirect method may be less suitable to measure their i/o ratios are below 1.35, they may in part indi-
BTVs for VOC mixtures because competitive VOCs cate the presence of nitrogen dioxide and ozone
may displace already adserbed VOCs (Comes et al., (e.g. Daisey et al., 1994). Artifact formation and
1994; Peters and Bakkeren, 1994; Schoene et al., incomplete desorption of adserbed VOCs which
1990; Vejrasta et al., 1983; Bertani et al., 1981). either disappear or rearrange, e.g. isomerization of
For WOC analysis, the choice of sorbent may a-pinene to 3-carene or loss of haloalkanes have
become important (Bayer, 1994) as an alternative been reported (Cao and Hewin, 1993c; De Bortoli
to cooled trapping. Harper (1994) has stated that et al., 1992; Konntinen et al., 1989; Rothweiler et
the BTV may increase considerably at low concen- al., 1991; Stromvall and Petersson, 1992; Walling
trations, however, dispiacement in VOC mixtures et al., 1986). Same of these reactions are likely to
appear also to be important (Peters and Bakkeren, occur at high desorption temperatures. Artifact
1994). degradation of alkenes has also been reported (Sei-
fert and Abraham, 1983). A few VOCs have been
Stabi/ity. The stability of samples collected on Tenax reported to give unexplainable low recoveries, like
have been reported to be at least two weeks at tertiary butanal (Health and Safety Executive,
- 15°C (Knoppet, 1992b), but it is likely to be 1993). Walling et al. {1986) suggested that increas-
32 Peder Wolkoff Volatile Orgonic Compounds
ing the sampling valurne should give indication of 2. Nan-speciated TVOC (total GC!FID dececcor re-
artifact formation. sponse). Gas chromatography separation and the de-
tector response (FID) o f the total integrated area of
all separated VOCs is converted to solvent equiva-
3.4 Analysis, Reporting, Validation lents/m3, after correction for artifacts and back-
Indoor air, usually, comains several hundred VOCs ground (Grot et al., 1991). Alternatively, the total
and the identification thereof by combined GC/MS ion current from GC/MS analysis is converted,
is a major analytical task. Normally, fult MS scans usually by the use of toluene-d8 or fluorinated hy-
are required, but selected ion monitorlog (target drocarbons as standards.
compound monitoring) may be applied if certain 3. Speciated TVOC (cotal GC separated VOCs). Gas
VOCs are searched for. The number of analyses chromatography separation and summation of indi-
may be reduced, depending on the sampling objec- vidually separated and calibrated VOCs (Fellin and
tive, e.g. the objective could be certain suspect Otson, 1993; Morey and MacPhaul, 1990; Seifert,
VOCs, responsible for irritation or odors. Alterna- 1990; Shields and Weschler, 1992; Wolkoff et al.,
tively, the analytical eriterion could be that VOC 199lb).
concentrations Jess than e.g. 5 J.tg/m3 are disre-
garded in the first screening. Another eriterion of Seifert (1990) has suggested that TVOC means the
selection could be that concentrations below certain sum of GC separated and quantified VOCs (WHO
comfort or health related thresholds are disre- 1989a definition). The ten most abundant VOCs of
garded. each VOC class (- formaldehyde) (see Tabte 1.2.2)
Morey and MacPhaul (1990) have proposed that should be summed up and finally all classes pooled
the VOC measurements should be ordered in chemi- to give the TVOC value.
cal dasses and ranked according to the highest con- There appears to be both anaJytical and interpre-
centration, rather than using TVOC. WHO {1989a) tational pitfalls associated with the use of TVOC as
recommended that "To facilitate the use of data on a marker for IAQ and SBS prevalence. From an
exposure to VOCs, the distribution of the respective analytical viewpoint, VOC and TVOC measure-
concentrations should b e reported as tbe l Oth, 50th, ments depend on sampling valurne and sampling
and 90th (if possible, 95th and 98th) percentiles". mediumlsorbent type, BTVs and desorption tech-
Recendy, it was indicated that evenshort-term meas- nique applied. For example, Rothweiler et al.
urements (15 min) may be inappropriate for evatu- (1992b) showed that the choice of sorbent may be
ating mucosal irritation and it was suggested that in crucial for the determination ofTVOC. In addition
addition to the average concentration, peak concen- to the sampling pitfalls, there are the principle of
trations and the time above relevant comfort values quantitation, use of GC detector and response fac-
should be reported Gensen et al., 1995c). tors, the desorption efficiency and the use of stan-
There have been several approaches to reduce the dards. The most commonly used detector is FID
analytical costs. These inelude quantitation of the which underestimates, in particular, low molecular
immediately perceived IAQ in decipol values (Fan- weight oxygenates and halogenated hydrocarbons
ger et al., 1988). The TVOC concept (Mølhave and because of their lower FID-response Gorgensen et
Nielsen, 1992) has been suggested as another poss- al., 1990). This, however, may be overeorne by use
ible analytical short cut. There are not yet standard- of MS as the detector unit (Wallace et al., 1991). lt
ized sampling nor analytical guide for TVOC and its is not surprising that TVOC based on a total FID
impact on IAQ and health is not well understood. integrated area response can ditfer markedly from a
However, there are three basic strategies for re- TVOC value deterrnined according to Seiferts' ap-
porting TVOC. These are: proach, in particular when oxygenates or halogenat-
ed hydrocarbons are dominant (cf. Epstein et al.,
l. Non-speci'aced TVOC (direct measurement) . The 1990; Otson and Fellin, 1993; Rothweiler et aJ.,
instrument signal from a direct reading instrument, 1993). However, if the VOC composition is largely
FID and PID (Gammage et al., 1989) is converted hydrocarbons, generally, good agreement has been
into solvent (e.g. toluene) equivalents/m3. Infrared found between TVOC based on the total FID inte-
(FT-IR) (Clobes et al., 1992) and photoacoustic grated area response and the summation of single
(Ekberg, 1994) detectors can in some cases monitor VOC concentrations.
specific VOCs. A more basic problem using TVOC as an IAQ/
Peder Wolkoff: Volatile Organic Compounds 33
SBS marker is the non-specificity of TVOC. In FID or GC-MS analysis of the same air sample
other words, we do not yet know how a mixture of (Berglund et al., 1982b; Berglund and Lindvall,
VOCs is assessed by the sensory system. The major 1992) and sirnilar experiences have been found for
question is whether the TVOC concentration or a beacispace analyses of linoleum and a building seal-
defined subset, either in mass or molar concen- ant, respectively Gensen et al., 1995b; Wolkoff,
trations, can provide an adequate description of the 1990a). In other words, the two types of detectors
exposure associated with SBS prevalence without arenot always comparible (Berglund and Lindvall,
knowledge about the mechanism(s) of symptom 1992). The link between perceived IAQ and VOC
generation having been established (Berglund and concentrations is further complicated because odor
Lindvall, 1992; Brown et al., 1994). The TVOC stimulus-response relationsbips usually become flat,
concept, implicitly, assumes that there exists a dose- while pungency functions show steeper relation-
respanse relationship with VOCs concentrations. ships. (Odors follow Steven's Jaw, S= K XC", here
Morey and MacPhaul (1990) found their rank C = concentration and S= perceived odor magni-
arder assessment of individual VOCs indoors and tude, where n = 0.1- 0.8 (Cometto-Muiiiz and Cain,
outdoors, was a good approach for evaJuating build- l 991 )). The consequence is that the substantial re-
ings. Several field studies have not found relation- duction of the concentration of an odarous VOC
sbips between VOC measures and SBS prevalence. may result in littie reduction in perceived odor in-
Some studies have indicated even lower TVOC tensicy. Hypersensitivity, has been reported
levels in sick building than in healthy buildings, see (Cometto-Muniz and Cain, 1991). Weak odors are
Chapter 4. generally considered hypoadditive (Berglund and
At present, it appears that a simple VOC meas- Lindvall, 1992; Cometto-Muniz and Cain, 1991),
urement eannot be used directly to describe the per- strong odors, usually, are additive (Berglund and
ception of VOCs (TVOC) (cf. Sundell, 1994). Lindvall, 1992), but hyperadditive effects are
Therefore, it appears that further development is re- known, but not often reported (Ahlstrom et al.,
quired befare TVOC may be used as a relevant con- 1986; Arctander, 1969). lt has also been shown that
centration measure and IAQ/SBS marker. One ap- single odorants below threshold, but in mixture,
proach could be fraerianation of TVOC according may become perceptible (Patterson et al., 1993). Ir-
to VOC classes, e.g. TVOC(aromatics) (cf. Shields ritants are considered additive (Cometto-Muftiz
and Fleischer, 1993). It has been suggested that and Cain, 1991, 1992, 1993) or even hyperadditive
lipophilic VOCs may have similar irritative thresh- (Cometto-Muniz and Cain, 1993).
olds if their partial vapor pressure is divided by the Recent studies have indicated that a relative
saturated vapor pressure (Ferguson principle, cf. change of VOCs (.1-TVOC) concentrations during
Abraham et al., 1994) rather than molar concen- the workday may be better correlated with SBS
tration is used (Cometto-Muniz and Cain, 1991, prevalence than (T)VOC concentrations (Lundin,
1992, 1993). Therefore, another approach to pres- 1993; Sundell et al., 1993). In a Canadian study,
ent TVOC could be the total chemical activity ex- the best correlation with symptom reporting was
pressed as the sum of ratios over the partial and obtained using the combined effect of the total pol-
saturated vapor pressures of each VOC present lutant exposure load based on Arnerlean air quality
(Mølhave and Nielsen, 1992). Likewise, the total standards and WHO guidelines, i.e. effects of car-
lipophilicity could be another approach, cf. Chapter bon monoxide, TVOC, formaldehyde, nitrogen
6. However, one has to be aware that the chemical dioxide, dust and fungi were inelucled (Menzies et
activity, e.g. the irritative potential expressed in al., 1993). Thisis comparible with the proposed ex-
RD50 values, can vary tremendously, due to small posure model for eye irritation suggested by Wolkoff
chemical differences (Bos et al., 1992; Mølhave and et al. (1992).
Nielsen, 1992). Despite the above Iimitarians associated with the
Combined TVOC and decipol results obtained use of the TVOC measurement, it has its justifi-
from the emission of selected building materiais cation for campararive purposes (e.g. intervention
have also indicated that these parameters should be study). When the VOC profile is known or relatively
used cautiously as IAQ markers (Wolkoff et al., constant, such as in produet development, produe-
1991 b). In another study it was shown that a GC- tion control and in studies with a controlled VOC
odorgram (GC sniffing) evaluation exhibited odor profile, TVOC can also be used. For example,
perceptions with different intensities than the GC- TVOC can be measured by a direct reading instru-
34 Peder Wolkoff Volatile Orgonic Compounds
homes. Two partems were idemilled and assigned of the air (Berglund and Cain, 1989) and the per-
to mixtures of common petroleum-based solvents ceived odor intensicy (Mølhave et al., 1993a), in ad-
of differem boiling ranges. The use of multivariate dition to ligbring and noise (Clausen et al., 1993a).
statistical packages appears to be a powerful tool for However, neither high concentrations of carbon
searching of common VOC patterns. Daisey et al. dioxide Ookl et al., 1993) nor about 0.75 mglm 3
(1994) identified various sources in 12 buildings by formaldehyde concentration would be perceived by
use of multivariate analysis. The indoor sources a panel which reparts the immediately perceived air
were: dry cleaning, bioeffiuents, produets and out- quality (Wolkoff et al., 1991b). There are several
door sources like motor vehicle emission. Nelson et other factors influencing such panel evaluation, i.a.
al. (1991) identified three groups, solvent-like the different time scale of perception of odors versus
VOCs, one group of six aromatic VOCs and meth- irritants (Engen, 1986; Hudnell et al., 1993). It has
ylene chloride as a separate group. The VOC frac- been suggested that panel evaluation may be useful
tianation approach applied by Shields and Fieiseher as a total measure and identification of chemical
( 1993) identified personal care products. and biological odor loads (Moschandreas, 1992;
The impact of emissions from building materials, Cone and Shusterman, 1992).
the ventilation system, human activities including
bioeffiuents, renovation and maintenance pro- 3.6 FutureNeeds for Sampling and
cedures on perceived IAQ may be evaluated by Analysis
panel of judges and quantified, e.g. by the olf Apart from the reactive aldehydes, formaldehyde
method (Fanger et al., 1988). The panel is trained and acrolein, littie information is available about
in a standardized manner to express different ace- other species which may cause increased SBS. One
tone concentrations each corresponding to the per- theory is the indoor air chemistry, which may form
ceived air quality given in decipol values (ac- "reactive" organic species like peroxides, hydroper-
ceptabilicy rating). The evaluation provides a snap- oxides, peroxy-acetyl nitrates and radkaJs formed
shot (in Jess than l min) of the perceived air quality by reactions with ozone and nitrogen oxides. An-
when entering a room and does not necessarily re- other example of potentially irritative species is sur-
flect the overall impact of the IAQ and SBS preva- factants (cf. Kreiss et al., 1982; Taylor and Hind-
lence, in particular mucous airway irritation during son, 1982). Some of these are carried in dust par-
8 hours work. Such a method should also consider ticles. They could destabilize mucous membranes
the impact of temperature, i.e. perceived freshness due to their surface tension reduction.
4. VOC Field Investigations
Table 4. 1.1 Major national f el d studies o f VOCs measur ed i ndoors and methods applied
Table 4.2.1 Exomples ol field studies in office·like env ,ronments ond VOC meosurements !ossociotrons found with SBS prevalence)
lin alphobetic order ol lirstouthor l
Table 4.2.2 Exomples ol field studies in office·like environments ond VOC meosurements Ino associations found with SBS prevolence)
(m alphobetic arder ol lir si outhor)
had a different ventilation system and it was unoc- concentrations or VOC patteros (cf. Weschler and
cupied (Baird et al., 1987). In a foliow-up study, Hodgson, 1992). Additionally, the multivariate
it was suggesred that the main distinenon between analyses carried our, in both studies, only incor-
the healthy and sick building was "location-to- porated about 20% of VOCs (nonpolar) present in
location differences in chemistry within the build- the air. (It is rempting to draw a parallel to the
ings and not the concentrations of the chernicais finding that fluetuating exposures of m-xylene
as a whole" (Noma et al., 1988). The healthy (100-400 ppm) resulted in greater effect (body
building only exhibited minor differences with re- balance and reaction time) than a constant ex-
gard to light hydrocarbons from the outdoor air. posure (Riihimaki and Savolainen, 1980)). In a
Interpretation of the results is difficult, partly be- later study, TVOC levels in a sick building and a
cause the sick building had a different ventilation control building were both very low (ca. 80 )lg/m 3)
system, was unoccupied during VOC sampling, and so were the levels of other pollutants (par-
and it is questionable whether a 15 min air rides, aldehydes and ionic species) (Berglund et
sample, at a certain location, reflects representative al., 1992).
40 Peder Wolkoff: Volatile Orgonic Compounds
Recently, some Swedish studies have identified a possible internetion of VOCs with formaldehyde
loss of'IVOC (6 'IVOC) during transport from the and other indoor pollutants such as particles and
intake to exhaust (Berglund et al., 1993; Lundin, ozone. In one field study, in which a mobile
1993; Sundell et al., 1993). The results by Sundell chamber was anached to a sick preschool, healthy
et al. (1993) showed a weak indkation that high subjects were exposed to 170 f.lg/m 3 formaldehyde,
'IVOC in room air was associated with reduced wbile varying percentages of air from the sick build-
symptom prevalence in 29 buildings. Mean gea- ing were added. A fourfold increase in perceived
rnettic TVOC levels, however, were generally below odor intensity was observed when the "sick building
l 00 f.lg/m3 • Disregarding the generally low VOC air" was increased from l O to l 00% (Ahlstrom et
levels, the tindings are comparible with the results al., 1986).
by Baird et al. (1987), the results obtained from the Recently, it was shown that dust particles carry a
studies of the reaction of carpet emissions with large number of VOCs and SVOCs (Hirvonen et
ozone (Weschler et al., 1992) and a human ex- al., 1994; Schlitt et al., 1993; Wolkoff and Wilkins,
posure study in a simulared office environment 1994). This leads to the hypothesis that particles,
study (Wolkoff et al., 1992, see 6.3) . These Swedish though present in low concentrations, may be ad-
studiesinfer that reactive species (e.g. formaldehyde ditional important pollutanes due to their adsorbed
and acetic acid from limonene) may be formed by chemistry (e.g., the combinations of surfaetanes and
VOC reactions with ozone and nitrogen modes (cf. VOCs!SVOCs) (see also Berglund and Lindvall,
Table 2.5.2). These studies also indicate that the 1986).
relative change of VOCs or TVOC concentration Smoking is another important indoor pollutant.
may be a bener measure o f the VOCs for the identi- It is well-known that smoking increases the com-
fication of associations between VOC exposure and plaint rate (Hedge et al., 1989a; Jaakkola et al.,
SBS prevalence. In the Swedish library study, a cor- 1991; Robertson et al., 1988; Taylor et al., 1984)
relation was found between changes in the preva- and deteriarates the IAQ (Fanger et al., 1988; Gun-
lence of 8 SBS symptoms observed during one narsen and Fanger, 1992).
workday and the mean concentration of 34 VOCs Measurernents, generally, do not represem the
as measured in the exhaust air (Berglund et al., VOC concentration in the breathing zone, but
1990; Lundin, 1991 ). rather the mean time-integrated concentration
Norback et al. (1993) showed a relationship be- measured over a certain duration (from less than
tween the concentration of rwo MVOCs, 1-octen- one hour to several hoursldays) in the center of a
3-ol and 2-ethylhexanol and rated air quality. This, roorn. Concentration gradients may occur near the
despite the faet that the odor deteecion chresholds breathing zone (Rodes et al., 1991). Hodgson et al.
(Devos et al., 1990) for the MVOCs are about one (199lb) and Hodgson (1992) found that women
to two orders of magnitude higher than the meas- were exposed to higher mean concentration of both
ured concentrations. However, individual sensi- TVOC (l 00% higher) and total particles (50%
tivities can range over several orders of magnitude higher) than men. This observation could be linked
and that is not reflected in the reported odor thresh- to the general finding that women usually have
olds. higher SBS symptom prevalence, disregarding their
Finally, Menzies et al. (1993), used "that day" job category (Burge et al., 1987; Espir et al., 1988;
questions and found associations between symptom Hedge et al., 1989b; }aakkola et al., 1991; Lam et
prevalence and the combination of all measurable al., 1987; Skov et al., 1989; Stenberg et al., 1993;
pollutants, thus calling for a multi-pollutant ex- Stenberg and Wall, 1995). However, Hodgson et
posure model comparible with the proposed ex- al. (1991 b) did not find any gender differences o f
posure model for eye irritation (Wolkoff et al., symptom reporting, despite the exposure differ-
1992). ences, which agrees with a recent chamber exposure
Some studies have not yielded association be- srudy (Ono et al., 1993). Higher TVOC exposure
tween VOCs and SBS prevalence (Fisk et al., 1993; of women could be rationalized in terms of use of
De Bortoli et al., 1990; Mosehandreas et al., 1990; personal care produets inelucting perfumes (Shields
Nelson et al., 1991) or occupant perception of IAQ and Fleischer, 1993; Wallace et al., 1991 b), less of-
parameters (Moschandreas et al., 1990), see Table fice space and Jess mobility. Also, Berglund et al.
4.2.2. (1992) failed to find gender differences o f impaired
Most studies have generally not considered the performance in a sick building.
Peder Wolkoff: Volatile Orgonic Compounds 41
At present, it appears that the associations with studies have carried out objective symptom meas-
VOCs identified could also reflect the internetion of ures (e.g. physiological measures) along with en-
other indoor parameters such as the occupant den- vironmental measurements, e.g. VOCs. Future
sity and activities, concentration gradients and par- analyses of field studies should focus on the possible
ticles as VOC carriers. Hitberto unknown reactive action of VOC patteros associated with reported
VOCs formed by atmospheric (indoor air) chemis- SBS prevalence and inelude objective (physiologi-
try (Weschler et al., 1992), cf. Zhang et al. cal) measures. This should lead to identification of
(1994a,b), is another hypothesis (Sundell et al., chemical patteros and establish which VOCs could
1993), previously suggesred by Sterling and Sterling b e responsible for the perceived differences (cf.
(1983). Noma et al., 1988; Wilkins et al., 1993). Also, re-
!t should be clear from the lirerature that the as- cent findings related to indoor air chemical reac-
sociation between VOC exposure and SBS preva- tions which form "reactive species" should be pur-
lence is not yet understood, but several hypotheses sued.
have been proposed (see Conclusion). Few field
5. Emission Testing ofMaterials
Ieeted building materiais and office machines are
5.1 Introduetion presented in Chapter 6.
Development of healthier building materiais and The ultimate goal of emission testing is to evalu-
produets and produet control has been prompted ate the impact of building materiais on IAQ. Such
by an ever increasing public interest in and demand information can be used by building materlal manu-
for more environmentally friendly indoor building facturers to produce bener materiais and also en-
materiais and office equipment. lmprovement of the able building designers and architects to select the
IAQ by the use of healthy indoor materiais (Wol- best indoor environmentally friendly materials. This
koff, 1990a), i.e. materiais with low and harmless should reduce the probability of increased dis-
emission of VOCs, may be carried out by materlal comfort problems, like SBS symptoms, in particular
selection (Andersen et al., 1982) and source control in new or renovared buildings. Future evaluation of
Gayjock, 1994; Levin, 1992; Tucker, 1991; WHO, the impact ofVOCs on IAQ from building materiais
1989a), in addition to adequate flush-out periods should incorporate: l) Emission characteristics, i.e.
or increased ventilation prior to occupancy of new VOC emission profiles as function of time under
buildings. controlled conditions, transferable to real scenarios;
Until now, the objective has been emission testing 2) Knowledge of the materlal emission processes
of building materiais and describing the VOCs and and models which can predict the short-term and
their emission profiles (concentrations over time). Jong-term behaviors; and 3) Principles for establish-
Furthermore, factors influencing the emission pro- mg comfort and health criteria for ranking and
file have been investigated. The important goal selection of indoor environmentally friendly ma-
should be to relate these measurements to real terials. Additionally, the evaluation should consider
world scenarios by proper modeling. Emission test- both short-term and Iong-term effects and it should
ing of building materiais should be carried out take into account other potential emitting sources.
under controlled conditions, usually, in climatic A rating system for classitication of the emission
chambers. Technical guides thereof have already from building materiais has been suggesred by Sei-
been prepared (ASTM, 1990; ECA, 1991; Nord- fert (1992). Herated the emissions from a materlal
test, 1990; Tichenor, 1990). Only Jimited efforts according to their Jong-term effects caused by car-
have focused on the intercomparability of climatic cinogens, mutagens, terntogens and allergens, in ad-
test chambers (ECA, 1993; Gunnarsen et al., dition to short-term effects as mucous membrane
1994). The problem still remains to establish the irritation and odor annoyance, using a point system.
entire procedure from the choice of the "right" Previously, Person et al. (1991) have applied TLVs
chamber, the preconditioning of the test material, to evaluate the emission from household products.
the analysis, translate data to real scenarios and The first national system for the combinanon of
comfort and health evaluation. In addition, predic- emission testing with a health evaluation has ap-
tion of the emission profile should be possible to peared recently (Dansk Standard, 1994; Nielsen et
evaluate the impact on IAQ over time. E.g., in a al., 1994).
recent study, Mølhave et al. ( 1995) could predict
formaldehyde concentrations over time in a new
aparttnent, based on Jong-term emission testing of 5.2 Chemical Emission Testing
major materiais used in the same aparttnent. Table 5.2.1 lists the various methods used for emis-
There are several approaches to emission testing: sion testing of building materiais and produets and
chemical and sensory tests, studies of the sorption some of their advantages and disadvantages. The
properties, bioassays and human exposure studies. methods are extraction analysis, static and dynamic
This chapter deals with chemical emission testing headspace analysis, the latter using a climatic
and briefly the use of other methods, like a mouse chamber, dynamic emission testing with a climatic
bioassay, while human exposure studies with se- chamber, dynamic large scale and full house testing
Peder Wolkoll· Volatile Orgonic Compounds 43
Table 5.2.1 Emission source testing of VOCs from moleriels (modified from T chenor, 19921
• Extraction analysis:
Provides information on material's composition. It provides information of the total contcnt of VOCs to bc cmitted. lt does not,
however, provide emission raw data, i.e. the emission profile.
• Static emission testing (beadspace analysis):
Provides information about emissions' composition. Static headspacc amliysis 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 immcdiately pcrccivcd air qualicy.
Sorption propertics of materiais can be determined.
Animal bioassays can provide information about the effect of the pollutant load. In particular, thc potential irritativc effect can be
determined with a mousc bioassay.
• Dynamic large chambers:
Provide composition data and emission profile data. Human cxposure studies provide information about subjective SBS symptoms
and objective clinical measures may establish dose-respanse relationships.
• Test house studies:
Provide information about emission profile bchavior under renlistic conditions and the contribution of human activities. Rcalistic
sorption effects can be determincd.
• Field studies with a portable micro emission chamber (FLEC) :
Non-destruerive emission testing of suspected materiais to idcntify and apportion emission sources in the field. Emission testing can
bc carricd out in the laboratory.
and field emission analysis by use of a portable (Knoppel, 1992a) and so are climatic chambers. The
micro chamber (FLEC), vide infra. need for a flexible, easy to use and relatively inexpen-
Extraction can provide better information than sive chamber prompted the development of a port-
normal headspace analysis, in particular if the ma- able micro emission chamber (cell volume, 35 cm 3)
terlal contains large amounts of SVOCs (Pleil and (Wolkoffetal., 1991c, 1995). This Field andLabara-
Whiton, 1990). tory Emission Cell (FLEC) has two purposes: it can
Static and dynamic headspace analysis can pro- provide VOC emission data on suspected emitting
vide information of ernined VOCs. The former is materlal surfaces in case of problem buildings for
conveniently carried out by insertion of the sus- source identification, be used for source strength de-
pected materlal into a "non-emitting" bag filled terminations, apportionment studies and it can also
with clean air. The VOCs are identified by the com- be used in the labaratory as a climatic chamber. The
bination of headspace sampling on solid sorbent, unique feature of the FLEC is that the source (ma-
thermal desorption, followed by GC and MS tech- terlal surface) becomes an integral part of the micro
niques and, when necessary, combined with snifting chamber, see Fig. 5.2.2. Because of its design, the
of eluted VOCs (Eustache et al., 1988). Using this surface air velacity (which is proportional to the air
latter approach, malodarous sulfurous containing exebange rate) in the FLEC is under better control
VOCs ernined from a polysulfide based sealant, see than traditional climatic chambers with and without
Fig. 5.2.l.A (Wolkoff, 1990a) and odarous alde- fans. In addition, the time to reach chamber equilib-
hydes (hexanal) from a cured paint (Young, 1992), rlum has been reduced considerably for polar
respectively, have been identified. This technique SVOCs, due to the FLEC's relatively small valurne
was later used to develop a more indoor environ- compared to other small chambers and its high ex-
mentally friendly odorless sealant (Wolkoff, 1990a), change rate. Both repeatability and reproducibility
see Fig. 5.2.1B. However, instatic headspace analy- have been shown to be satisfactory for selected ma-
sis, the emission profile may be dominated by non- terlals (Roache et al., 1996; Wolkoff et al., 1991 c,
polar VOCs relative to higher boiling and polar 1995).
VOCs depending on the materlal matrix (Colombo
et al., 1991; Pleil and Whiton, 1990). Static 5.3 Experimental Parameters
headspace analysis has the advantage that the ma- lnfluencing the Emission of VOCs
terlal loading can be large increasing the analytical from Building Materials
sensitivity o f VOCs emitted. One of the goals of emission testing is transform-
Good quality (chemical) emission testing is costly ation of emission data to real senaries by modeling.
44 Peder Wolkoff: Volatile Organic Compounds
A 31
OT. AL ....
27
lO T. ••· ueø:n
8
Fig. 5.2.2 The F eld and laborolory Emission Cell "FlEC"
Age. Knowledge of emission characteristics as a strongly dependent on the AER (air velocity) and
function of age is important, because most materials almost proportional to the AER, using a first order
exhibit decaying emission profiles. This is particu- decay model including a sink effect. After the initial
lady relevant for wet produets within a short time, film formation, the emission process may change to
but some may continue emirting for several months, be diffusion controlled within the filmlmaterial. The
such as waterborne paints (Berglund et al., 1982a; emission may also be a cernbination of evaporation
Clausen et al., 1991; Wolkoffet al., 1991a; Wolkoff and internat diffusion, as suggesred by Clausen et
and Nielsen, 1993). The age is also to some extent al. (1991).
associated with materlal storage time and handling lf the emission is controlled by internal diffusion,
processes prior to testing and during analysis. The change of the AER should have minor effect on the
age or history after building completion is also re- emission rate. The emission profiles of thick layer
lated to seasonal variation (temperarure and venti- materials, e.g. carpet and sealant, could be de-
lation) as found, e.g., in the Danish Twin Apart- scribed satisfactorily by a recently developed expo-
ment Study (Wolkoff et al., 1991a). lt appears that nential diffusion model (Wolkoff et al., 1993b). This
two of the most important parameters determining was also the case for PVC flooring materiais
the outcome of emission testing are the precon- (Clausen et al., 1993b) and linoleum Gensen et al.,
ditioning period and the handling of the materlaL 1995a). lt appeared that for carpet and sealant, the
emission constants showed Jess dependence on the
Air exclta11ge rate, air velacity and co11cemration gradi- AERs which corresponded to air velocities from
em. The air exebange rate (AER) is an important 0.3-1.4 cm/s (Wolkoff et al., 1993b). linoleum,
parameter, because it reflects the amount of dilution however, behaved differently, apparendy because a
and the fresh air supply to the climatic chamber. "stable" concentration gradient had not yet been es-
Therefore, it has a major impact on the chamber tablished within the material, in addition to the
concentration. What is important in this context is possibility of oxidative degradation Gensen et al.,
whether AER or the air velacity in the material's 1996, 1995a).
surface (boundary layer) has an influence on the A concentration gradient in the boundary layer
emission rate. The mean air velocity was measured should increase the emission rate. During the early
to be 7.2 cm/sec in six occupied homes (Matthews stage o f the emission testing of textile carpets, it has
et al., 1989). The frequency distribution maximized been observed that increased AER resulted in an
at 0- 2.5 cm/s. In another study, Kovanen et al. enhanced emission rate (Sollinger et al., 1993;
(1987) measured air velocities up to 9 cm/s in Ullrich, 1990; Wolkoff et al., 1993b), in spite of a
homes and offices, but velocities up to 20 cm/s have supposed diffusion controlled emission. One ration-
been reported (cf. Girman, 1993). The impact of ale could be the composition of textile carpets
the air velocity may be strongly associated with the (backing and fibers) and the fibers themselves form
type of emission process and the identification of a boundary layer.
these is crucial for prediction of the Iong-term emis- The loading factor has also been shown not to
sion profile by modeling. affect carpet emissions under static conditions (Sol-
The emission rate of VOCs from wet materiais linger et al., 1993). However, it must be realized
(paints and lacquers) which evaporate, befare dry- that the loading factor, per se, is only a practical
ing, is likely, but not necessarily, to be controlled by parameter, providing proper charnber concen-
evaporation (Clausen, 1993). Their emissions have trations by use of standardized loadings.
been found to be sensitive to the AER (Tichenor
and Guo, 1991; Tichenor et al., 1993; Wolkoff et Atmosphen'c chemistry. The presence of air oxidants,
al., 1993b). Tichenor and Guo (1991) found that such as ozone, may influence the measurement of
the emission rate was proportional to the ratio of the emission. This has been shown for carpets for
the AER and the materlal loading (material surfacet which the addition of ozone showed not only a
chamber volume). This relationship was shown also marked decrease of styrene and 4-phenylcyclohex-
for formaldehyde (Matthews et al., 1987; Konopin- ene (latex VOCs) emissions, but an enhancement
ski, 1985; Repanen et al., 1991).1n a study by Wol- of aldehydes and TVOC (Weschler et al., 1992).
koff et al. (1993b) using the FLEC, it was shown The ratio of measured aliphatic acids over their cor-
that the emission rates for selected VOCs ernined responding aldehydes from linoleum also appeared
from a waterborne paint, a thin film material, were to depend on oxidation, because the ratio decreased
46 Peder Wolkolf Vololile Orgon,c Compounds
under anaerobic conditions (nitrogen instead of air) pet srudy by Sollinger et al. (1994), no signitkant
Gensen et al., 1996). The observed increase of e.g., dependence on hurnidity was observed for 22 cliffer-
hexanal during the summer in an occupied apart- em VOCs, except aniline which showed a weak in-
ment could be rationalized by increased oxidation crease at elevated hurnidity, prahably caused by de-
and chain scission of fany acids present in the lin- composition.
oleum floor and other fatty acid residues (Wolkoff
et al., 1991a). Other studies point to ozone as a Vapor pressure. Vapor pressure effects would gen-
cause o f increased aldehyde and add formation (cf. erally not be expected under dynamic emission test-
Tabte 2.6.2) and deteriaration of materlal surfaces ing and indoor realistic concentrations. However, it
(Weschler et al., 1990b). is possible during the initial burst ofVOCs from wet
and un-conditioned materiais that a vapor pressure
Maten"al film chickuess. The importance of the film effect may be important, because high concen-
thickness and struerure has not been studied in de- trations may be achieved in the boundary layer and
tail. The question is whether differences in the the chamber zone decelerating the evaporation.
thickness has any impact on the emission rate and Tichenor and Guo ( 1991) observed a vapor press-
emission process. Clausen (1993) showed that the ure effect for woodstain and polyurethane some
emission rate decreased on increasing the film thick- hours after application. However, TVOC concen-
ness of a waterborne paint. He has also suggested trations were 3-5 orrlers greater than normally en-
that variation of the thickness may provide infor- countered indoors. Very high materialloadings may
mation about the emission process. It is anticipated also result in a buffer effect (fichenor et al., 1990),
that a change from a solid surface (e.g. steel) to a so increased ventilation may increase the emission
porous surface will prolang the emission decay of rate of VOCs controlled by evaporation Gayjock,
e.g. paints (Gehrig et al., 1994). The difference in 1994). One study has not been able to verify vapor
porosity to a more impermeable film struerure in a pressure effects at realistic concentrations (Clausen
paint appeared also to prolang the emission profile et al., 19 90, l 9 91). The vapor pressure (chamher
of Texanal considerably (Wolkoff and Nielsen, concentration) can to same extent be controlled by
1993). the loading factor and the AER in the climatic
chamber.
Temperamre aud relative humidicy. The temperature
affects the vapor pressure and the ditfusion coef- Siuk effeccs. The impact of the sink effect is twofold.
ficients of the ernined VOCs. Therefore, the tero- The climatic chamber usually has a sink effect, i.e.
perature has a major impact on the emission rate of adsorption onto chamber walls (De Bortoli and
VOCs from building materials. This has been Colombo, l 992; Tichenor, 1992) and the materiais
shown in several bake-out studies where the VOC have adsorption (mass uptake) and desorption
concentration was enhanced by a temperature in- (mass loss) properties. The chamber sink effect has
crease (Girman, 1989). The temperature and hu- to be accounted for by necessary mathematical
midity dependence of formaldehyde reJease is well- modeling (Dunn and Tichenor, 1988). However,
known (Van Netten et al., 1989). However, it is at certain camperirive effects may possibly play a role.
present difficult to generalize for VOCs, because For example, the emission of Texanol, a high boil-
their emission may depend partly on the VOC po- ing VOC, from waterbome paints did not exhibit a
larity and the material's composition. The emission noticeable chamber sink effect in the FLEC (Wol-
of VOCs, with ditferent volatility and polarity, from koff and Nielsen, 1993) as anticipated from a pre-
a textile carpet showed dependence (increased vious srudy (Wolkoff et al., 1993b). A rationale
chamber concentrations) at elevated temperatures, could be that the most abundant VOC (propylene
most pronounced for the high boiting benzothiazole glycol), 2- 3 orrlers of magnirude greater, competed
(Sollinger et al., 1994); this was found related to by adsorption onto the chamber wall. VOCs emit-
deearnposition of an added accelerator. Similarly, ted from one materlal may adsorb onto another ma-
both Seifert et al. (1989b) and Van der Wal et al. terial and desorb depending on the climatic con-
(1994) have observed increased emission of 4-phe- ditions (Berglund et al., 1989); likewise dust par-
nylcyclohexene from textile carpets (latex backing) ticles aet as a VOC reservoir (Wolkoff and Wilkins,
and 2-ethylhexanol from PVC flooring materials, 1994). The fleecy factor (area o f the textile surfaces
respectively, by a temperature increase. In the car- over room volurne) has been shown in Danish and
Peder Wolkoff Volattle Organic Compounds 47
Finish studies Gaakkola et al., 1994; Nielsen, 1987) Sink effects may be important and they could
to correlate with SBS symptom prevalence. How- have an influence on the emission decay, in particu-
ever, this effect was not found in two other studies lar for SVOC (Ligocki et al., 1992). The sink effect
(Sundell et al., 1994; Zweers et al., 1992). The sink may extend the residence time ofVOCs and thereby
effect of materiais has been measured, usually at prolong the exposure period (Neremieks et al.,
high concentrations (Borrazzo et al., 1993; Calom- 1993; Sparks et al., 1993). In the case of evaluation
bo et al., 1993; Jørgensen et al., 1993; Kjær and of suspected building materiais the sink effect must
Nielsen, 1991; Levsen and Sollinger, 1993; Schmall be considered (Berglund et al., 1989). However,
and Seifert, 1987). steady state indoor concentrations may not be
affected if completely reversible sorption occurs, sion profiles and the associated emission constants
e.g. VOCs having vapor pressures greater than derived from the model should be independent of
torr (Ligocki et al., 1992). the climatic chamber provided the air velocity,
chamber sink and chamber concentration all are
Materia/ Homogeneity. The measurements of the under control, cf. Girman (1993).
emission rate of TVOC, 4-phenylcyclohexene, styr- A majoricy of the studies so far have been carried
ene and toluene ernined from new latex based car- out within a rather short time duration (less than
pets at different manufacturing conditions, led to one week). Generally, a first arder exponential de-
the overall condusion that evaluation of carpet cay model o f the type, R= Ro · e- k · t where R and
emission is camplex (Hawkins et al., 1992). The Ro are the emission rate at time t and t = O, respec-
emission testing was carried out l and 24 hours tively, and k= rate constant, has been applied (Dunn
after unwrapping and placernem in the chamber and Tichenor, 1988). One major finding is that the
and large variability within samples was revealed. It emission rate of some wet products, e.g. paints and
is likely that a longer term testing would have re- waxes, may be enhanced by increased AER under
sulted in a clearer pieture of the emission profile the test conditions applied.
behavior (cf. Wolkoff and Nielsen, 1993). Mass transfer models have been applied to thin
It was shown in an interlaboratory study that films (coatings) within 25 hours after application, in
sample inhomogencity should be considered with which time the transfer rate is assumed to be con-
the use of, in particular, small chambers (ECA, trolled by transfer in the boundary layer. lt is the
1993). 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-
5.4 Models terial in a 21-compartrnent model (Neremieks et
Most of the studies carried out in climatic chambers al., 1993). Finally, double exponential models have
(l.evin, 1992) have just measured the "supposed", been applied to obtain bener model fits, however,
steady state emission rate and characterized the these models do not necessarily retleet the emission
ernined VOCs under the supposition that the emis- process. l t is important that the controiling emission
sion rate was constant after a certain time. mechanism has been properly identified. Therefore,
A prerequisite for prediction of the emission rate/ models should be evaluated at least at two air velo-
profile after a certain time is knowledge about the dties (Guo, 1993). Even if a proper model has been
emission process and models associated therewith. identified there are many factors which may ob-
If the emission testing is performed under "realistic" struct modeting of primary (and secondary) pol-
and contrailable conditions, mathematical modeling lutant source emissions, in particular after long
should be able to predict the emission profile after time. Some of these are:
a certain time. If an incorrect model is applied, de-
termination of the time to reach a given emission • The pre-conditioning (duration) may be very
rate may be erroneous. For example, it was shown critical.
using a first arder decay model that the concen- • Hardening/curing process o f applied materlal has
tration of two VOCs ernined from a vinyl floor not yet finished at the start of emission testing.
covering decreased faster than predicted. An expo- • A uniform concentration gradient has not yet
nential diffusion model resulted in a bener tit been established within the materlaL
(Clausen et al., 1993). This laner model is basedon • Change of emission process may occur after a
Fiek's First Law and incorporates that the diffusion certain duration.
coefficient depends, exponentially, on the concen- • Multiple emission processes may occur from the
tration gradient within the materlaL Similarly, the same material.
emission profile of styrene from processed paper • Campering emission processes of critical VOCs.
showed a bener model fit using the exponential dif-
fusion model than a first order decay model (Wol- One approach for emission testing could be evalu-
koff et al., 1993a). ation of the impact on the IAQ and coupling to the
Tabte 5.4.1 lists some of the major tindings re- time aspect of emission decay to be able to develop
garding modeling of the emission profiles of VOCs more indoor environmentally friendly materiais and
from various building materials. ldeally, the emis- products. This could secure occupants against high
Peder Wolkoff: Volatile Orgonic Compounds 49
exposures, in particular in new buildings and after (ASTM, 1984). The method measures the sensory
renovation. The first example using modeling to de- irritation, based on analysis of the respiratory pat-
termine the necessary time to reach a certain emis- tern o f mice, e.g. exposed to the emission o f VOCs
sion rate of waterbome paints was developed and from building materials. The decrease of the respir-
used for ranking purposes by Clausen et al. (1991) . atory rate, mediared via a trigeminal or vagal reflex,
Later, Wolkoff and Nielsen (1995) have suggesred a is a measure of the potential irritance. The method
system which unifies chemical emission testing over can distinguish between sensory and pulmonary ir-
time with mathematical modeling, when necessary, ritation. The RD50, the concentration inducing a
and comfort evaluation. The principle was to deter- 50% reduction of the respiratory rate, has been pro-
mine the time value, t(Cm), necessary to reach the posed for TLV assessment (Bos et al. (1992) have
relevant indoor air value, Cm. This value was based discussed the ]imitations of this method).
on odor andfor aitway irritation thresholds in a stan- The modified bioassay was applied to carbonless
dard room of l 7.4 m 3 (Dansk Standard, 1994; copy paper forms (Wolkoff et al., 1988), later to
Nielsen et al., 1994). Coupling of emission testing paints (Hansen et al., 1991) and building materiais
o f some household produets within the first l 00- (Nielsen et al., 1996b; Wolkoff et al., 1991 b).
150 hours with TLVs and compartment modeling Formaldehyde was identified as a major causarive
has been deseribed by Person et al. (1991 ). Finally, agent for the response in the first and third studies.
Black (1992) has proposed a method to rank car- In the first srudy, it was found that a certain paper
pets according to their TVOC emission rate meas- which showed the greatest bioresponse also con-
ured 24 hours after chamber installation. The tained several hundred ppm of free formaldehyde.
method does not consider the possibility of different The bioresponse was comparible with a reported
emission profiles and it assumes that TVOC is a outbreak of complaints in a post office during han-
health marker relevant for comparison. dling of a new batch of copy forms. Similarly, a hu-
Testing should ideally be performed under con- man exposure study on building materiais showed
ditions, such that emission data can be transformed that eye and airway irritation reported in connection
to real senarios. Air velocities, when relevant, and with exposure to the emission from a partide board
specific ventilation rates (lis per m 2 ) should be re- coated with an acid-curing paint gave rise to a pro-
alistic. Ir appears at present that the emission rate Jonged bioresponse comparible with a massive
of a particular VOC depends on the concentration formaldehyde emission Qohnsen et al., 1991; Wol-
in the boundary layer above the materlal surface, koff et al., 1991 b). The method requires high ma-
more so for evaporation than diffusion controlled terialloadings, thus justifying its use for comparison
processes. However, there is still much more knowl- studies, screening purposes and selecting for de-
edge required about the impact of the various par- tailed chemical analysis and toxicological evaluation
ameters discussed above befare emission test data (Tepper and Costa, 1992).
can be properly compared. Study of the olfactory properties can also be
helpful for understanding the sensory emission of
building materiais (Gunnarsen, Fanger, 1992). Re-
5.5 Emission Testing- Other Methods cently, Jensen et al. (1995b) have compared the
One goal of emission testing is to evaluate the im- perceived (relative) odor intensities with chemical
pact of ernined VOCs on the IAQ over the time emission data from 13 linoleum products. Multi-
span from the building completion or renovation variate analysis of the data revealed that two prin-
thereof. It is not unusual that comfort and health cipal factors could explain 68% of the odor inten-
data are unavailable from the lirerature (Nielsen et sicy variation. The factors were heavily weighted
al., 1996a). Furthermore, it is difficult to evaluate for aliphatic C 6 --C8 acids and C 5 , C 7 and C 10 un-
the cumulative effects of emitted VOCs. One other saturated aldehydes, respectively. The GC/sniffing
method may be to evaluate the irritative potential of analysis of emissions and the above approach ap-
the emission. This is a bioassay based on moditi- pear to be a powerful cernbination to identify
cation of the standard ASTM mouse bioassay odorous VOCs.
6. Chamber Exposure Studies with VOCs
tation in eyes and the upper, lower airways, facial
6. 1 Introduetion skin effects, poor IAQ (odor annoyance) and other
Human chamber exposure studies eliffer from field SBS symptoms according to standardized ques-
studies in several ways. In chamber studies, environ- tionnaires (Andersson et al., 1988; Lund and Rice,
mental measurements, both subjective and objective 1992). Objeetive measurements inelude i.a. ehanges
can be performed simultaneously. In addition, some of the eye tear film physiology (Nom, 1983, 1992;
climatic parameters, such as temperature, humidity, Kjærgaard, 1992a,b). The tear film quality Gohnsen
exposure, air exebange rate can be controlled dur- et al., 1991) expressed as the pooled effect of re-
ing the exposure period. Chamber exposure studies duced break-up time of the tear film (precomeal
can provide information about dose-response re- film) (Franck, 1986), semiquantitative measure-
lationships, whereas field studies may only provide ment of reduced precomeal superficial (multi-lipid)
information about associations between exposure fatty layer (Franck, 1991), and reduced foam for-
loads and e.g. SBS prevalence. mation at inner eye lid (Franck and Skov, 1989), in
Some of the salient problems associated with addition to micro damage of the conjunerival epi-
evaluation of chamber exposure studies are: l) that thelium (Franck, 1986) have been used as measures
they do not normally mimic the source dynamics of effects of the eye. Another objective instrument
encountered indoors and therefore it may be difl:i- is the nose (Witek, Jr., 1993). Tests have dealt with
cult to extrapolate the results obtained to real world airway resistance (Morgan and Camp, 1986) and
scenarios. Furthermore, 2) the choice of subjects the valurne and cross-seetional area of the nose cav-
may be a problem with regard to representativeness, ity (Grymer et al. 1989; Rasmussen et al. 1990),
3) the sensitivity of the selected subjects and 4) nasal lavage and analysis of biomarkers, such as
power of the study (i.e. the number of subjects that leukoeytes, neutrophils and histamine reJease (Kor-
can be tested) is limited. Either the subjects are se- en et al., 1992). Other parameters are attention,
lected as particularly sensitive to the indoor elimate performance (Mølhave et al., 1986) and lung fime-
or normal, healthy subjects are selected. Although tion (Harving et al., 1991; Johnsen et al., 1991).
randomizanon is possible, it is difl:icult, in particular Entering the exposure chamber, a trained panel
with odorous VOC mixtures, to conduet the ex- ean evaluate the immediately perceived air quality
posure in a blind manner and overreporting of SBS on the decipol scale (Fanger et al., 1988).
symptoms eannot always be excluded (recall bias, Traditionally, subjects have been exposed to cer-
cf. Knasko, 1993). In faet, two field studies indicate tain VOCs or mixture of VOCs, see 6.2. In some
that odor annoyance can be associated with in- exposure studies, subjeets have been exposed to
creased SBS symptom reporting of headache, eye ETS, human bioeffiuents, in addition, the emission
and throat irritation and nausea (Shusterman et al., of VOCs from building materiais and a simulated
1991; Wallace et al., 1993). One chamber exposure ofl:iee environment, respeetively, have been investi-
study has shown that fewer SBS symptoms were re- gated, see 6.3.
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- 6.2 Chamber Exposure Studies with
port may depend on prior sensations or visual con- VOCs and VOC Mixtures
tact. For example, Mosehandreas and Relwani In the classic work by Mølhave et al. (1986b), 62
(1992) observed that non-smokers reported a individual SBS sensitive subjects were exposed to a
higher odor intensity from ETS when smokers were mixture of 22 different VOCs at three different
visible than non-visible. levels for 2.75 hours, see Tabte 6.2.1. Mølhave's
There are subjective and objective effeets to be mixture of 22 different VOCs was seleeted on the
investigated in chamber exposure studies. The for- basis of measurements in Danish buildings and
mer ineludes perceived mueous membrane irri- emission testing of building materiais (Mølhave,
Peder Wolkoll· Vololile Orgonic Compounds 51
1982). The mixture contained two major VOCs, Lowest reported dose-response effect levels were at
butyl acetate and toluene in l : l ratio (==<73% 3 mg/m3 for odor intensicy, i.e. significant change in
weight of total mixture). The total concentration of perceived intensity. The lowest reported level was 8
VOCs were O, 5, and 25 mglm3 and the concen- mglm 3 for changes in perceived air quality, need for
tration ofthe single VOCs were about 1110 to 1/100 ventilation and perceived irritation in eyes, nose and
of their corresponding TLV value, but still higher throat.
than those usually encountered indoors today in Chamber exposure srudies should be able to ex-
non-industrial environments. plain the common result found in many field srudies
The effects srudied by Mølhave et al. were per- that women report a higher complaint rate, when
ceived air quality, mucous membrane irritation compensating for bias and confounders, than men.
(dryness), odor annoyance and attention quality. Whether this finding can be rationalized in terms of
The srudy was later repeated by others with healthy different reporting anirudes or job characteristics
subjects (Hudnell et al., 1992; Otto et al., 1992, and therefore possibly different environmental con-
1993), and in one srudy with both healthy and sen- ditions (Hodgson et al., 1991 b) is still an open
sitive subjects (Kjærgaard et al., 1991 ). The major question. Odor annoyance (from ETS) and mucous
tindings of these srudies for healthy subjects were a membrane irritation, have been reported to depend
dose-dependent increase of mucous membrane irri- to some extent on gender, women being more sensi-
tation and detericration of the air qualicy, both at 5 tive than men (Cain et al., 1987; Cometto-Muiiiz
and 25 mg/m3 levels, an increased sensitivity was and Cain, 1992; Cometto-Muiiiz and Noriega,
observed arneng sensitive SBS subjects at the 25 1985; Winneke, 1992). E.g., it has been shown in
mglm3 level. However, the difference, among chamber exposure srudies that in particular, young
healthy and sensitive subjects was not large non-smoking women appear to be more sensitive to
(Kjærgaard et al., 1991). Decreased attention, in ETS than men. On the other hand, Mølhave et al.
the form of short-term memory deficiency, was ob- (1991 ) found that smokers responded more
served in the study with SBS sensitive subjects, but strongly than non-smokers to questions about air
not with healthy subjects. A major question is quality and odor intensity. However, provocation
whether the sensitivity is due to hypersensitivity. srudies with carbon dioxide have only shown weak
The deeane srudy by Kjærgaard et al. ( 1989) indkations that women had an increased sensitivicy
showed that the hitherte considered "inert" VOC (Kjærgaard et al., 1992). Similarly, Otto et al.
could provoke increased mucosal irritation and re- (1993) did not find any gender difference in SBS
duce the tear film break-up time; however, the con- complaint rating during exposure to the 22 VOC
centration was about three orders of magnirude mixture. A possible explanation of the observed
higher than normally encountered indoors. In ad- gender difference could be that the two genders
dition, deteriaration of the air quality was reported. have attached different values to the wording used
So far, the majority of reported chamber exposure in the questionnaire, like "acceptability" (Mølhave
srudies have been performed at concentrations sub et al., 1991). However, Stenberg and Wall (1995)
TLV levels, but still higher than normally encoun- conelurled that the excess reporting prevalence is
tered indoors. One rationale for the observed effects real and not a reporting artefact.
could be (hyper)addition of VOCs, because VOCs The time scale and adaptation of perceived mu-
may aet by a common physical mechanism pro- cous membrane irritation and odor annoyance are
portional to their thermodynamic activity, rather two important aspects to be considered. Both con-
than by a chemical mechanism as proposed by srirute important parts of the overall perception of
Comeno-Mwliz and Cain (1991- 1993). the IAQ. Knasko (1993) found that intermittent
lndicators for assumed inflammatory response, bursts of odor (pleasant or unpleasant) did not in-
e. g. significant increase o f neutrophils has been ob- fluence the mood, performance and the perceived
served in nasallavage ofhealthy men exposed to the health (headache and eye irritation) (cf. the field
same 22 VOC mixture and the increase was ob- srudy by Berglund et al., 1992). The subjects, how-
served even 24 hours after the exposure (Koren et ever, reported that odors had a negative effect on all
al., 1992). factors. Time integrated response has revealed that
In one srudy, Mølhave et al. (1991) examined the perceived eye and airway irritation, generally, in-
subjective reactions at nearly "realistic" indoor creases over time, but the time to reach the asymp-
1VOC concentrations of the 22 VOC mixture. totic level depends on the concentration, while the
1.1>
Table 6.2.2 Some human exposure slud1es w1th WOCs m climohc chombers 1\.J
.."
<11
Study VOCs Subjccts/ Conc. (T)VOC Melbods Major effects measurcd a_
(time hours) Design mglm1 -<1>
M w Subjcctive Objcctive ~
;:;::
Molhave et al., 22 VOCs (2. 75) 23 39 1 qucstionnairc ~
O, 5, 25 mucous mcmbranc irritation - brain: performance .!.
l986b o, 2, 5, 15 digit span odor intcnsicy i ~
acoustic rhinomctry [
l99lb (50 min) 25 double O, l, 3, 8, 25 split tamp - tcar film qualicy iD
blind o
cO
o
Mølhave et al., 22 VOCs ( l) lO O, lO qucstionnairc scnsory effccts i eye: tear film - :>
1993 ( 18, 22, 26°C} digit span nosc: nasal cavity arca, volumc ! o·
()
acoustic rhinometry o
split lamp - tcar film qualicy 3
-o
o
c:
Ircgrcn et al., Butyl acetate 24 35- 1400 questionnaire eye: break-up time - :>
a...
1993 (20 min, 4 hrs) cye redncss lipid laycr - "'
split tamp - tear film quality epithclial damage -
blinking frequency rcdness-
blink frequcncy (-)
Kja:rgaard deeane (6) 32 31 o, 54, 189, 540 questionnaire mucous membrane irritation in cye: break-up time !
et al., 1989 double blind split tamp, tear film eye, nose, and throat i PMN' i
performance air qualicy ! nose: PMN-
odor intensity i brain: performance -
Kjærgamrd 22 VOCs (2.5) 35 2 5, 25 qucstionnaire air quality .!. eye: PMN i
et al., 1991 digit span odor intensity i tear film -
nose: PMN-
brain: performance !
Korenet al., 22 VOCs (4) 14 O, 25 nasal lavage nose: PMN i
1992
Hudnell et al., 22 VOCs (2. 75) 66 0,25 questionnaire over time odor intensity !,
1992 30% decrease over time
Hudnell et al., 22 VOCs mix. (4) 46 O, 6, 12, 24 Odor intensity ! adoptation
1993 IAQ i improvcd
Mucous membrane irritation i
(concentration depcndent)
Otto et nl., 22 VOCs mix 66 o, 25 performnnce mucous mcmbrane eye and throat brain: performance -
1992 (2,75) irritation i
fatigue i
mental confusion t
IAQ, some adnptation, men and
women equal
Otto et al., 22 VOCs mix (4) 26 15 odor intensity i performnncc -
1993 IAQ .!.
Peder Wolkoll: Volatile Orgonic Compounds 53
Tear film quallty tive benzalkonium chloride reduces the surface ten-
sion and destabilizes the tear film (Holly, 1978; Wll-
o • t.422 son et al. 1975). Surface active species, such as ionic
surfactants are known to be eye and skin irritants,
-1 •4 and also to cause respiratory irritancy (Chiuchta
and Dodd, 1978; Kreiss et al., 1982). (A common
-2 •1
detergent, sodiurn dodecyl sulphate, has been
-3 •3 shown to cause pronounced cytotoxic effects on cut-
tures of oral mucosa epithelium (Arenholt-Bindslev
-4 •2 et al., 1992; Bleeg, 1990)).
-5 So far, as pointed out by Franck and Skov
3 4 5 6 7 (1989), it is not known whether e.g. reduced foam
Total log llpophfllclty
formation eauses changes of the tear film or vice
Fig. 6.3.2 Meosured ond pooled leor film quolity ol 25 subjects,
see text for explonolion, versus totallog lipophilicity of VOCs from versa. It is noteworthy that the tear film quality was
four building moleriels in on exposure chomber. 11 Pointed gypsum unaffected in the office environment study; only epi-
board, 21 Rubber floor; 3} nylon corpel with rubber mal; 41 Portide thelial damage was observed and vice versa in the
board cooled with acid-curing point. Teor film quolity:- 4 =worst
destobilization. lipophilicity wos colculoled for eoch materiel as r building materlal exposure study. The different ef-
C,x(Ka;wl.. where C;=chomber concentration !mg/m3) af VOC; fects coulcl be rationalized in terms of ditferent com-
in the building materiel exposure sludv !Wolkoff el al.. 1QQ 1b). binations o f pollutant levels and user specific related
ll<o;w),=octanol/woter parlilion coefficient ol VOC;. Corr. coef.=
0.93. M22acalculated totallog lipophilicity ol 22 VOCs 15 work requirements, e.g., VDT work in the simu-
mg/m3 1evel; Kjærgaord et ol., l QQ l J lated office study.
controls the process. This destabilization could lead 6.4 The Association between Field
to a thinner fany Jayer and cause a decrease of the Studies and Chamber Exposure
break-up time (Norn, 1992). This again could en- Studies
hance the access to free nerve endings. Conse- The results of the office environment study are in
quently, irritation caused by pollutants would be ef- agreement with findings obtained in recent field
fective at lower concentrations than for an intact studies. Kjærgaard and Brandt ( 1993) found an as-
fatty layer (tear film). The proposed hypothesis is sociation between an increased concentration of
comparible with the observed decrease of break-up polymorphonuclear neutrophils in the eye and VDT
time in the deeane study (Kjærgaard et al., 1989). work (cf. Franck, 1986). VDT work has been as-
However, a decrease was neither found in the study sociated with increased SBS prevalence (Nunes et
with the 22 VOC mixture (Kjærgaard et al., 1991) al., 1993; Skov et al., 1989; Stenberg et al., 1993;
nor with butyl acetate at supra 1LV levels (lregren Stenberg and Wall, 1995) and the same has been
et al., 1993). The discrepancy may be partly ration- reported for paper handling (Fisk et al., 1993). The
alized by ditferent measures of the tear film qualiry, use of computers, however, was not found to be
different concentrations and the total lipophilicity significantly associated with SBS prevalence in the
of pollutants; e.g., the lipophilicity of butyl acetate, study by Fisk et al. (1993), but use of photocopy
expressed as the k.:.1w partition coefficient, is about machines (Sundell et al., 1994) (see also Wallace et
four orders lower than that of decane. In the deeane al., 1993) and handling of carbonless copy paper,
study, only break-up time was measured, while re- have been found to be associated with increased
sules for break-up time, foam formation and thick- SBS (Fisk et al., 1993; Skov et al., 1989; Taylor et
ness of the fatty layer were pooled together in the al., 1984). In addition, Kjærgaard and Brandt
materlal study Oohnsen et al., 1991; Wolkoff et al., (1993) in their field study found that micro damage
1991b). lt has been shown that pollutants such as of the conjunerival epithelium was weakly associated
paraffin oils (alkanes), silkone emulsion (Gluud et with photocopying. The reactions of pollutants
al., 1981; Norn and Opauszki, 1977), and white ernined from office machines, i. e. formation of reac-
spirit vapor (Stokholm et al., 1994) reduce the fatty tive species by reaction with ozone (Eggert et al.,
layer, as well as foam formation, break-up time, and 1990; Schnell et al., 1992; Weschler et al., 1992;
enhance damage of the conjunerival epithelium. Wolkoff et al, 1992, 1993a; Zhang et al., 1994a,b)
Likewise, it is known that the ionic and surface ae- (cf. Tables 2.3.2.1 and 2.5.2), could be another
56 Peder Wolkolf: Volatile Orgonic Compauods
rationale for the observation of increased SBS proposed that eye irritation may be enhanced by at
prevalence in the simulated office study. Menzies et least three types of exposure: chemical, physical
al. (1993) found that eye irritation was associated (e.g., particles and thermal elimate inelucting
with dust and outdoer pollutants (CO, N0 2 and draught) and specific aerlvities (e.g. VDT work).
ozone). Dust particles have been shown to cause This is in agreement with the multi-pollutant ex-
eye redness (Kjærgaard and Pedersen, l 989) and posure approach applied by Menzies et al. (1993)
deposition of particles during VDT work could also and the condusion that the cause of indoor ocular
contribute to destabilization of the outer fany layer troubles are multifactorlal (Norn, 1992). Further-
of the tear film (Schneider et al., 1994) (cf. Stock- more, the relevance of considering the work situ-
holm et al., 1982). In addition, the use of make- ation, e.g. VDT work, is supponed by the repart
up has been found to be an important confaunder that the eye blink rate appears to be lower during
regarding reponed eye irritation (Franck, 1991; VDT work than under relaxed conditions (Shu-
Franck and Skov, 1989; Kjærgaard et al., 1993). Hung Wu et al., 1986; Tsubota and Nakamori,
The overall results from the studies of building 1993) and, in general, when visual tasks become
materiais and office environment suggest that evalu- difficult (Shu-Hung Wu et al., 1986). The combi-
ation of the indoor elimate should be cautious (Wol- nation of the observed decrease of the eye blink rate
koff et al., 1991b, 1992). Neilher VOCs or any and increased ocular surface (tear film) may in-
other indoor pollutant should be considered inde- crease the rate of evaporation, thus promoting an
pendently. The cumulative exposure of pollutants instability o f the outer fany layer (Tsubota and Nak-
and user-related exposure, e.g. VDT work and the amori, 1993). Although, one would expect an in-
amount o f paper handling should be considered. In crease of the blink rate as a result of eye irritation
addition, the impact of other exposure loads, e.g. (Prah et al., 1993; Prause and Norn, 1987), this is
temperature, noise and cold draughts (Clausen et prahably not the case for VDT work. Once the tear
al., 1993a; Mølhave et al., 1993; Wyon and Wyon, film has been ruptured by a surface active com-
1987). pound(s), repeated eye blinking eannot restore the
Based on the cernbined results of reported field film continuity within a short time (Burstein, 1985;
investigations and the simulated office srudy, it is Holly, 1978).
Conclusion
This document is an overview and ineludes some vananons (Wolkoff et al., 1991a). Concentration
of the thesis work of the author without going into panerns also indicate that stationary field measure-
experimental and technical details. ments so far carried out (e.g. in offices) most likely
The thesis studies cover several disciplines: air have underestimated the "real" exposure.
sampling and strategy, analysis of VOCs in air, lt is important to ask the right questions needed
emission testing of VOCs from materiais with a de- to test a hypothesis about the impact of VOCs, in
veloped micro climatic chamber and use of models order to plan a sampling strategy. In addition,
describing the emission profile over time. In ad- knowledge about the source dynamics, is required,
dition, two human exposure studies have been car- as well as the history and the building character-
ried out combining pollutant measurements with istics. Also, sampling technique, transport, storage
both subjective and objective clinical measures of and analysis, all with their own set of characteristics
the impact of the emission from selected building for selection, should be carefully chosen. At present,
materiais and office equipment, respectively, and it appears that TVOC as a SBS marker should be
also including the use of a bioassay. replaced with parameters bener associated with
IAQ complaints and SBS prevalence or mechanism
Sources. There is a plethorn of different emission of action (cf. Brown et al., 1994). This could be,
sources, each with its own emission characteristics, e.g., biological activity expressed as the sum of irri-
which contribute to pollution of the indoor air. The tant VOCs (TVOCirriumcy). The activity expressed
contribution of building materlal emissions relative as partial pressure of each VOC relative to its satu-
to all other sources was about 50% in a new occu- rated vapor pressure (Ferguson principle) has also
pied Danish apartment and the time to reach a rela- been suggested ( Comeno-Muftiz and Cain, 1991,
tively constant concentration level was in the order 1992, 1993; Mølhave and Nielsen, 1992). Physico-
of 100-140 days (Wolkoffet al., 1991a). Ona Iong- chemical properties such as total lipophilicity could
term basis, the emissions from new building ma- be a measure for eye irritation (Wolkoff et al.,
terials will decline. lndeed, the etiological relevance 1991 b). Other suggestions are VOC group fraericn-
of some building materlal emissions in older build- ation (Shields and Fleischer, 1993) and rank order
ings has been questioned (Sundell et al., 1994). The assessment (Morey and MacPhaul, 1990).
contribution of secondary pollutant sources and hu-
man activity related emissions will dominate the in- Fie/d Studies. The VOC concentrations have been
door air, in particular in older buildings. For ex- measured with a variety of methods, sampling strat-
ample, office machines, VDT use and paper han- egies and different analysis methodologies and re-
dling (e.g. carbonless copy paper) have been found porting. Large variations in TVOC concentrations
to be associated with increased SBS prevalence have been measured (Wolkoff, 1990b), which may
(Fisk et al., 1993; Skov et al., 1990; Sundell et al., indicate that time-integrated mean concentrations
1994). are inappropriate for evaluation of mucosal irri-
tation and odor annoyance. Generally, field studies
Measurements. The most common approach for have failed to identify associations between VOC
VOC air sampling indoors is preconcentration on a concentrations and increased SBS prevalence. SBS
solid porous sorbent (e.g. Tenax TA) followed by symptom reporting was carried out simultaneously
thermal desorption and gas chromatography. This with measurements in one study and it was found
approach allows air sampling with a high sampling that TVOC, light and noise were associated with a
frequency (< 60 min) and Iong-term sampling higher SBS prevalence (Hodgson et al., 1991b).
(weeks). The former has revealed that the TVOC Some studies have reported associations between
levels may show considerable temporal variations TVOC and SBS reporting, but they are less clear
during the workday in offices (Wolkoff, 1990b) and (cf. Berglund et al., 1992; Brown et al., 1994). Gen-
Iong-term air sampling has shown large seasonal erally, symptom reporting has been retrospective
58 Peder Wolkoff· Volatile Orgon·c Compounds
rather than reporting during sampling, thus possibly been developed for labeling building materiais'
resulted in a higher SBS rate, cf. Berglund (1992), emissions according to their possible impact on the
in addition to recall bias (Knasko, 1993) and the IAQ using comfort endpoints (Wolkoff and Nielsen,
bias of approach of the study applied (Berglund et 1996), standardized methods are required to com-
al., 1992). Other field studies have indicated that pare emission data. Modeting can also be used to
VOCs as a pattern rather than as a concentration estimate the relative contribution of a particular
may aet on the sensory system. "Lost TVOC" source, e.g., the emission profile of styrene from
(~TVOC) (Berglund et al., 1993; Lundin, 1991, photocopied paper can be used to estimate the styr-
1993) may reflect "reactive" indoor air chemistry ene in a standard room (Wolkoff et al., 1993a}.
and may follow increased SBS reporting (cf. Sund-
eli, 1994). This hypothesis, first proposed by Ster- Human Exposure Studies. Human chamber exposure
ling and Sterling (1983), is supported by other studies with single VOCs, mixtures of VOCs and
studies which have shown increased aldehyde and mixtures of VOC emissions from building materiais
TVOC emissions upon exposure of textile carpets and office equipment have indicated that VOCs
in the emission to ozone (Weschler et al., 1992), may contribute to deteriaration of the IAQ, in the
increased formaldehyde formation during operation form of odor annoyance and mucous membrane ir-
of office machines (Wolkoff et al., 1992), in ad- ritation at or close to concentrations relevant for in-
dition, to increased aldehyde concentrations indoors door settings, i.e. about two orders of magnitude
(Zhang et al., 1994a,b). below TLVs. Subjective perceptions of SBS symp-
toms have been found to be comparible with objec-
Macen·az Emissicm Testing. Emission testing of build- tive measures of the tear film quality in some
ing materiais may provide information abaut VOCs studies. Studies of the tear film quality (expressed
by the use of static or dynamic headspace analysis, as break-up time, semiquantitative measurement of
the latter using a climatic chamber. Some unstable precomeal fany layer, appearance of foam at eye lid)
VOCs can be identified using the combinanon of have indicated that it can be affected at 1- 2 mg!
preconcentration of a headspace sample, thermal m 3 speciated TVOC levels from building materiais
desorption and GC-port snifting technique (Wol- (Wolkoff et al., 1991b). Also, that the totallipophil-
koff, 1990a). Static headspace may also be used to icity of the VOCs present could be one physico-
compare the emissions from photoprocessed paper chemical property retleeting for destabilization of
from office machines (Wolkoff et al., 1993a). In the eye tear film. However, the action on airway
complaint cases, suspected emirting sources can be mucous membranes may be different. The immedi-
taken to the labaratory for determination of their ately perceived air quality as a measure of the IAQ
headspace emission profiles (Wolkoff, 1990a). Al- and SBS marker should be used cautiously in case
ternatively, the portable micro emission chamber of irritants, like formaldehyde (Wolkoff et al.,
(FLEC) can be applied in the field (non-destructive 1991b), because of the latency of mucous mem-
testing) for source identification and in a labaratory brane irritation, but also due to the faet that odor
for emission testing (Wolkoff et al., 1991c). The irri- perception before adaptation may mask irritative
tative potential of VOC mixtures emitted from ma- perception.
terials can also be screened by bioassays (rucker, Both subjective and objective effects (micro dam-
1993), e.g., the mouse bioassay (Wolkoff et al., age of conjunerival epithelium) observed at indoor
1988, 1991b), and the active agent(s) may then be relevant concentrations suggest the relevance of
identified by chemical analysis. considering aU potential pollutants in concert (i.e.
Emission testing of waterbased paints has shown VOCs, formaldehyde, ozone, particles), comparible
that the emission profile of high boiting VOCs may with the multi-pollutant exposure model (Menzies
continue for more than a year (Clausen et al., et al., 1993; Wolkoff et al., 1992), rather than look-
1991). Emission testing at different air velocities can ing at VOCs as a single pollutant entity. An inte-
be used to validate models which reOect the emis- grated evaluation of exposure loads should be con-
sion process (Wolkoff et al., 1993b). Emission test- sidered including the physical exposure (e.g. partieJe
ing of VOCs from building materiais should result exposure and thermal climate), in addition to the
in an evaluation of the materials' impact on the IAQ worker's situation, e.g. VDT work and paper han-
(comfort and health) on both a short-term and a dling.
Iong-term basis. Although, an approach already has The role of VOCs as causarive agents leading
Peder Wolkoff Volatile Orgoruc Compound~ 59
to increased IAQ complaints and SBS prevalence sources, including human bioeffiuents should be
appears to be multi-faceted and it is still not yet studied. The identified associations of SBS
clear how VOCs alone may cause SBS. Several prevalence with the use of office equipment and
hypotheses have been proposed which could ra- paper (Fisk et al., 1993; Skov et al., 1989; Liden
tionalize the possible impact of VOCs on the IAQ and Karlberg, 1992; Sundeli et al., 1994), daily
and explain SBS: a) The total exposure approach, activity related contributions, such as use of of-
where VOCs will exhibit a considerable additivity fice equipment, paper, maintenance, VDT use
despite sub-TLV levels through a nonspecific pro- and partide deposition all should be incorpor-
cess; b) the action of specific irritants, such as ated in models for evaluation. In addition, the
formaldehyde or acrolein in ETS; c) the multi-pol- relatively large surface area of furniture should
lutant exposure approach (Menzies et al., 1993; prompt more studies regarding emission testing
Wolkoff et al., 1992), including also the work situ- and evaluation thereof.
ation (VDT) and deposition of particles (Schneid- • Considering the huge amount of cleaning agents
er et al., 1994); d) sparlal variations, e.g. concen- used on a daily and yearly basis, ir appears that
tration gradients (Noma et al., 1988); e) physico- VOCs from residues and the ionic surfactants
chemical properties, such as concentrations ex- should be important indoor pollutants to measure
pressed as the chemical activity (Cometto-Muftiz in the air and particles.
and Cain, 1991, 1992, 1993; Mølhave and Niel- • There is a strong need to identify mechanisms of
sen, 1992), lipophilicity, or reduction of the sur- mucous membrane irritation (eye and airways).
face tension of the eye tear film by surface active Further, the identification of reactive causarive
substances (Franck, 1991; Wolkoff et al., 1991 b); agents and using multi-exposure approaches
t) the possibility of odors triggerlog certain symp- should be a new way of exploring and under-
toms, in addition to noise, ligbring and tempera- standing the etiology of SBS.
ture (Clausen et al., 1993a); g) reactive species, • Quantification of the impact of odor sensation
e.g., fonned by indoor air chemistry (Sundell et on other SBS symptoms, in particular the link
al., 1993). In addition, VOCs adsorbed on par- between chemical emission testing of building
ticles have been suggesred to form an efficient sen- materiais and sensory evaluation should be iden-
sory stimuli (Berglund and Lindvall, 1986). tified.
• Field studies which combine symptom reporting
Research Implications. So far, the research has fo- with simultaneous IAQ measurements, i.a.
cused on VOCs and the reactive fonnaldehyde and VOCs and other indoor pollutants should be car-
has tried to rationalize the health impact accord- ried out. Data should be analyzed with the use of
ingly. Future research aerlvities on VOCs and other multivariate analysis techniques to identify which
indoor pollutants are still needed, in order to ident- VOCs and other pollutants are associated with
ify the etiology of deteriorated IAQ and SBS. It ap- SBS symptom prevalence and in what context
pears from this overview that the foliowing research they do so.
topics would be necessary and fruitful: • Field studies should, in addition to personal ex-
posure measurements, incorporate objective
• The etiological fraction of SBS prevalence from (physiological) measures, e.g. deteriaration of the
indoor sources, e.g. building materials' emission eye rear film (Franck, 1986, 1991; Franck and
relative to daily activity related and other salient Skov, 1989; Kjærgaard and Brandt, 1993).
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