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Original Paper
Experimental Investigation
of Indoor Air Pollutants
in Residential Buildings
Caren C.L. Tan Karen N. Finney Qun Chen
Nigel V. Russell Vida N. Sharifi Jim Swithenbank
Sheffield University Waste Incineration Centre, Department of Chemical and Biological Engineering,
University of Sheffield, UK
Key Words
Air exchange rate E Emission rates E Indoor air
pollution E Particle composition E Particle
morphology E Particulate matter
Abstract
Indoor air quality is affected by many factors, including
energy provision/use. The main objective of this
research was to investigate indoor air pollutant emissions due to energy use in residential buildings, with a
specific focus on particulate matter (PM). Three environments were compared: (a) a rural house with an
electric cooker; (b) a city-centre flat with a gas cooker;
and (c) an urban flat on a main road, also with gas
appliances. Concentrations of PM, CO, NO2 and VOCs
were measured in the kitchens and emission rates were
calculated for cooking periods. Although there has been
a great deal of research examining the effects of
gaseous pollutants in the indoor environment, this is
one of the first studies to specifically focus on PM. Most
particles were small (2.5 mm) and thus respirable. The
elemental analysis of the PM revealed high metal
concentrations (Fe/Na/Zn), whilst their morphologies
indicated these were present as salt, skin and particles
of biological origin. Gaseous emissions, particularly
NO2 and CO, were more prevalent in homes with gas
Nomenclature
a Air exchange rate (h1)
Cin Indoor mass concentration of pollutants
(mgm3)
Cout Outdoor mass concentration of pollutants
(mgm3)
EDS Energy dispersion X-ray system
k Pollutant removal rate (h1)
NOx Oxides of nitrogen
p Penetration coefficient across building
envelope
PM Particulate matter
Se Emission rate (mgh1)
SEM Scanning electron microscopy
t Sampling time (h)
V Volume of the room (m3)
VOCs Volatile organic compounds
t Cooking time (h)
RVOCs Sum (total) of top 20 volatile organic
compounds
Karen N. Finney,
Sheffield University Waste Incineration Centre, Department of Chemical and
Biological Engineering, University of Sheffield, Mappin Street, Sheffield, S1 3JD,
UK Tel. 44 (0)114 222 7563, Fax. 44 (0)114 222 7501
E-Mail k.finney@sheffield.ac.uk
Introduction
We spend the vast majority of our time indoors on
average 90%. We control these indoor environments for
health, thermal comfort and productivity. However,
maintaining the quality of the environment in buildings
can have considerable consequences both on human health
and on the local and global environment. The quality of
the indoor environment is affected by many factors,
including the design of buildings, ventilation, energy
provision/use, thermal insulation and household activities
such as cleaning.
Tan et al.
Particulate Matter
The TSI Dust-Trak 8532 aerosol monitor was used to
measure the real-time PM2.5 concentrations in each indoor
and outdoor environment. The detection range was 0.001
150 mgm3 and the resolution was 0.1% of the reading.
The log interval of the concentration data was set at 30 s.
Although the particle size range of the instrument was 0.1
10 mm, during these measurements a size-selective impactor was attached to the inlet (with a cut size of 2.5 mm),
which pre-conditioned the size range of particles
(52.5 mm) entering the instrument.
For Cases 1 and 3, additional particle collection and
analysis was conducted. A multi-stage, multi-orifice
cascade Andersen 0.0283 m3min1 Ambient Particle
Sizing Sampler (Mark II version, Thermo Electron
Corp.) was used to collect PM samples from the kitchen
(Cases 1 and 3), as well as a bedroom and the outdoor
environment (Case 1 only) in order to establish the particle
size distribution. The sampler was calibrated with 1 gcm3
spherical particles. A pre-separator was used to prevent
particles greater than 10 mm from entering the subsequent
stages, which could help minimise particle bouncing and reentrainment errors. In each of the eight stages of
the Andersen sampler, aluminium foil was used as the
collection substrate and was placed on top of the collection
plates. The bedroom that was monitored for Case 1 had
dimensions of 4 3 2.5 m3. There was only one window in
this room. The sampling position was at the centre of the
room at a height of 1 m. Samples were collected in the
bedroom over a period of 6 weeks (1008 h). PM10 samples in
the outdoor environment were collected over a period of
1085 h, at a height of 2 m from the ground. Indoor samples
were taken over a monitoring period of 4 weeks in each case.
All PM samples collected were then analysed to
determine the particle morphology and composition. The
morphology of the PM10 samples was studied using
scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS). It was used to characterise
the bulk specimen from 1 to 100 mm. The EDS allowed
both qualitative and quantitative microanalysis and X-ray
mapping. Digital images were acquired using various
software packages available on the computer linked to
the SEM. In addition, the chemical composition (elemental analysis) of the PM10 samples was determined
using a Spectro Ciros inductively coupled plasma (ICP)
emission spectrometer.
Gaseous Pollutants
CO concentrations were measured for all three cases
using a TSI IAQ-Calc Model 7545 analyser. This
(a)
Sampling point
(b)
Sampling point
Up
HW
Balcony
(c)
U
NOT TO SCALE
Fig. 1. Layout of the kitchen for each case study environment: (a) the rural house Case 1; (b) the city-centre flat Case 2; and (c) the urban
flat on a main road Case 3.
Tan et al.
instrument is a hand-held portable device that simultaneously measures CO, CO2, temperature and relative
humidity. The CO sensor/detector was electro-chemical,
which was calibrated to a range of 0 to 500 ppm. CO2 was
measured using the non-dispersive infrared spectrometry
technique. The logging interval was 30 s for both species.
Different types of diffusion tubes were deployed to
monitor NO2 and VOCs. To measure NO2 concentrations,
Palmes-type diffusion tubes (Gradko International, 20%
triethanolamine) were used, which are widely utilised in
the UK for determining ambient nitrogen dioxide (NO2)
concentrations [10]. The analytical expanded measurement
uncertainty for the diffusion tubes in this study was
3.69%. The detection limit was 0.4 ppb (or 0.34 mgm3)
over a 2-week exposure period in each environment. The
tubes were stored in a sealed container in a refrigerator
prior to use. The tube was vertically mounted with the
open end at the bottom. NO2 was absorbed as nitrite in the
tubes. After exposure for 24 weeks, the lower end cap was
replaced and the NO2 concentration was quantitatively
determined using UV spectrophotometry (UVS04
Camspec M550). This gave the average concentration
over the entire exposure period for each case study.
For VOCs, DIFTXTA (Gradko International) VOC
diffusion tubes were used. The VOC sampler consisted of a
stainless steel tube (6.3 mm OD 5.0 mm ID 90 mm
length) filled with a solid polymer absorbent (TENAX
TA) with two brass Swagelok caps. During passive
sampling, an aluminium air diffuser was fitted to the
sampling end of the tube. After 34 weeks exposure, the
diffusion tubes were returned to Gradko for analysis and
the results were given as VOC concentrations. The
absorbent in the tubes was analysed through thermal
desorption and mass spectroscopy. The masses of the top
20 VOCs were identified. The analytical measurement
error was 14.8%. It should be noted that the average
VOC concentration over the period of exposure was
measured using this method.
Air Exchange Rate
Air exchange rates for the kitchen in each residential
building were also determined to aid the calculation of
pollutant emission rates. Building air exchange rates are
associated with the wind and thermally induced pressure
flows, as well as mechanical ventilation. The air exchange
rate can be measured through the tracer gas decay method,
the constant injection method or the constant concentration method. The concentration decay method is the most
widely used air exchange measuring technique and this is
the method employed in this study to determine the air
t2
t1
dCin t
a k
S
out
Cin t Vak
paC
ak
t2
dt
t1
Thus,
Cin t2
p a Cout S=V
ak
p a Cout S=V
Cin t1
ak
expa kt2 t1
The emission rate of a particular pollutant can consequently be solved from Equation (4):
paCout
out
C
t
Cin t2 paC
in 1
ak
ak
exp a kt2 t1 V a k
4
Se
1 expa kt2 t1
In this study, the concentrations of both CO and PM2.5
were measured; real-time values were monitored on a
continuous basis. The emission rates of CO and PM2.5
from indoor cooking activities can therefore be obtained
from Equation (4). For NO2 and VOCs, however, only
average concentrations can be obtained from the method
used (different types of diffusion tubes). Integrating each
term of Equation (1) over the sampling period gives
Equation (5):
Zt
Zt
Zt
dCin t p a
Cout tdt a k
Cin tdt
0
0
0
5
Zt
Se
dt
0 V
Since the average values of outdoor and indoor
concentrations are known, the average pollutant emission
rate can be defined by Equation (6):
Cout 1t
Se
Rt
0
Rt
0
Cin tdt,
6
R
1 t
t
0 Se tdt
2600
2400
2200
2000
Case 1
1800
Case 2
1600
Case 3
1400
Air exchange rate: 1.45 hr-1
1200
1000
800
0
8
Time (mins)
10
12
14
16
Fig. 2. CO2 concentration decay curves in the kitchens of all residential case study environments.
Tan et al.
was 0.9 0.1 hr1. The air exchange rates in all three
case studies were expected.
Particulate Emissions
Comparison of PM2.5 for all Three Case Study
Environments
PM2.5 Concentrations
Figure 3 shows the real-time concentrations of indoor
PM2.5 in the kitchens for all three case studies. Figure 3(a)
shows that the indoor PM2.5 concentration in the rural
house, Case 1, remained constant at around 1012 mgm3
during the initial measurement period; this is most
likely due to the fact that the house was unoccupied
during this part of the sampling period. This unoccupied
period gave a background reading for this case study
environment.
PM2.5 concentrations in the kitchen were found to
increase when there were more indoor activities taking
place. As shown in Figure 3(a), the highest value achieved
was 198 mgm3, where the spikes coincided with cooking
activities. Overall, the average indoor PM2.5 concentration
was 16 mgm3. This was slightly higher than the value
obtained using the Andersen sampler. The Andersen
sampler suggested that the average indoor PM2.5 concentration was 89 mgm3. The outdoor PM2.5 concentration
near the house was about 10 mgm3, similar to the indoor
background levels.
The real-time indoor PM2.5 concentrations in the
kitchen of the city-centre flat are presented in Figure 3(b)
Case 2. As shown, the PM2.5 spikes were much higher
than those for Case 1, often by an order of magnitude.
This is due to the type of cooker used the city-centre
flat has a gas cooker compared to an electric cooker in
the rural house. Other possible sources of such high
PM2.5 concentrations may include burnt food and
different cooking techniques, such as more frying with
cooking oil. The fumes emitted from frying pans can
nucleate, forming ultrafine particles inside the kitchen.
Most coarse particles generated in the kitchen are known
to be from frying and spattering during cooking [13].
The average indoor PM2.5 concentration in this kitchen
was 40.6 mgm3, much higher than Case 1, whereas the
average outdoor PM2.5 concentration near the flat was
14 mgm3, which is more similar, but still slightly
elevated compared to the rural house. Figure 3(c)
shows the real-time concentrations of indoor PM2.5 in
the kitchen of Case 3 the urban flat on a main road.
The average indoor PM2.5 concentration measured in
this environment was 38 mgm3, similar to Case 2 and
(a) 200
180
160
140
120
100
80
60
40
20
0
13/07 14/07 15/07 16/07 17/07 18/07 19/07 20/07 21/07 22/07 23/07 24/07 25/07
(b) 2000
1800
1600
1400
1200
1000
800
600
400
200
0
2/8
3/8
4/8
5/8
6/8
7/8
8/8
(c)
Fig. 3. Real-time concentrations of indoor PM2.5 in the kitchens of (a) the rural house Case 1; (b) the city-centre flat Case 2; and (c) the
urban flat on a main road Case 3.
Tan et al.
(a) 90
20/07/2009 (1)
80
20/07/2009 (2)
22/07/2009
70
60
50
40
30
22.5 mg/hr
20
5.4 mg/hr
6.4 mg/hr
10
0
0
10
20
30
40
50
60
70
80
250
31/07/2009
01/08/2009
04/08/2009
200
150
100
50
0
0
10
20
30
40
50
60
70
80
30
22/09/2010
27/07/2009
23/09/2010
28/07/2009
25
24/09/2010
31/07/2009
28/09/2010
01/08/2009
20
29/09/2010
04/08/2009
15
10
0
0
10
20
30
40
50
60
70
80
-5
(a)
Cut-off diameter, m
1.1
2.1
3.3
4.7
5.8
10
3.0
12
2.5
10
2.0
1.5
1.0
0.5
14
3
0.7
3.5
0.0
0.4
0
0-0.4
0.4-0.7
0.7-1.1
1.1-2.1
2.1-3.3
3.3-4.7
4.7-5.8
5.8-9.0
9.0-10
5.8
10
Aerodynamic diameter, m
(b)
Cut-off diameter, m
0.4
0.7
1.1
2.1
3.3
4.7
1.2
2.5
0.8
2.0
0.6
1.5
0.4
1.0
0.2
3.0
1.0
3.5
0.5
0.0
0.0
0-0.4
0.4-0.7
0.7-1.1
1.1-2.1
2.1-3.3
3.3-4.7
4.7-5.8
5.8-9.0
9.0-10
Aerodynamic diameter, m
Fig. 5. Mass size distribution of PM10 collected from (a) the kitchen; (b) bedroom; and (c) outdoor environment at the rural Hathersage
house Case 1; and (d) the kitchen at the urban Sheffield flat Case 3.
10
Tan et al.
Cut-off diameter, m
1.1
2.1
3.3
4.7
5.8
10
16
4.0
14
3.5
12
3.0
10
2.5
8
2.0
6
1.5
4
1.0
0.7
4.5
0.4
0.5
0.0
0
0-0.4
0.4-0.7
0.7-1.1
1.1-2.1
2.1-3.3
3.3-4.7
4.7-5.8
5.8-9.0
9.0-10
Aerodynamic diameter, m
(d)
Cut-off diameter, m
0.4
0.7
1.1
2.1
3.3
4.7
5.8
10
4.0
30
3.0
20
2.5
2.0
15
1.5
10
1.0
5
25
3.5
0.5
0.0
0
0-0.4
0.4-0.7
0.7-1.1
1.1-2.1
2.1-3.3
3.3-4.7
4.7-5.8
5.8-9.0
9.0-10
Aerodynamic diameter, m
Fig. 5. Continued.
11
160
Bedroom-Case 1
140
Kitchen-Case 1
120
Outdoor-Case 1
Kitchen-Case 3
100
80
60
40
20
0
Al
Ba Ca Cr Cu Fe
K Mg Mn Na
Pb
Si
Zn
Fig. 6. Chemical composition of the PM10 samples collected from the bedroom, kitchen and the outdoor environment of the rural house
Case 1 and kitchen of Case 3 using ICP-OES.
12
Tan et al.
(a)
(b)
(c)
(d)
A
B
Fig. 7. Morphology of the PM collected from (a and b) the kitchen; (c) bedroom; and (d) the outdoor environment of rural house Case 1.
13
Fig. 8. An example of the EDS analysis of the PM collected from the kitchen of Case 3.
(a) 22
20
18
16
14
12
10
8
6
4
2
0
27/07
28/07
29/07
30/07
31/07
01/08
02/08
03/08
04/08
(b)
Fig. 9. Real-time concentrations of indoor CO in the kitchens of (a) the city-centre flat Case 2 and (b) the urban flat on a main road
Case 3.
14
Tan et al.
Table 1. Average indoor and outdoor concentrations and emission rates of carbon monoxide, nitrogen dioxide and total VOCs at the three
study locations
Case 1: rural house
Indoor
CO
Average
Average
NO2
Average
Average
R20 VOCs
Average
Average
concentration (ppm)
emission rate (gh1)
Outdoor
Outdoor
Indoor
Outdoor
1.0
0.1
2.0
0.1
1.1
0.1
concentration (mgm3)
emission rate (mgh1)
10.2
10.8
47.1
65.5
14.7
20.7
23.4
concentration (mgm3)
emission rate (mgh1)
221.5
13.0
42.6
430.7
42.7
65.4
49.7
0.5
32.6
15
(a) 8
27/07/2009
28/07/2009
29/07/2009
31/07/2009
01/08/2009
02/08/2009
03/08/2009
6
5
4
3
2
1
0
0
10
20
30
40
50
Cooking time, min
60
70
80
(b)
16
Tan et al.
-m
T
et
U olu
n d en
Be hyle e
nz 2N can
en (1A e, m p- ona e
ce 1 et X n
tic ,2 hy yl e
ac ,4-t let ene
id rim hy
,
.al but eth l)ph yl yl
a. es E -P te
Et uc ine r
a
Be hylb lyp ne
nz en tol
Te othi zen
tr az e
P
Cy
e ad ol
cl Et nta eca e
o
d n
N hexhyl eca e
on a A n
an ne ce e
e, ,pr tat
2- op e
m y
Tr eth lN
on
i y
an Bdec lBe e, e an
nz 3- nz e
en me en
e, th e
p y
o- rop lBe Tric
X y
hl D yle ln
Be zen
or e ne
oe ca
nz e,
th n e
en 1,
yl
e, 2,3
Be
e
1
nz
,3 tri Phe ne
,5 m no
en
-tr et l
e,
im h y
2et let
h
hy
l-1 Styr ylH
,4 e en
-d p t e
im an
et e
hy
l-
Be
nz
en
e,
1
3
H
ep
lu
D ene
e
p- ca
X n
no B
U yle e
l, e n
nd n
2, ze
ec e
5- n e
a
bi ,
s( (1 D Non ne
1, - m o a
1- e d ne
d th ec
1S ime yle ane
-.a thy thy
lp le l)
ha th .-P yl)
Be
3- ine nz
Be T Car ne
en
nz rid en
e,
Be
yl ec e
1nz
A an
m
en
l e
e
Be e,
th o- coh
yl X ol
nz 1e
en th E 2- yle
Be e, 1 yl- thy prop ne
Be
nz -m 3,5 lbe yl
en et -d nz nz
e, hy im en
en
1, l-3 et e
e,
3, -p hy
15- r lm
tr op
et
hy
Te ime yll-2
t t
-(1 Na rade hyl-m ph ca
e t t ha ne
Be P
hy le
nz en
le ne
en ta
t
e, ne H hyl)
1, , 3 e x 2, -m an
4- e e
tri th
Pe
m yl
nt
et an
h
e, Ph yl2- e n
Cy
m o
e l
cl
Be thy
op
nz len
t a O en
ne c e
, m tan
et e
hy
lPh
e
To
(a) 100
Indoor
80
Outdoor
60
40
20
(b) 250
200
Indoor
Outdoor
150
100
50
(c) 16
14
12
Indoor
Outdoor
10
Fig. 11. Top 20 VOCs in the samples taken from indoor and outdoor environments at (a) the rural house Case 1; (b) city flat Case 2;
and (c) urban flat on a main road in Sheffield Case 3.
17
very low, just 0.5 mgh1 (Table 1). The reason for the
elevated R20 VOCs concentration in the city-centre flat
(Case 2) is most likely to be due to the difference in
cooking styles, as well as subtle differences in the gas
cookers used; emission rates of around 43 mgh1 were
calculated for such species here. The possible sources of
these indoor VOCs include combustion by-products
(gas stoves) and cooking activities (emissions from
food), as well as cleaning products and the various
construction materials used in the buildings.
The top 20 VOCs found at Cases 1, 2 and 3 are shown
in Figure 11. Toluene was by far the most common VOC
to be found in the indoor environment for both Cases 1 and
2: concentrations of this aromatic hydrocarbon reached
over 80 mgm3 at the rural house (Case 1), whereas
levels exceeded 200 mgm3 inside the city-centre flat (Case
2). This was also one of the most common VOCs found in
the outdoor environment at Case 1. Undecane and
pentadecane appeared to be the most common VOCs
found in the indoor and outdoor environment of Case 3,
respectively. Undecane reached indoor levels of 6 mgm3,
whereas pentadecane exceeded 12 mgm3 in the outdoor
environment. A number of other hydrocarbons were also
found mainly alkanes, such as decane, nonane and hexane.
Conclusions
This investigation into indoor air pollutants in different
residential buildings has shown that there are variations in
both the gaseous and solid-phase emissions in the indoor
and outdoor environments, as illustrated by the three case
studies presented herein. The main conclusions from this
experimental work are as follows:
. PM collected from the indoor environment of the rural
house were mostly composed of small particles
.
.
Acknowledgement
The authors thank the UK Engineering and Physical Sciences
Research Council (EPSRC PUrE Intrawise Consortium
(grant reference no.: EP/F007132/1): Pollutants in the Urban
Environment Integrated Framework for Improving
Sustainability of the Indoor Environment) for their financial
and technical support for this research study.
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Tan et al.
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19