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Environ Monit Assess (2014) 186:151–163

DOI 10.1007/s10661-013-3362-5

Determining the ventilation and aerosol deposition rates


from routine indoor-air measurements
Christos H. Halios & Costas G. Helmis &
Katerina Deligianni & Sterios Vratolis &
Konstantinos Eleftheriadis

Received: 10 February 2013 / Accepted: 24 July 2013 / Published online: 14 September 2013
# Springer Science+Business Media Dordrecht 2013

Abstract Measurement of air exchange rate provides ventilation rate, the outdoor measured number concentra-
critical information in energy and indoor-air quality tions and the particle loss rates as input values. The model
studies. Continuous measurement of ventilation rates is results for the indoors’ concentrations were found to be
a rather costly exercise and requires specific instrumen- compared well with the experimentally measured values.
tation. In this work, an alternative methodology is pro-
posed and tested, where the air exchange rate is calcu- Keywords Indoor air quality . Ventilation rate . Particle
lated by utilizing indoor and outdoor routine measure- loss rate . Urban aerosol
ments of a common pollutant such as SO2, whereas the
uncertainties induced in the calculations are analytically
determined. The application of this methodology is dem- Introduction
onstrated, for three residential microenvironments in
Athens, Greece, and the results are also compared against In indoor settlings, ventilation is one of the main factors
ventilation rates calculated from differential pressure that control thermal comfort and air quality, by regulat-
measurements. The calculated time resolved ventilation ing the indoor temperature, relative humidity, wind
rates were applied to the mass balance equation to esti- speed and concentrations of gases and particles. In a
mate the particle loss rate which was found to agree with literature review study (Sundell et al. 2011), it has been
literature values at an average of 0.50 h−1. The proposed reported that a dose–response relationship between Sick
method was further evaluated by applying a mass balance Building Syndrome related with health symptoms and
numerical model for the calculation of the indoor aerosol outdoor airflow rate has been indicated by several stud-
number concentrations, using the previously calculated ies, even though the nature of this relationship is not
quite clear; in particular, high ventilation rates, are as-
sociated with reduced health symptoms.
C. H. Halios
Findings on health risks from environmental expo-
Department of Meteorology, University of Reading,
P.O. Box 243, RG6 6BB Reading, UK sure to ultrafine particles in school classrooms in urban
areas reveal that the main source of the particles is
C. G. Helmis : K. Deligianni infiltration of outdoor emissions (Diapouli et al. 2008)
Department of Environmental Physics and Meteorology,
and the lifetime of particle indoors is dependent on the
Faculty of Physics, University of Athens, Building Phys 5,
University Campus, 157 84 Athens, Greece ventilation rate as well as on other parameters and
processes. The deposition of particles on indoor surfaces
S. Vratolis : K. Eleftheriadis (*) leads to their removal from the indoor air. As the cumu-
E.R.L., Institute of Nuclear Technology and Radiation
lative effect of these processes (deposition and coagula-
Protection, National Center for Scientific Research
“DEMOKRITOS”, Ag. Paraskevi, 153 10 Athens, Greece tion) is very difficult to be measured directly, they can be
e-mail: elefther@ipta.demokritos.gr estimated indirectly when the ventilation rate and the
152 Environ Monit Assess (2014) 186:151–163

pollutant concentrations are provided (Smolik et al. calculation of ventilation in buildings. The
2005; He et al. 2005). Multizone models solve mass, energy, and
Ventilation influences other mechanisms that con- chemical-species conservation equations assuming
cern the presence and evolution of indoor pollution uniform air temperature and chemical-species con-
such as deposition and sorption. Particle deposition is centration in a zone (Axley 2007). Zonal models
a function of the ventilation rate, with high ventilation divide a room into a limited number of cells and the
rates associated to high deposition rates (Nomura et al. temperature is calculated in each cell, whereas
1997), probably because of the enhanced indoor-air CFD models numerically solve a set of partial
flow intensity which in turn results in higher friction differential equations for the conservation of mass,
velocity (Lai and Nazaroff 2000; Zhao and Wu 2007). momentum (Navier–Stokes equations), energy,
In addition, it has been found that under small ventila- chemical-species concentrations, and turbulence
tion rates (e.g., 0.1 h−1), the sorption effect of materials quantities (Chen 2009).
with strong sorption capacity such as carpet and cush-
Ventilation that is obtained from analytical or semi-
ion should be considered, whereas under high ventila-
empirical relationships is widely used because of its
tion rates (e.g., 20 h−1) sorption may be neglected for
simplicity, even though it may not be accurate for
most materials (Deng et al. 2012).
complicated real-life situations (Chen 2009; Cornick
The ventilation rate can be directly calculated by
and Kumaran 2008); even experimental measurements
three methods: (a) experimentally, (b) by analytical or
may not be free from errors (Melikov et al. 2007). In
empirical relationships and (c) by model simulations
any case, full-scale or in situ measurements are used as
(Chen 2009).
reference to validate numerical models (Zhang et al.
2007).
(a) Direct measurement of ventilation can be obtained
This study aims to present a method for the contin-
in the frame of large- or small-scale experiments.
uous calculation of the ventilation rates, utilizing rou-
During small-scale experiments the ventilation is
tine measurements of indoor and outdoor key pollut-
evaluated with a reduced scale model of the build-
ants such as SO2, and limited ventilation measure-
ing or room, e.g., an experimental system consisted
ments, both common in indoor air studies, whereas
of a small acrylic tank of height 31 cm filled with
the uncertainties induced in the calculations were de-
water which simulates the natural ventilation in a
termined. The ventilation rates were also calculated by
building with heating at multiple levels (Livermore
a semi-empirical model, i.e., from the differential pres-
and Woods 2007). During large scale and in situ
sure measurements based on a method that can be
experiments, the ventilation rates are measured
found in the literature. Then, the obtained ventilation
usually using tracer gas methods. The tracer gas
rates were employed to calculate the loss rates of the
method involves the continuous measurement of a
particle number concentration. Finally, the two differ-
tracer gas, i.e., a nontoxic, nonreactive gas (for
ent methods for the calculation of the ventilation rates
example, SF6 or N2O) using an analyzer based
were compared using numerical simulations with an
either on gas chromatography or infrared tech-
indoor air quality model.
niques (Sherman 1990).
(b) Calculation of the ventilation from relationships
that are deduced from analytical, empirical, or
semi-empirical models that are based on fundamen- Data
tal equations of fluid dynamics and heat transfer,
such as mass, momentum, energy, and chemical The data employed in the present study were obtained
species conservation equations (Chen 2009). The during the “Urban Aerosol” experimental campaign,
governing equations can be analytically solved and which was carried out during 2002 in three residential
simplifications are employed for the indoor geom- microenvironments (MEs) in the city of Athens, Greece.
etry and the thermo-fluid boundary conditions. Details regarding the Urban Aerosol experimental cam-
(c) Computer-based programs (Zonal, Multizone, and paign can be found in Lazaridis et al. (2001). The
Computational Fluid Dynamics (CFD) models) are aerosol number concentration was obtained at five mi-
extensively used during the last years for the nutes intervals using a scanning mobility particle sizer
Environ Monit Assess (2014) 186:151–163 153

for the fraction between 10 and 550 nm (SMPS, DMA prior knowledge of the SO2 deposition rates is needed;
model 3071 and CPC 3022A, TSI Inc., USA). however, to obtain SO2 deposition rates from the mass
SO2 is commonly monitored in air quality studies balance equation, a limited number of ventilation mea-
considering the fact that it is the predominant anthro- surements are required. This iterative process is de-
pogenic sulfur-containing air pollutant (Seinfeld and scribed more analytically in the following three steps:
Pandis 2006), considered as a classical pollutant
Step a Limited ventilation rates measurements. Initially,
(World Health Organization 2000), even though its
limited measurements of the ventilation rate with
concentrations are reduced in the last years and low
the SF6 decay method were conducted.
levels are currently observed (Vrekoussis et al. 2013).
Step b SO2 deposition rates calculation. An average
In particular, it was selected for the needs of the present
value for the SO2 deposition rates was calcu-
study because its indoor homogeneous chemistry is not
lated, taking into account the ventilation rates
as intense as of other pollutants usually measured in the
that were measured with the SF6 method. The
indoor environment (e.g., nitrogen oxides and ozone);
proposed methodology is based on the analyt-
thus, even if it cannot be considered as an inert gas (as,
ical solution of the well known mass-balance
for example, SF6) it is nevertheless appropriate for
equation for the SO2 concentrations, as de-
simple indoor air calculations.
scribed below, provided that the indoor and
SO2 concentrations were measured using an APSA
outdoor SO2 concentrations are known. When
360A Horiba Analyzer, which was interfaced to a
the ventilation rate is known (from SF6 mea-
Campbell CR10-X model data logger. Sampling of
surements), the SO2 deposition rate is obtained
indoor and outdoor air was performed on a 15-min
from the solution of Eq. (3), as explained in
cycle from separate inlets for gases and aerosols. In
Appendix 1. The solution can be summarized
each ME, a number of measurements of the ventilation
as follows:
rate were performed by means of the tracer gas (SF6)

decay method. Differential pressure between the in- λðC 0 − C i Þ− ΔCi Δt
doors and outdoors was measured with a Setra 264 kτ ¼
differential pressure transducer. In addition, data of Ci
indoor and outdoor air temperature and relative humid- where C i and C 0 are the mean indoor and
ity, as well as wind speed and direction in the outdoor outdoor SO2 concentration during the time in-
environments were collected with instruments placed 
terval Δt, ΔCi Δt the slope of the linear regres-
indoors and outdoors. The data are analytically
sion of the indoor concentrations versus time, λ
presented in Halios et al. (2009).
the ventilation rate (in hours), kτ the deposition
rate (in hours).
In addition, the uncertainties involved in the
Methodology
calculation of the SO2 deposition rates were esti-
mated as analytically presented in Appendix 2.
The methodology for the determination of the ventila-
Step c Ventilation rates calculation. The resulting SO2
tion rates consists of a three-step iterative process.
deposition rates were employed along with the
Uncertainties involved in the calculations are estimated
other measured values (average indoor and out-
in Appendix 2 and at the end of the “Results and
door SO2 concentrations) and the ventilation
discussion.” The evaluation of the method and its
rate for each hour of the experimental campaign
application for the calculation of the particles loss rates
was calculated according to the relationship
is accomplished in three additional steps
 
k τ C i − ΔCi
Proposed method for ventilation rates λ ¼   Δt
C0− Ci

The proposed method is based on the solution of the


mass balance equation for SO2 concentrations which is Uncertainties induced in the ventilation rates
analytically described in Appendix 1. To apply this calculation are also analytically presented in
method for the determination of the ventilation rates, Appendix 2.
154 Environ Monit Assess (2014) 186:151–163

Evaluation and application of the method decay method and the results are presented in Table 1.
SO2 deposition rates, along with the respective uncer-
Ventilation rates were also calculated using available tainties were calculated (based on the methodology
indoor–outdoor pressure difference measurements, and presented in step b of the “Methodology”), are presented
they are compared against ventilation rates obtained in Table 2. For the needs of the calculations, the ventila-
with the new method (step d). Then both ventilation tion rates are shown in Table 1. It is of interest to note that
rates (obtained from steps (c) and (d)) were used to the deposition rates are different in the different MEs
calculate the particle indoor deposition rates (step e). apparently because of the different characteristics of the
Finally, ventilation and deposition values were set as MEs. The calculated deposition rates are in accordance
input to a mass-balance model to assess differences with the deposition rates that were found by Grontoft and
(step f). More specifically: Raychaudhuri (2004). The SO2 deposition rates at the
three MEs were calculated with a different method based
Step d Ventilation from pressure difference measure-
on the linear regression between the indoor and outdoor
ments. The ventilation rates were calculated
SO2 concentrations (Halios et al. 2009) and were found
with an alternative method, which is based on
to range between 3 and 4.7 h for ME1, 3 and 5.6 h for
the differential pressure measurements and were
ME2, and 1 and 2 h for ME3, respectively. These values
compared against the ventilation rates found in
are close to the deposition rates found here, with an
step c. The calculation of the ventilation rates
apparent exception for ME2. It should be noted though
based on the differential pressure measurements
that for this ME, there is only one measurement of the
is analytically presented in Appendix 3, along
ventilation rate and thus one deposition rate measure-
with the error induced in the calculations.
ment. The calculations of the SO2 deposition rates
Step e Particles deposition rates. The calculated ventila-
presented here are concerning hourly values, whereas
tion rates were employed to calculate the loss
the SO2 deposition rates that were calculated by Halios
rates of particle concentrations that were mea-
et al. (2009) were averages corresponding to the total
sured during the same experimental period. The
experimental period.
determination of the particles loss rate was based
on the methodology described by Smolik et al.
Ventilation rates
(2005) and is presented in Appendix 4.
Step f Model applications. Numerical simulations were
For the ventilation rate calculations in each ME with the
conducted with the use of the Multi-Chamber
new method (presented in step c of the “Methodology”),
Indoor Air Quality Model MIAQ (Nazaroff and
the average value of the deposition rates presented in
Cass 1986). Different simulations corresponding
Table 2 was employed. Figure 1 shows an illustrative
to the input values obtained from the new method
example presenting the time evolution of the hourly
(steps (c) and (e)) and the pressure difference
ventilation rates that were calculated with the new meth-
measurements (steps (d) and (e)) were conducted.
od during 24 h (13–14 Mar 2002) at ME1 is provided.
The results of the different numerical simulations
Ventilation rates estimated from differential pressure
were compared with the measured indoor particle
measurements are also presented. It can be seen that
number concentrations to assess the relative ac-
the ventilation rates calculated with the new method,
curacy of the different calculated ventilation
present intense variability not observed for the ventila-
rates.
tion rates that were calculated with the differential pres-
sure. The cumulative frequency distribution of the ven-
tilation rates that were calculated with the new method
Results and discussion
Table 1 Ventilation rate measurements with the SF6 decay method
SO2 deposition rates
ME1 ME2 ME3
To apply the methodology proposed here, the SO2 depo- λ1 (h-1) 1 0.5 0.3
sition rates indoors should be available. The ventilation λ2 (h-1) 1.1 0.5
rates that were measured by means of the tracer gas (SF6)
Environ Monit Assess (2014) 186:151–163 155

Table 2 Calculared deposition rates and related uncertainties for ME2 77 % of the λ−δλ values were lower than 0.6 h
ME1 ME2 ME3 and 80 % of the λ+δλ values were lower than 1 h.
From the analysis presented above, it is apparent
kτ1 (h-1) 2,71 1,72 1,11 that there are significant discrepancies between the
δkτ1 (h-1) 0,068 0,008 0,06 ventilation rates estimated with the two methods. In
kτ2 (h-1) 3,57 0,37 general, higher ventilation rates are obtained with the
δkτ2 (h-1) 1,17 0,01 new method and lower ones with the differential pres-
sure method. Kolmogorov–Smirnov tests showed that
there are statistically significant differences between
in all three MEs are presented in Figs. 2a, 3a, and 4. For the hourly ventilation rates calculated with the two
ME1, the ventilation rates were calculated to be between methods (steps c and d of the “Methodology”). For
0.6 and 3.4 h, whereas 80 % of the calculated values ME1, the maximum difference is 0.49 at 0.001 p-level
were lower than 2 h. The respective error values were whereas for ME2 the maximum difference is 0.52 at
found to range between 0.4 and 2.4 h−1 (λ−δλ) and 1 0.001 p-level. Further comparison between the two
and 5 h (λ+δλ). methods is presented at the model application method.
The average ventilation rates were found to range
between 0.2 and 3.2 h for ME2 and between 0.2 and Particle loss rates
3.4 h for ME3. For the corresponding errors in ΜΕ2, it
was found that 70 % was lower than 0.4 h (λ−δλ) and For the calculation of the deposition rates, the method-
75 % lower than 0.6 h (λ+δλ), whereas in ME3 it was ology presented in step e of the “Methodology” was
found that 83 % was lower than 0.4 h (λ−δλ) and 83 % employed. The particle concentrations data and the
lower than 2 h (λ+δλ). calculated ventilation rates for the time period from
The ventilation rates that were calculated with the 15 Mar 2002 at 22:00 to 16 Mar 2002 at 3:00 were
differential pressure measurements (step d of the used. The particle loss rates for ME1are as follows: kτ′
“Methodology”) are presented in Figs. 2b and 3b for (1)=0.50±0.28 h employing the ventilation rate that
MEs 1 and 2, respectively. For the ME3, the ventilation was calculated from the new methodology (step c),
rates were not calculated due to malfunctioning of the and kτ′ (2)=1.7±0.12 h employing the ventilation rate
differential pressure monitor. The hourly average that was calculated from the differential pressure (step
values were found to range between 0.2 and 1.8 h for d). The deposition rates for the particle number con-
ME1 and between 0.1 and 1 h for ME2. For the error centrations which are based on the ventilation rates that
values in ME1, it was found that 74 % were lower than were calculated with the new methodology are within
0.3 h (λ−δλ) and 70 % lower than 2 h (λ+δλ), whereas the range of values (0.2–2 h) summarized by He et al.

Fig. 1 An example of the 6


time evolution of the venti- -
lation rates calculated with
the new method (λ) and with 5 + ( P)
the differential pressure in ( P)+ ( P) ( P)- ( P)
ME1. In the same figure, the
4
calculated uncertainties of
the ventilation rates are
ACH (h )
-1

presented (δλ and δλ (P)) 3

0
13/3/02 21:00 14/3/02 3:00 14/3/02 9:00 14/3/02 15:00 14/3/02 21:00
Time
156 Environ Monit Assess (2014) 186:151–163

100 100
a 90
b
90

Cumulative Frequency Distribution (%)


Cumulative Frequency Distribution (%)
80 80

70 70
P
60 60
- P -
50 + 50 P +

40 40

30 30

20 20

10 10

0 0
0 2 4 6 0 2 4 6
Ventilation Rates (h-1) Ventilation Rates (h-1)

Fig. 2 Cumulative frequency distribution of the hourly ventilation rates (λ) along with the respective uncertainties (λ−δλ, λ+δλ)
calculated with the new method (a) and from the differential pressure measurements (b) in ME1

(2005) and have an average value of 0.5 h. The depo- were conducted with respect to the number of airborne
sition rates that are calculated considering the ventila- particles that were monitored in ME1 during the time
tion rates obtained from the differential pressure mea- period 13 Mar 2002 at 21:00–14 Mar 2002 at 21:00.
surements are significantly higher from the values re- The input values which were used during the numerical
ported by He et al. (2005). experiments were as follows: (1) the measured outdoor
particle number concentrations for each hour, (2) the
Model applications measured indoor particle number concentrations during
the first hour, (3) the ventilation rates calculated with the
To compare the ventilation rates obtained with the two two methods presented in ventilation rates paragraph of
methods, numerical simulations with the well-known this section, and (4) the particle deposition rates as
Multi-Chamber Indoor Air Quality Model (Nazaroff and presented in particle loss rates paragraph of this section.
Cass 1989) were performed. The numerical simulations The model takes into account the ventilation, deposition

100 100
a 90
b
90
Cumulative Frequency Distribution (%)

Cumulative Frequency Distribution (%)

80 80
P
70 - 70 P -
+ P +
60 60

50 50

40 40

30 30

20 20

10 10

0 0
0 1 2 3 4 0 1 2 3
Ventilation Rates (h-1) Ventilation Rates (h-1)

Fig. 3 Cumulative frequency distribution of the hourly ventilation rates (λ) along with the respective uncertainties (λ−δλ, λ+δλ)
calculated with the new method (a) and from the differential pressure measurements (b) in ME2
Environ Monit Assess (2014) 186:151–163 157
100
were calculated with the new method, showed fair
90
Cumulative Frequency Distribution (%) agreement with the measured concentrations. The de-
80 viations between the model-predicted concentrations
70 obtained from the average λ(1) and k τ (1) values from
the new method and the measured ones were about
60
12 %. Conversely, the model-predicted indoor concen-
50 trations, which were obtained considering deposition
-
40 + k τ (ΔP) and ventilation rates λ(ΔP) that were calcu-
30
lated with the differential pressure measurements are
underestimates of the measured concentrations (aver-
20
age deviation higher than 45 %). These discrepancies
10 can be attributed to the enhanced deposition values that
0 were calculated. It is apparent that the model perfor-
0 2 4 6 8
mance when the deposition and ventilation rates which
Ventilation Rates (h-1)
were calculated with the new method is significantly
Fig. 4 Cumulative frequency distribution of the hourly ventila- improved.
tion rates (λ) along with the respective uncertainties (λ−δλ,
λ+δλ) calculated with the new method in ME3
Limitations and further improvements

and coagulation of the particles (Nazaroff and Cass 1989). It is of significance to stress that the methodology
For the selected time period, six numerical experiments presented here is based on some underlying basic as-
were conducted, each one corresponding: (1) to the aver- sumptions, not always met in real-world studies, which
age ventilation rates calculated with the new method are summarized in the following: (a) uniform indoor
(λ (1)) and the corresponding loss rates (k τ (1)), (2) to mixing. To assess the fraction of the pollutant mass that
the overestimation of the predicted concentrations due to is completely mixed with room air, the mixing factor
uncertainties induced in the calculation of the ventilation (k) is usually used, with values ranging between 0.3
and loss rate (λ (1) + δλ (1), k τ (1)−δk τ (1)), (3) to the and 1, with k equals to 1 for completely mixed spaces.
underestimation of the predicted concentrations due In large rooms, the mixing factor may be lower than 0.3
to uncertainties induced in the calculation of the ven- and significantly vary (Chaloulakou and Mavroidis
tilation and loss rate (λ (1) – δλ (1), k τ (1) + δk τ (1)), 2002). In addition, under strong indoor sources such
(4) to the average ventilation rates calculated with the as cigarette burning mixing depends on the ventilation
differential pressure measurements (λ (ΔP)) and the cor- rate and the flow field in the room (Baughman et al.
responding loss rates (kτ(ΔP)), (5) to the respective under 1994; Gadgil et al. 2003). It is a common assumption
(λ (ΔP) − δλ (ΔP) and k τ (ΔP) + δk τ (ΔP)), and (6) over- though that for small indoor environments and with no
estimations (λ (ΔP) + δλ (ΔP), k τ (ΔP) − δk τ (ΔP)). indoor sources, pollutants are relatively uniformly
The particle number concentrations obtained from mixed. (b) Apart from deposition and transport be-
model simulations with ventilation rates that were cal- tween indoors and outdoors, no other SO2 transforma-
culated with the new method for the time period 13 tions (e.g., homogeneous chemical reactions) takes
Mar 2002 at 21:00–14 Mar 2002 at 21:00 are presented place in the indoor environment and (c) no other aero-
in Fig. 5a, whereas in Fig. 5b the corresponding con- sol transformations apart from deposition, transport
centrations obtained from model simulations with ven- between indoors and outdoors and coagulation take
tilation rates calculated from the differential pressure place. Changes due to other particle dynamics, i.e.,
measurements are presented. In these figures, underes- condensation, evaporation, and/or other processes are
timations and overestimations of the indoor concentra- assumed to be negligible (Hussein et al. 2006). (d)
tions due to the uncertainties in the calculations of the Ventilation rates are constant during the time periods
ventilation and loss rates are presented, along with the considered. (e) SO2 and aerosol deposition rates are
measured indoor particle number concentrations. In assumed to be spatially and temporally constant.
general, the model-predicted indoor concentrations, Actually, deposition is a dynamic parameter which
which were obtained considering ventilation rates that presents temporal and spatial variation and is sensitive
158 Environ Monit Assess (2014) 186:151–163
6.0E+04

a
5.0E+04
Concentration (# cm )

4.0E+04
-3

3.0E+04

2.0E+04

1.0E+04

0.0E+00
13/3/2002 21:00 14/3/2002 1:00 14/3/2002 5:00 14/3/2002 9:00 14/3/2002 13:00 14/3/2002 17:00 Time

measur Cin(λ(1)+δλ , kτ(1)-δkτ(1)) Cin(λ(1)-δλ , kτ(1)+δkτ(1)) Cin(λ1,kτ(1)) Outdoor

6.E+04

b
5.E+04

4.E+04
Concentration (# cm )
-3

3.E+04

2.E+04

1.E+04

0.E+00
13/3/2002 21:00 14/3/2002 1:00 14/3/2002 5:00 14/3/2002 9:00 14/3/2002 13:00 14/3/2002 17:00 Time

measur Cin(λ(ΔP)+δλ(ΔP) , kτ(ΔP)-δkτ(ΔP))


Cin(λ(ΔP)-δλ(ΔP) , kτ(ΔP)+δkτ(ΔP)) Cin(λ(ΔP) , kτ(ΔP))
Outdoor

Fig. 5 a Particle number concentrations obtained from experi- number concentrations obtained from experimental measurements
mental measurements and model simulations with ventilation rates and model simulations with ventilation rates that were calculated
that were calculated with the new method for the time period 13 with the pressure difference for the time period 13 Mar 2002 at
Mar 2002 at 21:00–14 Mar 2002 at 21:00. The line with circles 21:00–14 Mar 2002 at 21:00. The line with circles corresponds to
corresponds to indoor concentrations that were obtained during indoor concentrations that were obtained during simulations where
simulations where the average values of the ventilation and loss the average values of the ventilation and loss rates were consid-
rates were considered. The line with squares corresponds to over- ered. The line with squares corresponds to overestimations due to
estimations because of the uncertainties in the calculations of the the uncertainties in the calculations of the ventilation and loss
ventilation and loss rates, whereas the line with triangles corre- rates, whereas the line with triangles corresponds to underestima-
sponds to underestimations for the same reasons. b Particle tions for the same reasons

to ventilation rates (Morrison and Wiseman 2005) and ultrafine particles (Rim and Koutrakis 2010; Chen and
spatial pollutants distribution (Zhao and Wu 2007); Zhao 2011). Here for reasons of simplicity, we consid-
thus, fluctuations to the deposition process should be er that the penetration factor is 1 and deviations should
expected. (g) Particle penetration factor is the fraction be expected as the datasets include particle with diam-
of particles of a specific diameter that pass through the eters that range between 10 and 550 nm. If size-
building shell along with infiltrating air (Chen and resolved particle concentrations are available, the pen-
Zhao 2011). In several studies, it has been found to etration factor could be also estimated. (h) The surface
vary with particle size, higher values correlated with to volume ratio might significantly deviate from the
Environ Monit Assess (2014) 186:151–163 159

values estimated here because of the different architec- measured values. Satisfactory agreement between the mea-
tures and indoor furnishings (e.g., Knutson et al. 1992). sured and model concentrations was observed with devia-
In cases when there is not even a limited number of tions smaller than 12 %. When the ventilation and deposi-
direct ventilation measurements available, the method de- tion rates calculated from differential pressure measure-
scribed here could be significantly simplified if the SO2 ments were set as input to the model, the comparison
deposition rates are not calculated (steps a and b of the between the measurements and model predicted concen-
“Methodology”) but instead representative values are taken trations was poor (as high as 45 %). The model perfor-
from the literature (e.g., Grontoft and Raychaudhuri 2004). mance is significantly improved when deposition and ven-
Then the ventilation rates could be directly calculated from tilation rates calculated with the proposed method were
step c of the “Methodology,” and the relevant uncertainty employed.
could be estimated from the range of SO2 deposition rates.
In this study, we used SO2 measurements; however, Acknowledgments The authors would like to thank Prof. Ian
Colbeck. The measurements which were used for this study were
the method could also be performed by using other
conducted in the frame of the European project “Urban Aerosol.”
routinely measured indoor gases which are relatively inert
or not chemically active (e.g., carbon monoxide), provid-
ed that the conditions described here would be fulfilled.
Appendix 1. Calculation of the ventilation and SO2
deposition rates
Conclusions
The mass balance equation is given as follows:

In this study, a method for the continuous calculation dC i
dt
¼λPC 0 −λC i −k τ C i ð1Þ
of the ventilation rate based on routine indoor air
measurements was introduced. The method consists where Ci is the indoor concentration (in micrograms per
of a three-step process, which is based on analytical cubic meter), C0 the outdoor concentration (in micro-
solution of the mass-balance equation for the concen- grams per cubuc meter), λ the ventilation rate (in hours),
trations of key pollutants such as SO2. k τ the deposition rate (in hours), t is the time (in hours),
The method was applied to three indoor MEs with and P is the penetration factor (dimensionless).
different characteristics. The hourly average ventilation By integrating Eq. (1) and if we set P=1 (see “Results
rates were calculated to range between 0.6 and 3.4 h for and discussion” for a discussion about this assumption),
ME1, 0.2 and 3.2 h for ME2, and 0.2 and 3.4 h for ME3, one gets:
with median values of 1.36, 0.34, and 0.79 for ME1, ME2,
and ME3, respectively. Results obtained from the new Zt2 Zt2 Zt2 Zt2
dC i
method were compared against ventilation rates calculated dt¼ λC 0 dt− λC i dt− k τ C i dt
dt
from concurrent differential pressure measurements, and t1 t1 t1 t1
statistically significant differences were found. Ventilation By assuming that λ=constant for the time period from
rates calculated with the later method were in general t1 to t2
lower than the ventilation rates estimated from the former.
Particle loss rate due to the coagulation and deposition ZC2 Zt2 Zt2 Zt2
was calculated in one ME, using the ventilation rates dC i ¼λ oC dt − λ C i dt −k τ C i dt ð2Þ
found from the new method as well as the method based C1 t1 t1 t1
on the differential pressure measurements. Particle loss
rate calculated with ventilation rates from the former By definition
method was 0.50 h, in accordance with the loss rates Z
1
found in literature, whereas higher loss rates were found Co ¼ C o ðt Þ dt
Δt
when the ventilation rates calculated from the differential
pressure method was used. and
The proposed method was indirectly evaluated by ap- Z
plying a mass balance numerical model and. predicted 1
Ci ¼ C i ðt Þ dt
concentrations were compared against experimentally Δt
160 Environ Monit Assess (2014) 186:151–163

Thus from Eq. (2) one gets k τ C i − ΔCi


λ¼  Δt ð4Þ
ZC 2 C0 − Ci
dC i ¼ λΔtC 0 −λΔtC i −k τ ΔtC i ⇔
and the determination of the ventilation rate is possible.
C1
Conversely, when the ventilation rate is known, the
SO2 deposition rate is obtained from the solution of
Eq. (3):
    
ΔC i λ C 0 −C i − ΔCi Δt
¼λ C 0 −C i −k τ C i ð3Þ
Δt kτ ¼ ð5Þ
Ci
C i and C 0 are the average values of the indoor and
outdoor SO2 concentration during the time interval Δt,

and ΔCi Δt the slope of the linear regression of the Appendix 2. Calculation of the uncertainties
indoor concentrations versus time. It should be noticed involved in the calculation of deposition
that the Δt=1 h. During this time interval, λ=constant. and ventilation rates
When indoor and outdoor SO2 measurements are
available, the solution of the mass balance equation Uncertainties induced into the deposition and ventila-
leads to Eq. (3) which has two unknown parameters: tion calculations were determined with the error prop-
the ventilation rate λ and the deposition rate kτ. If the agation method. The error propagation method for the
SO2 deposition rate kτ is known, then from Eq. (3) one determination of the deposition rates as expressed by
obtains: Eq. (5) provides:

vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
!2 !2 !2
u 
u ∂k ∂k τ ∂k τ ΔC i
δk τ ¼ t τ
δC i þ δC 0 þ  δ ð6Þ
∂C i ∂C 0 ∂ ΔC Δt
i Δt

The partial derivatives can be calculated as follows:

0 1
2   ΔC 3 ΔC i ΔC i ΔC i
∂ 6 λ C 0 −C i − Δt 7 ∂ B C −λC 0
i
∂k τ B C0 Δt C C0 Δt Δt
¼ 4 5¼ Bλ −λ− C ¼ −λ 2 þ ¼ ð7Þ
∂C i @ C i Ci A
2 2
∂C i ∂C i Ci Ci Ci Ci

0 1
ΔC i calculated to be:
∂k τ ∂ B B C0
C
Δt C λ
¼ Bλ −λ− C¼ ð8Þ
∂C 0 ∂C 0 @ Ci Ci A Ci

vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
u0 12 !2 !2 
u ΔCi
u = −λC 2
 ! δk τ ¼t@ Δt 0 A δC i 2 þ λ δC 0 2 þ 1 δ ΔC i
∂k ∂ C0
ΔC i
1
2
Ci Ci Δt
Ci
 τ ¼  λ −λ− Δt
¼− ð9Þ
ΔC i ΔC i Ci Ci Ci ð10Þ
∂ ∂
Δt Δt
Correspondingly the error propagation method for
After substituting Eqs. (6), (7), and (8) to Eq. (5), the the determination of the ventilation rates (shown in
resulting uncertainty for the deposition rates was Eq. (4)) provides:
Environ Monit Assess (2014) 186:151–163 161

vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
!2 !2 !2ffi
u
u ∂λ 2
∂λ ∂λ ∂λ ΔC
δλ¼t
i
δk τ þ δC i þ δC 0 þ ΔC i
δ ð11Þ
∂k τ ∂C i ∂C 0 ∂ Δt
Δt

with
∂λ Ci
¼ ð12Þ
∂k τ C −C
0 i
!  !
∂λ ∂ k τ Ci ∂
ΔC i
∂  −1 ΔC i ∂  −1
Δt
¼ þ ¼k τ C i C 0 −C i þ C 0 −C i ¼
∂C i ∂C i C 0 −C i ∂C i C 0 −C i ∂Ci Δt ∂C
i
 −1  −2 ΔC  −2
i
¼k τ C 0 −C i þk τ C i C 0 −C i þ C 0 −C i ¼
Δt
 
kτ ΔC i
k τ Ci 1 k τ C 0 −k τ C i þk τ C i þΔCi Δt
k τ C 0 þΔCi Δt
¼ þ 2 þ  2 ¼  2 ¼  2 ð13Þ
C 0 −C i Δt
C 0 −C i C 0 −C i C 0 −C i C 0 −C i

and after substituting Eqs. (12), (13), (14), and (15) to


(11), the resulting uncertainty for the ventilation rates is:

∂λ k τ C i þΔC Δt
¼−  2 ð14Þ
∂C 0 C 0 −C i

∂λ 1
¼ ð15Þ
ΔC i C −C
∂ 0 i
Δt

vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
0 12 0 12
u !2 !2
u
u C B τ 0k C þ ΔC i =
C B τ i k C þ ΔC =
C 1 ΔC i
u
δλ¼t
i
δk τ þ@  Δt Δt
2 δC i A þ@  2 δC 0 A þ δ
C 0 −C i C 0 −C i C 0 −C i C 0 −C i Δt (16)

Appendix 3. Ventilation rates from differential where ΔP is differential pressure, C the flow coeffi-
pressure measurements cient (m3 s−1 Pa−n) related to the size of the crack, while
n is the flow exponent which characterizes the flow
Airflow through cracks and air leakages across the regime. n values range between 0.5 for fully turbulent
building shell is frequently represented by a power flow and 1.0 for fully laminar flow.
law equation (Orme et al. 1994): According to Walker et al. (1998), it can be assumed
that the air enters through a series of a number (k) of
Q ¼ C  ΔPn ð17Þ cracks, which are arranged in a parallel order. The
162 Environ Monit Assess (2014) 186:151–163

pressure differences between the indoor and the out- For the calculations, the values of the flow coeffi-
door environment for each of the k cracks are equal: cients were taken from the work of Orme et al. 1994.
Uncertainties induced into the ventilation calcula-
ΔP1 ¼ ΔP2 ¼ … ¼ ΔPk ð18Þ
tions were determined with the error propagation meth-
Thus, the total flow is expressed as: od. The resulting uncertainty for the ventilation rates
was calculated to be:
Q ¼ Q1 þ Q2 þ ::: þ Qk ð19Þ

ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
s
  n−1 2  n 2  n 2  n 2
dQ¼ C 1 þC 2 þ:::þC k n  ΔP  dP þ ΔP dC 1 þ ΔP dC 2 þ:::þ ΔP dC k þ
rffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
h    iffi
n
þ C 1 þC 2 þ:::þC k ΔP þln ΔP dn ð20Þ

sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
  ffi
Then the ventilation rate λ can be obtained from the 2 2
0 dκτ dκτ 0
airflow Q from the equation: δκ τ ¼ δa þ δλ ⇒δκ τ
da dλ
. qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
λ¼Q V ð21Þ
¼ ðδaÞ2 þ ðδλÞ2 ð24Þ

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