AE International – Europe

Atmospheric Environment 37 (2003) 1737–1744

The active surface of suspended particles as a predictor of lung

function and pulmonary symptoms in Austrian school children
Hanns Moshammer, Manfred Neuberger*
Institute of Environmental Health, University of Vienna, Kinderspitalgasse 15, A-1095 Vienna, Austria
Received 14 June 2002; received in revised form 21 January 2003; accepted 24 January 2003

Abstract

At a central elementary school in the capital of Upper Austria children aged 7–10 years underwent repeated
respiratory health checkups (questionnaires, diaries, spirometry). Between March and May 2001 the daily means of the
signals of a diffusion charging sensor, measuring the ‘‘active surface’’ of suspended particles, and a photoelectric aerosol
sensor, measuring the particle-bound polycyclic aromatic hydrocarbons, were related to spirometric results of the total
164 children examined and to the daily symptom scores of a susceptible subgroup. Significant reductions of forced vital
capacity ðp ¼ 0:006Þ and forced expiratory volume in the first second ðp ¼ 0:001Þ and significant increases of wheezing
ðp ¼ 0:001Þ; shortness of breath ðp ¼ 0:041Þ; cough in the evening ðp ¼ 0:031Þ and at night ðp ¼ 0:018Þ were found
with increase of ‘‘active surface’’ of suspended particles measured at the adjacent outdoor monitoring station, but not
with the increase of particle-bound polycyclic aromatic hydrocarbons. Monitoring ‘‘active surface’’ of particles with
diameters of about 10 nm–1 mm by means of a diffusion charging sensor might provide additional information in
surveillance of particulate matter for prevention of acute effects on respiratory health.
r 2003 Elsevier Science Ltd. All rights reserved.

Keywords: Particulate matter; Dust surface; Diffusion charging; Respiratory health; Asthma

1. Introduction for their interaction with biological membranes. For

Suspended particles have recently received much
interest because of increasing epidemiological and
experimental evidence of their health impact. Notwith-
standing the fact that the exact biological mechanisms
are not entirely clear, both mass and number of very fine
particles have been shown to correlate with acute health
effects and measurable functional changes in the
cardiovascular and respiratory system (Penttinen et al.,
2001a; Peters et al., 1997; Pope et al., 1991; Schwartz
et al., 1993). Suspended particles differ widely in size as
well as physical and chemical properties, and surface
properties of particles seem to be of special importance
*Corresponding author. Tel.: +43-1-4277-64711; fax: +43-
1-4277-64799.
E-mail address: manfred.neuberger@univie.ac.at
(M. Neuberger).
health risk assessment of fibrous particles such as
asbestos, gravimetric measurements are no longer in
use, because the importance of fibre number and surface
(Neuberger, 1989; Timbrell et al., 1990; WHO, 1986) has
been established. Recent studies suggest that also the
surface of non-fibrous particles is more important for
cell interaction and health effects than the particles’ core
. et al., 2002; Oberdorster
(Dye et al., 2001; Hohr . et al.,
1995; Tran et al., 2000). Hence it makes sense to measure
total active surface in addition to mass or number of
particles. Apart from this consideration, combining
different methods of dust monitoring could provide
improved insight into different biological effects arising
from the various fractions of fine dust and help us to
understand the relevant biological mechanisms.
We had the opportunity to measure two different
surrogates of particle surface by operating both a
diffusion charging particle sensor (LQ 1-DC) and a

1352-2310/03/$ - see front matter r 2003 Elsevier Science Ltd. All rights reserved.
doi:10.1016/S1352-2310(03)00073-6
1738 H. Moshammer, M. Neuberger / Atmospheric Environment 37 (2003) 1737–1744
photoelectric aerosol sensor (PAS 2000 CE) during
6 weeks in spring 2001 at the central air monitoring site
of the ‘‘Austrian Project on Health Effects of Particles’’
(AUPHEP) in Linz, the capital of Upper Austria. In this
town of 200 000 inhabitants with steel and chemical
industry and heavy motor traffic, chronic respiratory
health effects of air pollution on children had been
found (Neuberger et al., 1995) and improvements in
lung function were related to improvements of air
quality (Neuberger et al., 2002), but from the remaining
pollution with particles and other air pollutants we still
suspected acute respiratory effects on days with elevated
concentrations. Therefore we chose the elementary
school next to the AUPHEP monitoring station (Hauck
et al., 2003) for an additional examination. During the
whole school year 2000/2001 different air quality
monitoring data were obtained as well as several health
data from the pupils (age 7–10 years). Here, however, we
only report on the day-by-day association between the
values of the two surrogates of particle surface (which
were monitored in spring only) in relation to the lung
function of the pupils and the symptoms score of a
subsample of ‘‘susceptible’’ children. To our knowledge
this is the first study on acute respiratory health effects
of ‘‘active’’ particle surface.
2. Material and methods
2.1. Air monitoring
The LQ 1-DC measures the active surface of
suspended particles by unipolar diffusion charging: Ions
are produced in the carrier gas by a corona discharge.
The ions attach to the surface of the particles which
are collected in an electrically insulated particle filter.
The electric charge is converted to a voltage signal.
The number of attached ions over a wide size range
of particles depends linearly on the active surface
(or ‘‘Fuchs’ surface’’) which can be interpreted as
that fraction of the geometrical surface of the particles
which is directly accessible from outside (Keller et al.,
2001; Quian et al., 2000), thereby capable of contacting
to and interacting with cells in the respiratory tract. The
signal of the LQ1-DC sensor is called ‘‘LQ’’ in the
following.
The PAS 2000 CE is a photoelectric aerosol sensor.
Particles are exposed to pulsed UV light with a
wavelength of 207 nm. Depending on chemical proper-
ties of the particles’ surface, UV irradiation stimulates
photoemission leaving the particle positively charged.
Generally in environmental air samples almost exclu-
sively polyaromatic hydrocarbons (PAH) are capable of
photoemission when irradiated in this manner. There-
fore the increase in positively charged particles during
the UV-pulse correlates well to the amount of particle-
bound PAH (Burtscher, 1992; Burtscher and Siegmann,
1994). The signal of the PAS 2000 CE is called ‘‘PAS’’ in
the following.
Both LQ 1-DC and PAS 2000 CE were operated from
26 March to 6 May 2001 with a storage time interval of
60 s. Half-hour means were calculated for each fully
covered half-hour. Daily means were calculated if at
least 16 h were covered by half-hour means. Mean values
of the first 8 h of the day were calculated when at least
7 h were covered. No daily means could be calculated
for 7 days (LQ 1-DC) and 2 days (PAS 2000 CE),
respectively. The same applies for the 8-h means from
0:00 till 8:00 o’clock. This time interval was chosen
because the lung-function tests were performed between
8:00 and 10:00 o’clock in the morning.
2.2. Lung function
At the school adjacent to the monitoring station every
second day (Monday, Tuesday, Wednesday, and Friday,
between 8:00 and 10:00 a.m.) about 20 of 164 children
(age 7–10 years) underwent lung-function tests, so
that each of the 69 girls and 95 boys had spirometry
about every fortnight from March to May. FVC,
FEV1, MEF25, MEF50, MEF75, and PEF were obtained
following the protocol of the American Thoracic
Society (1987), except for the minimum exhalation
time of 6 s which is not feasible for children. In this
analysis, each child served as its own control, because we
used the percent difference of the individual lung-
function parameter to the arithmetic mean of this
parameter of all tests during the school year as the
outcome variable.
On the whole 161 of the 164 children were tested on 13
days during the 6 weeks. Of these 161 children 91 were
tested 2 or more times. The outcome variables (differ-
ence from individual mean) of the two consecutive tests
of each of these 91 children did not correlate highly nor
significantly. (Because only 13 distinct data points in
time exist, more sophisticated multivariate analysis
controlling for auto-correlation was not feasible.) Only
12 of the 13 days are covered by sufficient LQ
respectively PAS data also.
2.3. Symptoms score
Parents of 78 children from the schools in the districts
around the monitoring station with either history of
asthma or a pathological lung-function test during the
preceding school year were asked to keep a diary for 4
weeks in each season. They had to fill in the child’s
medication and symptoms score with the following
items: itching or red eyes, fever, sore throat, cough in the
morning, cough during daytime, cough before sleep,
cough during sleep, shortness of breath, ears aching,
wheezing, runny nose.
 H. Moshammer, M. Neuberger / Atmospheric Environment 37 (2003) 1737–1744 1739

Since not all children started with their diary in the
same week, nearly every day of the observation period
was covered by at least some of the children.
3. Results
3.1. Air monitoring
LQ and PAS data correlated significantly ðpo0:001Þ
with Pearson’s correlation coefficient of 0.684 for half
hourly and 0.708 for daily means. While LQ data
correlated well with particle weight (PM10, PM2.5, PM1)
and particle number (condensation particle count-CPC),
the correlation was weaker for the PAS data (Table 1).
Both data sets (LQ and PAS) showed sufficient
variability to encourage further investigations (Table 2).
Supposing all airborne particles have the same size,
the surface of all particles would be directly proportional
to the number of the particles and the square of the
radius. Because the total volume (resembling particle
mass) is proportional to the number of particles times
the cube of the radius, the surface would be proportional
to (particle mass)2/3 times (number)1/3. Therefore the
logs of surface, number and mass would show a linear
association
logðsurfaceÞ ¼ 2=3logðmassÞ þ 1=3logðcountÞ þ constant:
Table 1
Correlationa of LQ and PAS signal with PM and CPC (half-
hour means, n=1898–2120)
r PM1 PM2.5 PM10 CPC
LQ 0.660 0.751 0.751 0.673
PAS 0.276 0.354 0.406 0.472
a
All po0.001.
Obviously the particles do not all have the same size
and the true size distribution is not known. Assuming
for the given location over one season this distribution
to be fairly stable, we expected a good linear regression
fitting for the logs of surface, mass and number variables
with the coefficients acting as an indirect measure of the
size distribution (formulas relate to half-hour mean
values):
logðLQÞ ¼ 0:337logðPM1 Þ þ 0:378logðCPCÞ
 0:584 ðr ¼ 0:551; po0:001Þ;
logðLQÞ ¼ 0:522logðPM2:5 Þ þ 0:300logðCPCÞ
 0:412 ðr ¼ 0:654; po0:001Þ;
logðLQÞ ¼ 0:453logðPM10 Þ þ 0:280logðCPCÞ
 0:222 ðr ¼ 0:630; po0:001Þ:
3.2. Lung function
On 12 days that were also covered by LQ and/or PAS
measurements on average 21 children underwent lung-
function tests. No systematic change of any of the six
lung-function parameters was seen in repeated tests
over the 6 weeks when particle surface was monitored
(Table 3). The LQ signal (first 8 h of the day on which
the lung function was performed) showed a consistent
negative association with the change in lung function,
which was significant for FVC, FEV1 and MEF50
(Table 3). This was not observed for the PAS signal.
Because LQ and PM data did correlate highly the
effect from surface and particle mass at this single site in
this short period of time cannot be distinguished.
Therefore we calculated the linear regression coefficients
of PM10, date and seasonal trend on the lung-function
parameters (difference from individual mean) collected
over the total school year. When PM10 showed a
significant effect on a lung-function parameter (this
was true for FEV1, MEF75, and MEF50) we used the

Table 2
Ranges of measurements for particle mass, number, and surface

Number Minimum Maximum Arithmetic mean Standard deviation

Half-hour means
PM1 (mg/m3) 2202 n.d. 98.90 10.79 9.31
PM2.5 (mg/m3) 2202 n.d. 119.92 14.61 10.83
PM10 (mg/m3) 2202 n.d. 190.79 23.13 20.08
CPC (part/cm3) 2202 20 140 972 25 024 16 937
LQ (mm2/cm3) 1898 4.80 342.77 57.54 42.64
PAS (ng/m3) 2120 1.50 174.70 14.68 15.53

Daily means
LQ (mm2/cm3) 38 18.67 109.56 57.46 25.25
PAS (ng/m3) 43 5.71 45.17 14.60 7.39

n.d.: below detection limit.

1740 H. Moshammer, M. Neuberger / Atmospheric Environment 37 (2003) 1737–1744

Table 3
Correlation between lung-function parameters with the LQ and PAS signal (mean value from 0:00 until 8:00 o’clock) and the date of
the test (26 March–6 May 2001)

r D-FVC D-FEV1 D-MEF75 D-MEF50 D-MEF25 D-PEF

LQ 0.179nn 0.213nn 0.102 0.172n 0.085 0.092

LQa 0.173n 0.059 0.140n
PAS 0.068 0.098 0.031 0.063 0.066 0.039
Day 0.103 0.055 0.016 0.059 0.039 0.003

D-FVC and following: difference of the individual lung-function parameter to the arithmetic mean of this parameter of all tests which
the individual child has performed during the school year.
a
Adjusted for MP10 (see the text).
n
po0.05.
nn
po0.01.

Table 4 throat and ‘‘aching ears’’ all correlated with fever but
Rank-correlation between symptoms of single children (from did not necessarily coincide (Table 4).
4  4=16 weeks of observation, n=1059–1074)) Based on this grouping of the symptoms from the
r Short breath Runny nose whole year we expected the groups 1 (wheezing, etc.) and
nn
2 (cough at different parts of day) more likely to be
Wheezing 0.307 0.158nn influenced by the air quality of the same day while for
Runny nose 0.139nn
the third group of symptoms (fever and signs of
inflammation associated with infectious diseases even if
Cough in they Morning Night Day
triggered by air pollution) a lag of several days between
nn nn
Evening 0.630 0.634 0.627nn the initial irritation of the mucous membranes and the
Morning 0.486nn 0.697nn full outbreak of the symptoms would be expected.
Night 0.408nn Therefore these symptoms were less likely to be captured
by the study design chosen to detect acute effects.
Red eyes Sore throat Aching ears
The LQ signal (daily mean) was positively associated
Fever 0.189 nn
0.201nn
0.135nn with the daily mean score of most of the symptoms
Red eyes 0.044 0.072nn (Table 5). This was also true for the PAS signal but at
Sore throat 0.007 least for the symptoms of prime interest the association
nn was less strong and significant only in one instance
po0.01.
(cough in the evening). These findings remained fairly
stable when only days were considered on which 7 or
residual of the regression analysis to check if LQ was more (respectively 13 or more) children provided
still correlated to these residuals. Correlation coefficients symptom data (on 37 and 30 days, respectively, data
and levels of significance were only slightly reduced by not shown).
this adjustment. After controlling for PM10 (all available In the logistic regression of the individual child’s
8-h mean morning values each) on the other hand the symptoms score, a nearly significant negative impact of
residuals of the LQ values were no longer correlated to the LQ signal was found for ‘‘wheezing’’ ðp ¼ 0:058Þ:
the lung-function parameters (data not shown). When both LQ and PAS signals were considered both
turned out to have a significant effect; however, the
3.3. Symptoms score coefficient of the PAS signal went negative (Table 6).

Between 23 March and 6 May symptoms from 48

boys and 30 girls were documented (on 44 days on
average 24 children participated). According to the
symptoms score per day, the symptoms registered during
all seasons (for 4 weeks in spring when particle surface
was measured and in the other 3 seasons for 4 weeks
each) could be grouped into three subsets: the four
‘‘cough’’ items correlated well with each other. The same
held for the triplet ‘‘wheezing’’, ‘‘shortness of breath’’,
and ‘‘runny nose’’. Symptoms of eye irritation, sore
4. Discussion
Monitoring active surface of total airborne particle
mass by diffusion charging is a relatively novel method
still in the need of evaluation. Our data show that the
daily mean (respectively the 8-h morning mean) of active
surface correlates well with various day-by-day health
outcomes in children visiting the school next to the
monitoring site. This indicates that during this period in
 H. Moshammer, M. Neuberger / Atmospheric Environment 37 (2003) 1737–1744
Table 5
Rank-correlation between daily mean symptoms score and the daily mean LQ and PAS
r Fever Sore throat Red eyes Aching ears
LQ 0.234 0.175 0.231 0.067
PAS 0.275 0.011 0.015 0.039
n
po 0.05.
nn
po 0.01.
Table 6
Logistic regression of individual child’s daily wheezing
Regression coefficient Standard error p (two-sided)
LQ 0.029 0.011 0.008
PAS 0.066 0.032 0.041
Constant 4.863 0.785 0.000
spring 2001 some biologically important properties of
suspended particles were captured by diffusion charging.
Acute decrements of pulmonary functions were related
to active surface of particulates also after adjustment for
PM10 (Table 3) which indicates for short-term lung-
function impairments that active particle surface is a
better index of exposure than what is currently used for
exposure assessment. Recent research has indicated that
insoluble ultrafine aerosols (i.e., particles whose physical
diameters are less than 100 nm) may cause adverse
health effects due to their small size, and that
toxicological response may be more appropriately
represented by particle number or particle surface area
(Zimmer, 2002). Particle mass measurements can be
strongly influenced by mechanically produced, soil-
derived particles, which may not be associated with
adverse health effects. Therefore, Penttinen et al.
(2001b) claim that air quality monitoring should include
particle number concentrations, which mainly reflect
ultrafine particles. While condensation counts of parti-
cles typically are most sensitive for ultrafine particles
(o0.1 mm), the particle mass o10 mm (PM10) tends to be
driven stronger by particles >1 mm. Diffusion charging
is most sensitive for the diameter range in between
(roughly around 1 mm and less) which has only been
assessed by surrogates like SO4 up to now. Of course
diffusion charging results are not equivalent to results
obtained by a different methodology, but also depend
on chemical properties of the particles’ surface (Matter
et al., 1999). This applies even more to the results
obtained by the photoelectric aerosol sensor (Hart et al.,
1993; McDow et al., 1990). Nevertheless both measures
correlated significantly with the particle mass and a
linear regression of the log values of number and mass
gave a good estimate of the logs of the surface values.
1741
Cough in the Short breath Wheezing Runny nose
Evening Morning Night Day
n n
0.350 0.117 0.382 0.199 0.334n 0.510nn 0.166
0.357n 0.126 0.111 0.183 0.118 0.228 0.052
This indicates that at a given measurement site during
one season the size distribution of the particles is
relatively constant. When sites are compared there is a
change in particle size distribution with increasing
distance from the source such as a heavy duty road
(Zhu et al., 2002). One year prior to the measurements in
Linz a similar campaign was performed in Vienna.
During this campaign we had performed a pilot study to
test the feasibility of measuring active surface. We
operated a measurement device similar to the LQ 1-DC
during January 2000. The coefficients of the linear
regression of the logs of the half-hour means differ
between Linz and Vienna. This difference certainly
reflects differences in the size distribution of the particles
at the two locations in winter respectively spring. Data
from more locations are wanted to further analyse this
issue:
Linz : logðLQÞ ¼ 0:337logðPM1 Þ þ 0:378logðCPCÞ
 0:584 ðr ¼ 0:551; po0:001Þ;
Vienna : logðLQÞ ¼ 0:184logðPM1 Þ þ 0:821logðCPCÞ
 5:782 ðr ¼ 0:374; po0:001Þ:
Comparing the health impact of PM10 and active
surface it should be noted that the two parameters are
correlated with each other which makes it difficult to
statistically separate any effect of both because of the
limited number of data points. But when considering the
data from a rather qualitative point of view some
differences as to specific health parameters or the time-
lag between exposure and effect are noted. If active
surface only were a surrogate marker for particle mass,
it would be expected that any effect caused by PM10
would be mirrored equally or less well by active surface.
Quite on the contrary PM10 of the preceding day was
highly associated with several lung-function parameters,
which was not seen with active surface. On the other
hand, active surface in the morning hours preceding the
lung-function testing was a better predictor for decrease
of FEV1 and other lung-function parameters. Fig. 1
illustrates the different time course of effects of PM10
and active surface on FEV1 (short-term lag structure).
1742 H. Moshammer, M. Neuberger / Atmospheric Environment 37 (2003) 1737–1744

FEV1 dependence on Half Hour Means of LQ

0.0005

00:00
00:30
01:00
01:30
02:00
02:30
03:00
03:30
04:00
04:30
05:00
05:30
06:00
06:30
07:00
07:30
-0.0005 B
upper CL
-0.001 lower CL

-0.0015

-0.002

FEV1 dependence on Half Hour Means of PM10

0.001

0.0005

0
B
00:00
00:30
01:00
01:30
02:00
02:30
03:00
03:30
04:00
04:30
05:00
05:30
06:00
06:30
07:00

-0.0005 07:30 upper CL

lower CL
-0.001

-0.0015

-0.002
Fig. 1. Coefficients (B) and their 95% confidence intervals of linear regression of FEV1 (measured between 8:00 and 10:00 a.m.) and
the half-hour mean values of LQ and PM10 between 0:00 and 8:00 a.m. of the same day.

To our surprise, the daily mean values from the other hand, the effect of PAH more closely resembled
photoelectric aerosol sensor—although correlating well that of the particle mass and combustion particles might
with those from the diffusion charging—did not predict be a better predictor of respiratory effects with longer
respiratory health outcome (acute short-term effects) time lags and of other health effects (Laden et al., 2000)
equally well (Tables 3, 5 and 6). On the contrary, when not captured in our study.
looking at individual children’s symptom scores (espe- The very short delay in time between exposure and
cially typical asthmatic symptoms like wheezing) it effect as well as the nature of the symptoms and the
appeared as if rather this part of the LQ signal, which lung-function parameters hint at an allergic mechanism.
was not accounted for by the variance in the PAS signal, Therefore we hypothesize that part of the observed
had the relevant effect (Tables 5 and 6). Since Burtscher effect could be caused by organic material relevant for
(1992) claims that the PAS signal indicates PAH- asthma and bio-aerosols smaller than intact pollen
covered aerosol from combustion sources we would (Knox and Suphioglu, 1996). In this case we would
have to conclude for this very location and time interval expect a seasonal effect. This is supported by prelimin-
that the non-combustion part of active surface led to ary findings on the PM10 data of the whole year: while
acute exacerbation or aggravation of wheezing in there was no short-term effect on these symptoms
children. The same conclusion would have to be drawn throughout the whole school year, there was a positive
also for lung-function decrements in healthy children, association between PM10 and wheezing in spring.
especially those lung-function parameters sensible to Monn and Becker (1999) found cytotoxicity and
irritation of the upper airways (like FVC and FEV1 cytokine induction caused by (non-combustion) coarse
which were influenced without delay by the active particles but not by fine particles (from combustion
surface and not by the particle-bound PAH). On the sources). While long-term effects of particulate matter
 H. Moshammer, M. Neuberger / Atmospheric Environment 37 (2003) 1737–1744
have been related to insoluble combustion products
retained in the lung (Brauer et al., 2001), acute
respiratory effects like asthmatic attacks have rather
been related to soluble components such as transition
metals on the surface of combustion particles (Lighty
et al., 2000); however, Brown et al. (2000) suggest that
other components of ultrafine particulate matter are
responsible for inflammation. Our results cannot explain
all the discrepancy in the results of these studies, but
challenge again traditional sampling of PM10 and
suggest including measures of active particle surface in
further investigations.
5. Conclusion
Acute effects of ‘‘active particle surface’’ as measured
by diffusion charging were found on pulmonary func-
tions (FVC, FEV1, MEF50) of elementary school
children and on asthma-like symptoms of children who
had been classified sensitive (from spirometry in the
preceding school year or from a history of asthma).
Diffusion charging is an easy way of monitoring surface
properties of suspended particles. Therefore we recom-
mend that this technique should be evaluated further.
While in a given setting the LQ-values correlate well
with particle mass, the association might differ depend-
ing on the size distribution and even chemical properties
of the particles which are influenced by the local
situation. Therefore particle surface as an additional
measure might help to understand differences of health
outcomes from the same amount of particle mass at
different locations.
Acknowledgements
This study was supported by the Clean Air Commis-
sion of the Austrian Academy of Science and conducted
within the AUPHEP Project. We thank the Municipality
of Linz (Departments of Health and Environment) and
the AUPHEP team for their support.
Dr. Gerd Oberfeld from the public health department
of Salzburg kindly provided the two sensors.
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