Upload
cranfield
View
0
Download
0
Embed Size (px)
Citation preview
Exposure to air pollutants in English homes
GARY J. RAW, SARA K.D. COWARD, VERONICA M. BROWN AND DERRICK R. CRUMP
BRE, Watford, UK
BRE has conducted a national representative survey of air pollutants in 876 homes in England, designed to increase knowledge of baseline pollutant levels
and factors associated with high concentrations. Homes were monitored for carbon monoxide (CO), nitrogen dioxide (NO2), formaldehyde and volatile
organic compounds (VOCs). In the majority of the homes, concentrations of the measured pollutants were low. However, some homes have
concentrations that would suggest a need for precautionary mitigation. Those factors that are most likely to lead to exposures of concern in homes are
identified as gas cooking (for CO and NO2), the use of unflued appliances for heating (for CO and NO2), emissions from materials in new homes (for total
VOC (TVOC) and formaldehyde), and painting and decorating, with a significant increase in risk suspected to exist where there is not a place to store
materials away from the living space (for TVOC). It is noteworthy that seasonal effects on CO and NO2 were largely due to indoor sources. This would
need to be considered when interpreting time series studies of the effect of outdoor air pollution on health. It is also of some significance that the critical
factors are related much more to sources than to ventilation: source control is therefore, as would be expected, the most appropriate approach to reducing
the risk of hazardous exposure to air pollutants in homes.
Journal of Exposure Analysis and Environmental Epidemiology (2004) 14, S85–S94. doi:10.1038/sj.jea.7500363
Keywords: homes, carbon monoxide, nitrogen dioxide, volatile organic compounds, formaldehyde, measurements.
Introduction
There is an increasing general recognition that, for most
people, exposure to air pollution is determined principally by
indoor exposure. Furthermore, exposure in the home
represents a significant proportion of total exposure and,
for those who are housebound, the total of their annual
exposure. In this context, it is perhaps surprising that
relatively little has been quantified regarding exposures in
the home. Within the UK, several studies have provided
indicative data on exposure to some key air pollutants (e.g.,
Wiech and Raw, 1995, 1996; Berry et al., 1996; Venn et al.,
2001), but none could claim to be representative of the
housing stock. The largest single study (Berry et al., 1996)
included only 174 homes, all in one English county.
The UK Government therefore commissioned a larger,
more representative survey, which led to monitoring of air
pollutants and potential determinants of exposure in 876
homes in England (Coward et al., 2001). The pollutants
monitored were nitrogen dioxide (NO2), carbon monoxide
(CO), formaldehyde and other volatile organic compounds
(VOCs) (evaluated both as total VOCs (TVOC) and
individual VOCs). The study was restricted to England
because that was the remit of the commissioning
department.
The survey was designed to increase knowledge of baseline
pollutant levels and of factors associated with high concen-
trations. This paper focuses on the implications for exposure.
Method
The survey structure and methodology, including quality
control/quality assurance procedures, are described in a
published report (Coward et al., 2001) and are therefore only
summarized here to the extent necessary to understand the
findings.
The Selection of HomesThe Survey of English Housing (SEH) was used as a vehicle
for selecting homes (DETR, 1999). The SEH entails visits to
20,000 randomly selected homes per year, using a team of
interviewers located throughout England. Using the SEH as
a sampling base, the aim was to obtain indoor air pollutant
measurements in 1000 homes, the monitoring being dis-
tributed across a full year so that seasonal variation could be
investigated. The requirement was therefore to recruit 80–85
homes per month; the SEH interviewers approached
randomly selected households in order to achieve this
number. The proportion of households that agreed to take
part was less than anticipated, so that the BRE research team
received, from the SEH operators, approximately 80
1. Address all Correspondence to: Dr Crump, BRE, Bucknalls Lane,
Watford WD25 9XX, UK.
Tel.: þ 44-1923-664452; Fax: þ 44-1923-664786.
E-mail: [email protected]
Journal of Exposure Analysis and Environmental Epidemiology (2004) 14, S85–S94r 2004 Nature Publishing Group All rights reserved 1053-4245/04/$25.00
www.nature.com/jea
addresses per month on average, and only about 75% of
these completed the survey. Consequently, the survey was
extended from 12 to 17 months (October 1997 to February
1999). By the end of the study, results had been obtained
from 876 homes. The householders did not return usable
samples for every pollutant in each case; hence, the number
of measurements varies between pollutants.
During each selection visit, the SEH interviewer adminis-
tered a questionnaire on behalf of BRE, if the householder
had agreed to take part in the air quality survey. The
questions concerned the homes, the characteristics of the
occupants and their activities in the home. The interviewer
also demonstrated the use of the various types of air sampler,
and showed the householder suitable locations for exposing
the samplers. No samplers were placed at this time because
the pollutants were monitored using small, simple, passive air
samplers, which could conveniently be sent by post.
The air samplers were subsequently dispatched by post
from BRE to the householders, typically within a week of
each address being received. The sampler packs included full
instructions for the use of the samplers, self-completion
questionnaires about activities during the sampling time and
reply-paid envelopes for the return of the samplers and
questionnaires to BRE. The households closed and returned
the samplers at different times in order to optimize the known
detection range of the samplers, based on the expected range
of environmental concentrations.
Data Collection
Carbon Monoxide CO was monitored for 2 weeks in the
kitchen and a bedroom in each home, using colorimetric
diffusion tubes (Drager Ltd). A single tube was placed in
each room. No blanks were used; the tubes are sealed glass
until opened. The manufacturer’s quality control system
conforms to the requirements of DIN ISO 9001. To ensure
consistent quality, the manufacturer stores tubes from each
production batch for routine tests at regular intervals. The
manufacturer has tested the tubes for measurement of low
concentrations of CO over a period of up to 15 days
(Pannwitz, 1987) and claims an accuracy of 750% for a
single-tube reading.
During exposure, CO diffuses along the tube and reacts
with the chemicals on an inert support, producing a colored
stain. The length of the stain is compared to a nonlinear scale
on the side of the tube to indicate exposure over a range of
50–600 parts per million (p.p.m.) hours. The scale is marked
at only five intervals and thus interpolation is required to give
an approximation for exposure between these intervals. To
improve accuracy, the scale on the tube was measured and
regression analysis used to provide a second-order poly-
nomial equation that converted stain length to exposure,
allowing more accurate interpolation between the marked
intervals. The tubes were ‘analyzed’ by two researchers who
were trained and experienced in reading stain lengths on the
detector tubes. These quality procedures in the reading
process were considered to be a more cost-effective approach
than using duplicate tubes.
Nitrogen Dioxide NO2 was monitored using Palmes
diffusion tubes (Atkins et al., 1978). The samplers were
exposed for 2 weeks in each home, in the kitchen, the main
bedroom and outdoors. A single tube was placed in each
location (no duplicates). Previous work which used the same
method (Berry et al., 1996) has established that duplicate
measurements within the same room had a high precision,
and it was not felt the increased analytical cost was justified
for the present study. The error (combined accuracy and
precision) of NO2 measurement by Palmes Tube in
comparison with a chemiluminescent monitor is 710%,
for concentrations across the range found in the built
environment (Apling et al., 1979).
One tube from each batch was returned for analysis
unexposed to ensure that it was blank. Experience has shown
that the quality is consistent, and that unopened tubes do not
pick up NO2. The tubes were analyzed colorimetrically using
a Bran and Luebbe Autoanalyzer, dedicated to NO2
analysis. The instrument was calibrated for each run, using
three dilutions of a standard solution, whose concentrations
fall on a straight line. The calibration was checked using a
second independent standard.
Volatile Organic Compounds VOCs were determined by
passive diffusion using Perkin-Elmer-type sampling tubes
packed with Tenax TA adsorbent, with an exposure period of
4 consecutive weeks. A single sampling tube was placed in the
bedroom of each home. Previous studies (Berry et al., 1996;
Brown et al., 1996) have shown that VOC levels vary little
between rooms in the majority of UK homes and that a
single measurement in the bedroom is representative of levels
elsewhere in the home. The bedroom was selected for the
sampling location as that is where most people spend the
majority of their time indoors. In 10% of homes selected at
random, a duplicate sampling tube was exposed alongside the
first tube, for quality control purposes. Additionally, for
every 10 tubes despatched a blank sample was retained and
analyzed along with the field samples.
Analysis of exposed samplers was undertaken using
automated thermal desorption gas chromatography (Per-
kin-Elmer ATD 400 and Autosystem GC) with flame
ionization for measurement of TVOC and mass spectro-
metric detection for characterization and measurement of
individual VOCs. The chromatographic conditions and
procedures used have been published previously (Brown
et al., 1999). TVOC concentrations were calculated from the
sum of all peaks that have a boiling point within the range
defined by C6–C16 hydrocarbons and using the response
factor for toluene. The limit of detection of the analytical
Air pollutants in English homesRaw et al.
S86 Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1)
method is 2 ng toluene equivalent, which represents a 4-week
mean concentration of 0.1 mg/m3 in air. The analytical
quality assurance was provided through BRE’s participation
in the Workplace Analysis Scheme for Proficiency (WASP)
quality assurance scheme for determination of VOCs. WASP
is a proficiency testing scheme for the analysis of occupa-
tional hygiene and environmental air samples set up by the
UK Health and Safety Executive.
Formaldehyde Formaldehyde levels were measured over a
period of 3 consecutive days in the bedroom of each home
using a single GMD 570 series dosimeter. The analytical
procedure used desorption with acetonitrile and high-
performance liquid chromatography (HPLC) on Zorbax
ODS C18 with UV detection at 345 nm. The procedure
accords with the draft international standard ISO/DIS
16,000-4 ‘Determination of formaldehyde in indoor air
quality by the diffusive method’. The limit of detection for
formaldehyde is 1mg/m3 and the precision of replicate
measurements is 7.2%. The analytical quality assurance
procedures were as described previously (Berry et al., 1996)
and through BRE’s participation in the WASP quality
assurance scheme for determination of aldehydes.
Questionnaires Householders completed questionnaires on
homes, occupants and activities in the home. The main
independent variables derived from the sampling records and
questionnaire were season, region, area type (degree of
urbanization), building date, type of dwelling, presence/type
of garage, household size, number of habitable rooms,
occupant density, cooking fuel, heating system/fuel, heating
with portable/unfueled heaters or a gas cooker, having an
extract fan, amount of cigarette smoking, and the presence of
condensation, damp or mold. Season was defined according
to the month when sampling commenced: spring (March,
April, May); summer (June, July, August); autumn
(September, October, November); winter (December,
January, February).
Analysis
The measurements obtained for each of the pollutants were
log-normally distributed; therefore, the data were log-
transformed before analysis and only geometric means are
presented. The analysis employed t-tests for comparisons of
two groups and ANOVA for comparisons of more than two
groups. All of the dependent variables were used in the
analysis for each pollutant; hence, if a difference is not
mentioned as being significant, it is because it was included in
the analysis and found not to have a significant effect on the
pollutant in question.
Results and discussion
A detailed analysis of determinants of pollutant concentra-
tions has been reported (Coward et al., 2001, 2002). The
second report also covers relationships among the different
pollutants. Therefore, this paper concentrates on those
findings that have important implications for exposure.
Carbon MonoxideCO levels were measured successfully in 830 homes, with 821
homes providing results for both kitchens and bedrooms.
Minimum, maximum, geometric mean and percentile values
are shown in Table 1. Concentrations were significantly
higher in kitchens than in bedrooms.
The maximum 14-day average concentration of CO did
not exceed the WHO 8-h average guideline value of 10 mg/
m3 (WHO, 2000) in any home. The monthly mean
concentration was less than 1 mg/m3 in every month of
sampling. While there may be concerns that long-term
exposure to CO at concentrations below the WHO guideline
level may have health effects, this is yet to be confirmed.
Therefore, the measurements made in this study have little
direct implication for health at population level.
Of course, it remains possible that the guideline is exceeded
in homes over shorter periods. Previous work has shown that
exposures while cooking with gas can exceed 100 mg/m3 over
a period of 1 h, which is considerably in excess of the WHO
1-h guideline of 30 mg/m3 (Ross and Wilde, 1999).
Evaluation of hazardous exposure to CO should, therefore,
focus on the time spent in the presence of known sources.
Nevertheless, it should be clear that hazardous exposures
are very unlikely to occur unless there is an indoor source of
CO, and this can be confirmed by reference to the detailed
findings from the present study. Three indoor sources were
shown to be independent significant determinants of indoor
CO concentration: gas cooking, tobacco smoking and the use
of unflued combustion appliances for heating. In addition,
two factors related to outdoor concentration (and ventila-
tion/heating) were significant determinants of indoor CO
concentration: area type and season.
The analysis of cooking fuel compared three groups: (i)
homes with natural gas cooking including a natural gas oven,
(ii) homes with some natural gas cooking (hob and/or grill)
but no gas oven and (iii) homes with no fossil fuel cooking.
The difference between the groups was highly significant
Table 1. Statistics for CO concentrations (mg/m3).
Location Minimum Maximum Geometric
mean
Percentiles
10% 50% 75% 95%
Bedrooms o0.01 3.90 0.39 0.12 0.44 0.69 1.68
Kitchens o0.01 4.45 0.47 0.14 0.50 0.90 2.07
Air pollutants in English homes Raw et al.
Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1) S87
(kitchens: F¼ 98.1, Po0.001; bedrooms: F¼ 24.8,
Po0.001) with each group significantly different from the
other two except, in bedrooms, for the comparison of groups
(ii) and (iii). The geometric mean kitchen and bedroom levels
are given in Table 2.
In the case of kitchen CO levels, the effect of cooking fuel
was modified by an interaction with season (F¼ 2.1,
Po0.05), both factors also being significant as main effects
on CO levels both in kitchens (F¼ 37.5, Po0.001) and in
bedrooms (F¼ 48.4, Po0.001) F see Table 3. The overall
pattern was that CO levels were higher in autumn and winter
than in spring and summer. It is likely that the differences
were caused by a combination of increased fossil fuel use and
decreased ventilation in colder weather. Homes with a gas
oven had the highest kitchen CO levels in winter and this was
responsible for the overall slightly higher level in winter. The
other homes had the highest level in autumn.
Cookers and other unflued combustion appliances were
used for heating in some homes, resulting in higher CO
concentrations in kitchens (F¼ 5.8, Po0.001) and bedrooms
(F¼ 4.1, Po0.001). Means are shown in Table 4. CO also
varied significantly with tobacco smoking (kitchens: t¼ 6.1,
Po0.001, bedrooms: t¼ 6.4, Po0.001, Table 5), showing
that even a small intermittent indoor source can have a
measurable effect over an extended averaging period.
An indication of the background seasonal CO levels was
obtained by looking at homes where no fossil fuel was used
and where there were no regular smokers (Table 6). A one-
way ANOVA shows significant seasonal differences (bed-
rooms F¼ 3.6, Po0.05; kitchens F¼ 6.0, Po0.01). Au-
tumn CO levels were significantly higher than levels in spring
and summer in both locations. Levels in winter were higher
than in spring or summer, but the differences were not
significant, possibly because of the low numbers of cases. The
difference between kitchens and bedrooms was also not
significant for this subsample.
Taking spring and summer as the baseline, and combining
bedroom and kitchen data, concentrations are increased by
approximately 0.28 mg/m3 in autumn, and 0.14 mg/m3 in
winter. The effect of gas cooking (including gas oven) is to
increase mean concentrations in kitchens by amounts ranging
from 0.37 to 0.44 mg/m3 in spring, summer and autumn, but
0.67 mg/m3 in winter. This most likely reflects reduced
ventilation in the kitchen in winter. However, having extract
ventilation in the kitchen affected only bedroom CO and only
in interaction with season (Table 7).
There was a significant difference between area types for
CO concentration in kitchens (F¼ 12.4, Po0.001) and
bedrooms (F¼ 17.7, Po0.001) (see Table 8). Bedroom and
kitchen CO levels were significantly lower in rural areas than
in other areas, and bedroom levels were also significantly
Table 2. Geometric mean CO (mg/m3) by cooking fuel.
Cooking fuel Kitchens N Bedrooms N
(i) Natural gas oven 0.77 335 0.53 332
(ii) Natural gas cooking
but no gas oven
0.47 129 0.37 128
(iii) No fossil fuel cooking 0.30 349 0.31 347
Table 3. CO (mg/m3) by season and cooking fuel.
Spring Summer Autumn Winter
Kitchen CO
Gas cooking including gas oven 0.61 0.51 0.88 1.06
Gas cooking but no gas oven 0.41 0.20 0.60 0.57
No fossil fuel cooking 0.20 0.14 0.44 0.39
All kitchens 0.35 0.27 0.59 0.62
Bedroom CO
All bedrooms 0.28 0.21 0.53 0.53
Table 4. Kitchen and bedroom CO (mg/m3) by unflued heater use.
Any use of
portable or other unfueled
heater or gas oven for heating
Kitchens Bedrooms
Mean N Mean N
Yes 0.89 73 0.62 73
No 0.44 755 0.38 749
Table 5. Kitchen and bedroom CO (mg/m3) by smoking.
Regular smoking in home Kitchens Bedrooms
Mean N Mean N
Yes 0.66 242 0.55 239
No 0.41 585 0.34 582
Table 6. CO levels (mg/m3) in all-electric homes with no regular
smokers.
Season Bedrooms Kitchens
Mean N Mean N
Spring 0.13 10 0.14 10
Summer 0.17 8 0.06 8
Autumn 0.39 10 0.43 10
Winter 0.26 8 0.28 8
Air pollutants in English homesRaw et al.
S88 Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1)
lower in suburban than in central urban areas. Taking rural
areas as a baseline, CO exposure in the home is approxi-
mately doubled by living in a central urban area, a difference
of 0.41 mg/m3 in bedrooms and 0.38 mg/m3 in kitchens.
Nitrogen DioxideNO2 levels were measured successfully in 845 homes, with
812 homes providing results for all three locations (kitchen,
bedroom and outdoors). Minimum, maximum, geometric
mean and percentile values are shown in Table 9. Seasonal
NO2 levels are shown in Table 10.
NO2 levels were significantly higher in kitchens than in
bedrooms, because many homes had cooking-related sources
in the kitchen. In each season, bedroom levels were
significantly lower than the levels outdoors, most likely due
to the removal of infiltrating NO2 by indoor sinks. Indoor
sources would generally have less impact in bedrooms than in
kitchens because they are more likely to be in the kitchen.
NO2 levels in bedrooms were closest to outdoor levels in
summer, when it would be expected that windows were more
likely to be opened.
The most important effects on outdoor NO2 concentration
were of season (F¼ 35.8, Po0.001, Table 10) and area type
(F¼ 26.6, Po0.001, Table 11). Some other significant effects
can probably be explained by the area type, that is, effects of
region, dwelling type and age of home.
Effects on indoor concentrations were dominated by
cooking fuel (see Table 12). The difference between the
groups was highly significant (kitchens: F¼ 343, Po0.001;
bedrooms: F¼ 128, Po0.001) with each group being
significantly different from the other two (all Po0.001).
Heating fuel also had some effect, but this was confounded
with cooking fuel in a way that was difficult to untangle.
Considering only homes with no fossil fuel cooking
appliances, the homes with no fossil fuel heating had a mean
NO2 concentration of 6.7 mg/m3 compared with 15.5mg/m3
for those with individual gas heaters, a difference of only
8.8 mg/m3. The use of an unflued gas heater, including the use
of a gas oven for heating, had a greater effect, especially in
kitchens (F¼ 54.5, Po0.001) and also in bedrooms
(F¼ 19.0, Po0.001) (see Table 13). However, fewer than
10% of homes used unflued heating. Smoking also had only
a small effect but bedroom NO2 was significantly higher
(t¼ 4.0, Po0.001) in smokers’ homes (14.1 mg/m3) than in
other homes (11.1 mg/m3).
The effect of season on indoor NO2 concentrations was
significant (kitchens: F¼ 4.9, Po0.01; bedrooms: F¼ 7.4,
Po0.001). In kitchens, levels were significantly lower in
spring than in other seasons. In bedrooms, levels were highest
in summer.
Table 7. Bedroom CO (mg/m3) by season and extract fan.
Extract fan in home Spring Summer Autumn Winter
Yes 0.38 0.24 0.58 0.59
No 0.32 0.29 0.61 0.65
Table 8. Mean CO levels (mg/m3) by location and area type.
Area type Bedrooms Kitchens
Mean N Mean N
Rural 0.28 234 0.34 235
Suburban 0.41 336 0.52 339
Urban 0.50 220 0.54 222
Central urban 0.69 31 0.72 31
Table 9. Statistics for NO2 concentrations (mg/m3).
Minimum Maximum Geometric
mean
Percentiles
10% 50% 75% 95%
Kitchen 0.8 620.0 21.8 7.2 21.8 40.1 90.0
Bedroom 0.4 752.6 11.9 4.4 12.1 19.8 38.1
Outdoors 1.0 151.6 20.9 9.9 22.5 32.4 48.9
Table 10. NO2 levels (mg/m3) by season.
Spring Summer Autumn Winter
Kitchen 17.2 23.3 23.7 22.3
Bedroom 10.1 14.6 12.7 11.0
Outdoors 15.1 17.0 26.7 22.4
Table 11. Geometric mean outdoor NO2 (mg/m3) by area type.
Rural Suburban Urban Central urban
16.1 21.9 25.0 33.1
Table 12. Geometric mean indoor NO2 (mg/m3) by cooking fuel.
Cooking fuel Kitchens Bedrooms
Mean N Mean N
Natural gas oven 42.8 338 18.2 338
Natural gas cooking but no gas oven 22.4 128 12.8 128
No fossil fuel cooking 11.5 356 7.9 354
Air pollutants in English homes Raw et al.
Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1) S89
As with CO, for kitchen NO2, there was a significant
interaction between season and cooking fuel (Table 14).
Season had a greater effect in homes with a gas oven, where
NO2 levels were lowest in spring and highest in winter. In
homes with some gas cooking but no gas oven, the effect was
much smaller, but in the same direction. In electric-cooking
homes, NO2 levels were highest in summer and autumn and,
again, the variation is small and similar to the pattern seen in
bedrooms. This is depicted in Figure 1.
It seems likely that there was a higher ventilation rate in
summer and that this allowed more NO2 from gas cooking to
escape, but allowed more to enter from outdoors, thus
increasing NO2 levels in electric cooking homes. It is also
plausible that there was more cooking in the cooler months.
Of greater importance is the implication that indoor seasonal
variation results mainly from indoor sources, rather than
variation in outdoor concentrations.
The provision of extract fans had relatively little effect
overall, but resulted in slightly higher NO2 levels where there
was no indoor source and slightly lower levels where there
was an indoor source. An example is shown in Table 15. This
particular interaction was not significant for kitchen NO2
concentrations, suggesting that the effect of fans is more to
reduce spread around the home than to decrease levels in the
source room.
NO2 in kitchens was significantly related to area type
(F¼ 19.1, Po0.001, Table 16). NO2 levels also varied
significantly with dwelling type and age of home, but these
effects are probably explained mainly by the location of the
home.
Taking season and cooking fuel as the initial determinants
of indoor concentrations, the worst case shown in the data is
kitchens with a gas cooker, in winter (50.4 mg/m3) compared
with 9.0 mg/m3 for all-electric kitchens in spring. With some
reasonable assumptions, a somewhat higher value can be
determined. Being in a central urban, rather than rural,
location would add approximately 10–15mg/m3 and using an
unflued heater would add perhaps 20–25 mg/m3. With all
these conditions satisfied, simple summation would suggest
that an average of about 85 mg/m3 might be expected, but the
database is not large enough to confirm the validity of this
summation.
The WHO annual average guideline for exposure to NO2
of 40 mg/m3 (WHO, 2000) was exceeded in kitchens in 25%
of all homes and in 53% of homes with a gas oven. It is
exceeded in bedrooms in fewer than 5% of homes.
Maximum kitchen levels exceeded the WHO 1-h guideline
of 200mg/m3 in 6 months out of 17, and in bedrooms in 2
months out of 17. It can reasonably be assumed that the
guideline was exceeded more frequently for periods of an
hour (i.e. the reference period for the guideline).
Volatile Organic CompoundsVOC results are available for 796 homes. Typically around
150–200 individual VOCs exceeded the detection limit
(0.1 mg/m3) in each home. Of these, 22 were quantified and
seven were selected for statistical analysis: benzene, toluene,
Table 13. Geometric mean kitchen and bedroom NO2 (mg/m3) by
unfueled heater use.
Any use of unfueled heating Yes No
Kitchen NO2 44.7 20.3
Bedroom NO2 17.2 11.5
0
10
20
30
40
50
60
Spring Summer Autumn Winter
Season
Nitr
ogen
dio
xide
con
cent
ratio
n
Gas oven Gas cooking but no oven No fossil fuel cooking Bedroom
Figure 1. Interaction effect of season and cooking fuel on NO2
concentrations (bedroom NO2 concentrations also shown for compar-ison).
Table 14. Geometric mean kitchen NO2 (mg/m3) by cooking fuel and
season.
Cooking fuel Spring Summer Autumn Winter
Gas oven 32.4 41.0 45.4 50.4
Gas cooking but no oven 19.1 21.9 23.1 23.5
No fossil fuel cooking 9.0 13.1 14.1 10.0Table 15. Geometric mean bedroom NO2 (mg/m3) by cooking fueland extract fan.
Any extract fans? Gas cooking No fossil fuel cooking
Yes 15.0 7.8
No 18.1 8.0
Table 16. Geometric mean kitchen and bedroom NO2 by area type
(mg/m3).
Rural Suburban Urban Central urban
Kitchen 14.5 25.9 24.5 31.6
Bedroom 8.4 13.4 13.8 17.6
Air pollutants in English homesRaw et al.
S90 Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1)
m/p-xylene, limonene, undecane, 2,2,4-trimethyl-1,3-penta-
nediol monoisobutyrate (TPDMIB) and 2,2,4-trimethyl-1,3-
pentanediol diisobutyrate (TPDDIB). These were chosen to
represent various groups of substances and different types of
source. Table 17 shows minimum, maximum, geometric
mean and percentile values. The remainder of this section
deals only with TVOC. Results for the individual VOCs can
be found in Coward et al. (2002).
Season significantly affected TVOC (F¼ 11.6, Po0.001),
with significant differences between spring and autumn,
summer and autumn, summer and winter, and autumn and
winter (see Table 18).
Homes where painting had been undertaken during
sampling or during the previous 4 weeks had significantly
higher TVOC concentrations than other homes (F¼ 40.6,
Po0.001). Concentrations were higher where the painting
was in the same bedroom as the sampler than where it was
elsewhere in the home (means 368 vs. 319 mg/m3).
There was a significant effect on TVOC concentration
(F¼ 7.2, Po0.001) of whether the home had an integral
garage (244 mg/m3), detached garage (179 mg/m3) or no
garage (218 mg/m3). Homes with an integral garage had
significantly higher TVOC levels than homes with detached
garages. It is perhaps initially surprising that homes with no
garage had higher TVOC levels than homes with a detached
garage, since homes with no garage tend to be older, and
would therefore be expected to have lower TVOC levels. A
possible reason for this is that, in the absence of a garage,
greater amounts of volatile substances might be stored in the
home. The availability of storage space for decorating
materials, separately from the living space, may therefore
be a critical issue for reducing exposure to VOCs. This is
supported by an interaction between garage and painting for
TVOC (see Figure 2).
After removing data for homes where painting had been
undertaken, a significant effect of building age was found
(F¼ 3.0, Po0.1), with pre-1919 homes having significantly
lower TVOC levels than homes built since 1990 (means 147
vs. 269mg/m3). Over most of the age range, the change was
modest, but became more marked in the newest homes
(Figure 3).
Dwelling type was a significant factor for TVOC (F¼ 2.5,
Po0.05, in homes where no painting had taken place before
or during the study) (see Table 19). Bedsits (a bedsit is a small
apartment in which the living room and bedroom are
combined into a single space) and other flats had higher
levels of TVOC than other dwelling types. This may, again,
relate to the availability of suitable storage space, in addition
to relative ventilation rates and air exchange between
neighboring dwellings.
There are no WHO guidelines for exposure to TVOC but
a number of groups have proposed guideline levels (see
Table 20). In general, TVOC concentrations were low by
these standards, but the group average exceeded 300mg/m3 if
there had been any painting and decorating in a home
without a separate garage, and in homes under 2 years old.
Table 17. Statistics for TVOC and selected VOC concentrations (mg/m3).
Minimum Maximum Geometric mean Percentiles
10% 50% 75% 95%
TVOC 15 3360 210 72 202 352 1010
Benzene o0.1 93.5 3.0 1.0 3.3 5.8 14.6
Toluene 0.3 1783.5 15.1 4.4 14.9 27.9 74.9
m/p-Xylene 0.1 152.8 3.8 0.9 3.7 7.5 30.3
Limonene o0.1 308.4 6.2 1.3 7.1 15.5 51.0
Undecane o0.1 246.6 2.6 0.5 2.3 5.5 33.6
TPDMIB o0.1 770.4 5.1 1.1 5.7 13.5 61.2
TPDDIB o0.1 100.0 1.6 0.5 1.8 3.8 13.8
Table 18. Geometric mean TVOC concentrations by season (mg/m3).
Spring Summer Autumn Winter
189 161 264 208
0
100
200
300
400
500
600
700
Painting in bedroom Painting elsewhere No painting
TV
OC
Garage Integral Garage Other No Garage
Figure 2. Geometric mean TVOC (mg/m3) by painting activity andgarage type.
Air pollutants in English homes Raw et al.
Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1) S91
The group average TVOC concentration exceeded 500 mg/m3
in homes where there had been painting and decorating in the
room where the sample was taken, and there was an integral
garage, or if the home was under a year old.
About 5% of homes exceeded 1000mg/m3. Some occu-
pants exposed to this level of TVOC may well report an odor
nuisance and may suffer some discomfort. Maximum 28-day
average TVOC levels exceeded 2000mg/m3 in 12 months out
of 17 and exceeded 3000 mg/m3 in 3 of these months. At this
higher level, occupants of the homes are likely to suffer
adverse health effects including headache, nausea and slight
narcotic effects.
FormaldehydeResults are available for concentrations of formaldehyde in
833 bedrooms. The geometric mean, minimum, maximum
and percentile values are shown in Table 21. Season had a
significant effect (F¼ 6.8, Po0.001), with a significant
difference between autumn and winter (Po0.001) (see
Table 22).
Formaldehyde concentrations varied significantly with
building age (F¼ 22.0, Po0.001), newer homes having
higher concentrations (Figure 4).
A second factor that was shown to be a determinant of
formaldehyde concentration was the presence of particle-
board flooring in the home. The mean concentration
recorded in the 145 homes with particleboard floors was
32.0mg/m3, while the mean concentration for the 673 homes
without particleboard flooring was 20.3mg/m3. There was a
significant difference between these concentrations (t¼ 7.0,
Po0.001). Homes with particleboard floors were then
grouped according to whether or not there was a particle-
board floor in the main bedroom where formaldehyde was
measured. Homes with a particleboard floor in the main
bedroom were found to have a higher mean concentration
(37.7 mg/m3) than homes where the particleboard flooring
was situated elsewhere in the home (23.2 mg/m3). A
significant difference was found between these groups
(t¼ 4.5, Po0.001).
Overall, it seems that formaldehyde exposure in the home
is likely to be of concern only in new homes. The 3-day mean
concentrations in six homes (0.7% of the total) exceeded the
WHO 30 min air quality guideline of 100mg/m3 (WHO,
2000). Of these six, five were built after 1995, that is, within
about 3 years of the study. Levels in two very new homes,
built since 1998, were 135 and 128 mg/m3. Levels in homes
built 1 year earlier were on average considerably lower. The
WHO guideline value may have been exceeded over a 30-min
period in a greater number of homes.
0
100
200
300
400
500
600
1991 1992 1993 1994 1995 1996 1997 1998
TV
OC
con
cent
ratio
ns (
µg m
-3)
Figure 3. TVOC levels in homes built since 1990.
Table 19. Geometric mean TVOC concentration by dwelling type
(mg/m3).
Bedsit
or flat
Terraced Semi
detached
Detached Bungalow
TVOC 224 165 172 190 178
Table 20. Suggested TVOC guideline concentrations (mg/m3).
Reference Concentration Comment
Dingle and Murray (1993) 500 No single compound should contribute 450%
M�lhave, L (in European Concerted Action, 1992) o200 Comfort range
200–3000 Multifactorial exposure effects
3000–25,000 Discomfort
425,000 Toxic
Seifert, B (in European Concerted Action, 1992) 300 Target guideline value; no individual compound should exceed 10% of
target value
Finnish Society of Indoor Air Quality and Climate (1995) o200 Target values of indoor climate; best air quality; 90% of occupants
satisfied
o300 Intermediate air quality; room may have slight odor
o600 Minimum requirement
Japanese Ministry of Health, Labor and Welfare (2000) o400 Advisable TVOC value for indoor air quality for residential air
Air pollutants in English homesRaw et al.
S92 Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1)
Conclusion
It is apparent that, in the majority of homes in England,
concentrations of the measured pollutants are low for most of
the time. However, some homes have concentrations that
would suggest a need for precautionary mitigation.
The survey has identified many factors influencing
concentrations of CO, NO2, TVOC and formaldehyde in
homes. While we can draw conclusions only about those
independent variables that were included in the study, those
variables were selected on the basis of past findings and a
logical analysis of what might have an effect on one or more
of the pollutants.
The most important omission is probably that ventilation
rate was not measured; this is difficult enough to do in a
single home in a way that represents ventilation rate
throughout the home and under different conditions of
outdoor climate and operation of ventilation devices. For the
number of homes in this study, it would have been
impossible. However, the presence and use of various
ventilation devices was assessed, and this should reveal any
major effects of ventilation that occur.
Few of the findings are individually unique to this paper
(see Spengler et al. (2001) for a wide-ranging review of
pollutants and their determinants), but the collection of
findings for a national sample is unusual and provides much
better data than we have previously seen in the UK or a
comparable country. From these results, it is possible to
identify those factors that are most likely to lead to exposures
of concern in homes. These factors are:
� gas cooking (for CO and NO2);
� the use of unflued appliances for heating (for CO and
NO2);
� emissions from materials in new homes (for TVOC and
formaldehyde);
� painting and decorating, with a significant increase in risk
suspected to exist where there is not a place to store
materials away from the living space (for TVOC).
Other factors had an effect, but not so great an effect that
they are likely to lead to hazardous exposures to the
pollutants measured. These factors are:
� gas heating appliances (for CO and NO2);
� tobacco smoking (for CO and NO2);
� lack of extract ventilation in rooms with a significant
pollutant source (for CO and NO2);
� outdoor concentrations (for CO and NO2).
This is not to say that the above factors will always result
in hazardous exposures, or that the hazard will be great in
most cases. Also, some exposures will either (a) be reduced
naturally over time as materials age, or (b) be significant only
in some rooms in the home and/or for part of the day. Even
so, there are clear implications for mitigation of exposure and
these are consistent with current thinking derived from other
work:
� avoid being in the same room as gas cooking activities,
especially if a gas oven is in use, and/or ensure good
extract ventilation close to gas cooking appliances;
� use low-emission materials in the construction and
furnishing of homes, and ensure good ventilation,
especially during construction and the first year of
occupancy;
� efforts to improve the outdoor air will lead to improve-
ments in the indoor air, especially in winter in urban areas,
but will do little to affect the largest exposures indoors;
� the mere provision of ventilation devices has little effect Fthey need to be used (obvious but worth emphasizing);
� avoid exposure to tobacco smoke.
It is noteworthy that seasonal effects on CO and NO2 were
due largely to the presence of indoor sources, combined with
seasonal variations in air change rate. Outdoor seasonal
variations appear to have little impact on indoor concentra-
tions. This would need to be considered when interpreting
time series studies of the effect of outdoor air pollution on
health.
Table 21. Statistics for formaldehyde concentration (mg/m3).
Minimum Maximum Geometric mean Percentiles
10% 50% 75% 95%
1 171 22.2 9.8 24.0 35.2 61.2
Table 22. Mean formaldehyde concentration by season (mg/m3).
Spring Summer Autumn Winter
Concentration 21.0 22.5 26.1 19.5
0
5
10
15
20
25
30
35
40
45
HC
HO
con
cent
ratio
ns (
µg m
-3)
Before1919
1919-1940
1941-1960
1961-1970
1971-1980
1981-1985
1986-1990
1991-1998
Figure 4. Geometric mean formaldehyde concentration by buildingdate.
Air pollutants in English homes Raw et al.
Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1) S93
It is also of some significance that the critical factors are
related much more to sources than to provision for
ventilation: source control is therefore, as would be expected,
the most appropriate approach to reducing the risk of
hazardous exposure to air pollutants in homes.
Acknowledgements
The work was commissioned and funded by the Chemicals
and Biotechnology Division of the Department of the
Environment, Transport and the Regions, now the Depart-
ment of the Environment, Food and Rural Affairs
(DEFRA). Palmes Tubes were analyzed by AEA Technol-
ogy, Harwell, England. Advice on sampling methods for CO
and NO2 was provided by Dr. David Ross of BRE. Dr. Jeff
Llewellyn played a major role in managing the whole project
and the authors are grateful for his support.
References
Apling A.J., Stevenson K.J., Goldstein B.D., Melia R.J.W., and Atkins D.H.F.
Air pollution in homes 2: validation of diffusion tube measurements of
nitrogen dioxide. Warren Spring Laboratory Report LR 311 (AP), WSL,
Stevenage,, 1979.
Atkins D.H.F., Healy C., and Tarrant J.B. The use of simple diffusion tubes for
the measurement of nitrogen dioxide levels in homes using gas and electricity
for cooking. AERE Report R9184, AERE Harwell, Oxfordshire, 1978.
Berry R.W., Brown V.M., Coward S.K.D., Crump D.R., Gavin M., Grimes
C.P., Higham D.F., Hull A.V., Hunter C.A., Jeffery I.G., Lea R.G.,
Llewellyn J.W., and Raw G.J. Indoor air quality in homes. The BRE Indoor
Environment Study. BRE Reports BR299 and BR300, CRC press, London,
1996.
Brown V.M., Crump D.R., and Mann H.S. The effect of measures to alleviate the
symptoms of asthma on concentrations of VOCs and formaldehyde in UK
homes. Proceedings of Indoor Air ‘96, Vol. 4, Indoor Air ’96, Nagoya, 1996:
pp. 69–74.
Brown V.M., Mann H.S., and Crump D.R. Formaldehyde and VOC levels in
homes in England. Proceedings of Indoor Air 99, Vol. 4, CRC press, London,
1999: pp. 95–100.
Coward S.K.D., Brown V.M., Crump D.R., Raw G.J., and Llewellyn J.W.
Indoor air quality in homes in England: volatile organic compounds. BRE
Report 446, CRC press, London, 2002.
Coward S.K.D., Llewellyn J.W., Raw G.J., Brown V.M., Crump D.R., and Ross
D.I. Indoor air quality in homes in England. BRE Report 433, CRC press,
London, 2001.
DETR. Housing in England 1997/98, ISBN 0116213655, 1999: (also available on
DEFRA Statbase Website).
Dingle P., and Murray F. Control and regulation of indoor air: an Australian
perspective. Indoor Environment 1993: 2: 217.
European Concerted Action. Guidelines for ventilation requirements in buildings.
ECA Indoor air quality and its impact on man, Report No. 11. Report EUR
14449 EN, Commission of European Communities, Luxembourg, 1992.
Finnish Society of Indoor Air Quality and Climate. Classification of Indoor
Climate, Construction and Finishing Materials, Finnish Society of Indoor Air
Quality and Climate, Helsinki, 1995.
Japanese Ministry of Health, Labor and Welfare. Committee on Sick House
Syndrome: Indoor air Pollution, Progress Report No. 1 F Summary of
Discussions from the 1st to 3rd Meetings, 26 June 2000,, 2000.
Pannwitz K.-H. Monitoring of inorganic air contaminants in indoor environments
by direct reading diffusion tubes. Proceedings of Indoor Air ‘87, Vol. 1,
Institut fur Wasser- Boden- und Lufthygiene, Berlin, 1987: pp. 440–444.
Ross D.I., and Wilde D.J. Continuous monitoring of nitrogen dioxide and carbon
monoxide levels in UK homes. Proceedings of Indoor Air 99, Vol. 3, CRC
press, London, 1999: pp. 147–152.
Spengler J.D., Samet J.M., and McCarthy J.F. Indoor Air Quality Handbook.
McGraw-Hill, New York, 2001.
Venn A., Cooper M., Brown V., Crump D., Britton J., and Lewis S. Common
indoor air pollutants in the home and the risk and severity of wheezing illness
in school children. Paper submitted to the Conference of the American
Thoracic Society, May, 2001.
Wiech C.R., and Raw G.J. Asthma, dust mites, ventilation and air quality: study
design and initial carbon monoxide results. Proceedings of Healthy Buildings
‘95, Vol. 1, Healthy Buildings ’95, Milan, 1995: pp. 425–430.
Wiech C.R., and Raw G.J. The effect of mechanical ventilation on indoor nitrogen
dioxide levels. Proceedings of Indoor Air ‘96, Vol. 2, Indoor Air ’96, Nagoya,
1996: pp. 123–128.
World Health Organization. Guidelines for Air Quality. WHO, Geneva, 2000.
Air pollutants in English homesRaw et al.
S94 Journal of Exposure Analysis and Environmental Epidemiology (2004) 14(S1)