Article

pubs.acs.org/est

Improving the Accuracy of Daily PM2.5 Distributions Derived from the

Fusion of Ground-Level Measurements with Aerosol Optical Depth
Observations, a Case Study in North China
Baolei Lv,†,‡ Yongtao Hu,§ Howard H. Chang,⊥ Armistead G. Russell,*,§ and Yuqi Bai*,†,‡
†
The Ministry of Education Key Laboratory for Earth System Modeling, Center for Earth System Science, Tsinghua University,
Beijing 100084, China
‡
Joint Center for Global Change Studies, Beijing 100875, China
§
School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
⊥
Department of Biostatistics and Bioinformatics, Emory University, Atlanta, Georgia 30322, United States
*
S Supporting Information

ABSTRACT: The accuracy in estimated fine particulate

matter concentrations (PM2.5), obtained by fusing of station-
based measurements and satellite-based aerosol optical depth
(AOD), is often reduced without accounting for the spatial
and temporal variations in PM 2.5 and missing AOD
observations. In this study, a city-specific linear regression
model was first developed to fill in missing AOD data. A novel
interpolation-based variable, PM2.5 spatial interpolator
(PMSI2.5), was also introduced to account for the spatial
dependence in PM2.5 across grid cells. A Bayesian hierarchical
model was then developed to estimate spatiotemporal
relationships between AOD and PM2.5. These methods were
evaluated through a city-specific 10-fold cross-validation
procedure in a case study in North China in 2014. The cross validation R2 was 0.61 when PMSI2.5 was included and 0.48
when PMSI2.5 was excluded. The gap-filled AOD values also effectively improved predicted PM2.5 concentrations with an R2 =
0.78. Daily ground-level PM2.5 concentration fields at a 12 km resolution were predicted with complete spatial and temporal
coverage. This study also indicates that model prediction performance should be assessed by accounting for monitor clustering
due to the potential misinterpretation of model accuracy in spatial prediction when validation monitors are randomly selected.

■ INTRODUCTION
Fine particulate matter, a complex mixture of particles with
aerodynamic diameters of 2.5 μm or less (PM2.5), has been a
major component of the severe air pollution levels experienced
in many cities in China in recent years. PM2.5 is the dominant
pollutant of concern, especially during the winter.1−3 Since
PM2.5 can efficiently penetrate into human lungs and bronchi,4,5
long-term and short-term exposures to PM2.5 can increase
premature mortality and morbidity.5
One major limitation with ground-level measurements of
PM2.5 is the sparse spatial coverage of monitoring networks.
Alternatively, satellite-based aerosol optical depth (AOD)
observations have been used to estimate continuous spatial
and temporal patterns of ground PM2.5 concentrations.6−8
Optical properties of atmospheric aerosols are sensitive to the
optical properties of the particles that make up particulate
matters, including size and composition. A large fraction of the
particles that make up PM2.5 particle mass scatter sunlight,
leading to a strong association between the mass of PM2.5 and
observed AOD.9,10 All else being equal, as the number (and
mass) of particles increases, light scattering increases, leading to
an increase in AOD. While the association between PM2.5 and
AOD is typically strong, the relationship can change due to
changes in the particle size distribution, particle composition,
mixing height, humidity, and other factors.
Early studies used various linear regression modeling
techniques to estimate PM2.5 concentrations using AOD as
well as other spatial and spatial-temporal predictors, such as
land cover, elevation, meteorological parameters, and indicators
for holidays.10,11 More complex models were then developed,
including the linear mixed effect (LME) model,12,13 geo-
graphically weighted regression (GWR) model,14,15 remote
sensing formula,16 semisupervised learning approach based on
multiple factors,17 and complex ensemble models.18 Atmos-
pheric chemistry models were also used to determine the
relationships between AOD and PM2.5.8,19 Among all these
studies, treating the linear slopes and intercepts between AOD
Received: December 10, 2015
Revised: March 23, 2016
Accepted: April 4, 2016
Published: April 4, 2016

© 2016 American Chemical Society 4752 DOI: 10.1021/acs.est.5b05940

Environ. Sci. Technol. 2016, 50, 4752−4759
Environmental Science & Technology
Figure 1. Study area and the locations of PM2.5 monitoring stations as shown by points. The right panel depicts the average satellite-based AOD
values in 2014.
and PM2.5 at different locations and at different time points as
spatially and temporally correlated random effects has been
shown to be promising in a study conducted in the southeast
United States.20 However, to our knowledge, such a statistical
model structure has not been previously applied in China.
AOD data derived from instruments aboard satellites, such as
the moderate resolution imaging spectroradiometer (MODIS),
are often missing due to clouds, high surface albedos21 (e.g.,
snow and ice), and potentially, very high PM2.5 pollutant
levels.22,23 If the missing AOD values are related to high PM2.5
pollution levels, the average PM2.5 concentrations estimated
using only the retrieved AOD fields can be underestimated.
Several attempts have been made to solve this issue. Kloog et al.
filled in missing AOD values by smoothing the mean PM2.5
levels across the study area.24,25 Van Donkelaar et al. used the
sampling bias correction factor method.7,26 Their calculations
were usually month or year specific,19,27 such that the bias
could not be effectively corrected when calculating the mean in
a small number of days. Just et al. predicted PM2.5 levels within
the grid cells with missing AOD by using PM2.5 levels in the
neighboring grid cells, based on season-specific spatial
patterns.28 Ma et al. used ordinary Kriging to interpolate the
available retrieved AOD values.14 However, their method could
have significant uncertainties if only a limited number of AOD
values were present.29
In this study, we applied the Bayesian model proposed by
Chang et al.20 in North China to estimate the spatially and
temporally varied coefficients in a linear regression setting. We
also considered using spatially interpolated PM2.5 concen-
trations as a predictor and filled the missing AOD values with
novel methods. The rest of the paper is organized as follows.
The study area, data, statistical model, and missing AOD gap-
filling method are introduced in the Materials and Methods.
Model estimation, performance evaluation, and PM2.5 pre-
diction results are presented in the Results and Discussion.
■ MATERIALS AND METHODS
Study Area. Figure 1 shows the North China study area.
This region includes five provincial administrative divisions:
Shandong, Hebei, Liaoning, Beijing and Tianjin. Economic
development in this region is highly dependent on heavy
industries, such as iron and steel factories and cement
production, that are typical sources for emissions of PM2.5
and its precursors.30 Increasing vehicular population and
electricity demand also worsen the air quality in this region.31
The annual mean PM2.5 concentrations in this region was 93
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μg/m 3 in 2014, about nine times the World Health
Organization (WHO) recommended standard of 10 μg/m3.
Long-term exposure to such heavily polluted air is a major
concern for more than 250 million people in this area.32,33
Many atmospheric chemistry modeling applications in this
region, such as the use of the Community Multiscale Air
Quality model (CMAQ), have been run at a 12 × 12 km grid
resolution on a Lambert Conformal Conic map projection.
Therefore, the same grid was chosen in this study to enable the
comparison of and fusion with atmospheric chemistry model
output in future studies. The whole area was divided into 6561
grid cells (81 × 81).
Ground-Level PM2.5 Data. Hourly ground-level PM2.5
concentrations were obtained from the China National Urban
Air Quality Real-time Publishing Platform (http://113.108.142.
147:20035/emcpublish/). Calibration and quality control of
the monitors are conducted by the China National Environ-
mental Monitoring Center.34 Two hundred ninety-eight
monitors from 53 cities in the study area are located in 169
grid cells, described in Table S1, Supporting Information (SI).
To facilitate computation in the data fusion process, at each
time point we averaged PM2.5 concentrations from monitors
that are located in a same grid cell. It is worth noting that point
measurements of PM2.5 concentrations were used to represent
the area-average PM2.5 levels over a grid cell. This may cause
potential bias due to a change of support. Specifically, the grid-
average concentrations may not fully reflect the spatial variation
in PM2.5 as captured by multiple monitors within a grid cell.
MODIS AOD Data. MODIS is a sensor on board two of the
U.S. National Aeronautics and Space Administration (NASA)’s
Earth Observation System (EOS) satellites: Terra and Aqua.
The sun-synchronous satellites provide two column aerosol
observations at approximately 10:30 a.m. (Aqua) and 1:30 p.m.
(Terra) local solar times every day. The MODIS AOD values
are constrained between −0.05 and 5.0 to avoid bias introduced
during the retrieval procedure. A detailed description of the
MODIS AOD retrieval procedure is discussed in Remer et al.35
and Levy et al.21 In this study, MODIS AOD Level 2 data in
2014 were obtained from the Level 1 and Atmosphere Archive
and Distribution System (LAADS, https://ladsweb.nascom.
nasa.gov/). The nominal resolution of this data set is 10 × 10
km at nadir. A nearest neighbor approach was utilized to regrid
the data to the 12 × 12 km setting.
MODIS AOD Missing Data Pattern. For each of the 169
grid cells in which at least one ground monitoring station is
available, averaged PM2.5 concentrations were computed among
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Environmental Science & Technology
Figure 2. (a) Average PM2.5 concentrations; (b) daily SVVR within the study area.
days when AOD observations were available, among days when
AOD values were missing, and across the whole year of 2014
(plotted, respectively, in black, red, and blue points in Figure
2a). The AOD averages were plotted in an ascending order
based on the mean PM2.5 concentrations in that grid cell. It is
clear that mean PM2.5 concentrations were consistently higher
on days when AOD observation were missing than when AOD
data were present (Figure 2a).
To quantitatively measure the spatial and temporal pattern of
AOD missing values, SVVR (spatial valid value ratio, defined in
SI) and TVVR (temporal valid value ratio, defined in SI) were
used. Daily SVVR values, shown in Figure 2b, indicate that
missing AOD was more significant in winter than in other
seasons. The annual TVVR was generally lower among grid
cells in the northwest grassland areas and urban areas (Figure
S1). In winter, the TVVR was quite low (as low as 10%) in
most grid cells, e.g., in heavily polluted south Hebei. Because
the missing AOD values were associated with higher pollution
levels (Figure 2a), negative bias in long-term PM2.5 estimates
will be present if only the retrieved AOD values are used in data
fusion.
MODIS AOD Gap Filling. To overcome the problem of
missing AOD data, we proposed a novel two-step method.
First, a city- and season-specific formula was introduced, based
on a linear assumption of the relationship between PM2.5 and
AOD:10
PMi , j
AODei , j = as AODos , j + bs
PMs , j (1)
AODei,,j refers to the estimated AOD value on day i in grid cell
j. PMi,j refers to the daily mean PM2.5 concentration observed
on day i in grid cell j. AODos,j refers to the average retrieved
AOD values in grid cell j and in season s, where s = 1 denotes
warm season from Apr 16−Oct 15 and s = 2 denotes cold
seasons as the remaining days in a year. PMs,,j refers to the
average PM2.5 concentrations in grid cell j in season s. The
linear relationship was fitted separately in 53 cities. The city-
specific models were then used to predict missing AOD values
in grid cells containing PM2.5 monitors. Second, we combined
the estimated and retrieved AOD values to interpolate missing
AOD values in the other grid cells without PM2.5 monitors
using ordinary Kriging (OK) with exponential covariance
function and obtained a final AOD data set with complete
spatial coverage for each day.
Interpolated Ground PM2.5 Data. We proposed a novel
variable based on the interpolation of PM2.5 observations to be
used in combination with AOD. A spatial interpolation utilizes
the spatial dependence among observations to obtain optimal
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weights for predicting PM2.5 levels at unobserved locations. The
uncertainties (prediction standard errors) of the interpolated
PM2.5 concentration field are not spatially uniform, and the
closer to the monitors a grid cell is, the lower its uncertainty
will be.29 To ensure that the uncertainties of the interpolated
values were generally uniform, a 10-fold leave-10%-cities-out
method was used to generate the interpolated PM2.5 (PMI2.5)
value using the OK method. Specifically, we first randomly
removed the monitors in 10% of 53 cities within the study area.
PMI2.5 values at the removed sites were obtained from kriging
the monitors from the remaining cities. This procedure was
repeated 10 times to obtain interpolated PMI2.5 values at all
monitors.
To further control the uncertainties with the variable PMI2.5,
we defined the final PM2.5 spatial interpolator (PMSI2.5) as
follows
σt PMI 2.5 × f (PMI 2.5)
PMSI 2.5 = PMI 2.5 = PMI 2.5
σ(PMI 2.5) SE(PMI 2.5)
(2)
and
1
f (x) = 10% × x
( α
+1 ) (3)
where σ(PMI2.5) and σt refer to, respectively, the uncertainties
of PMI2.5 and the target uncertainties in that grid cell. The
function f is a continuous inverse proportional function to
constrain the uncertainties of PMI2.5 to be a relatively small
proportion of the original interpolated values (PMI2.5). The
proportion begins with 10% and decreases with increasing
PMI2.5. The parameter α determines rate of decrease. When
PMI2.5 equals α, f is 5%. In this study, α was determined to be
700 based on an optimization between decreasing uncertainties
and decreasing variance information on PMSI2.5 as α increases.
Other Spatiotemporal Predictors. First, we obtained
meteorological data from the NCEP (National Centers for
Environmental Prediction) FNL (Final) Operational Global
Analysis that are on 1° × 1° grids and are prepared
operationally every 6 h. This product is from the Global Data
Assimilation System (GDAS), which continuously collects
observational data from the Global Telecommunications
System (GTS) and other sources. In this study, we used the
parameters of ground temperature (T), relatively humidity
(RH), and planetary boundary height (PBL) at 6:00 UTC
(14:00 Beijing local standard time). The second data source
included land cover and elevation data. Land cover data were
obtained from the MODIS land-cover classification of the
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International Geosphere-Biosphere Program (IGBP) product
in 2010 (http://lpdaac.usgs.gov). The data set was assigned to
the base grid. We used two parameters: green fractions and
urban fractions. Finally, the mean elevation from the USGS
GTOPO30 elevation data set (https://lta.cr.usgs.gov/
GTOPO30) for each grid cell was obtained.
Statistical Model Framework. A linear regression frame-
work was assumed to model the relationships between the
MODIS AOD values and ground PM2.5 measurements20 (eq 4)
PM(s , t ) = α0(s , t ) × AOD + α1(s , t ) + ε(s , t ) (4)
where PM(s,t) denotes the PM2.5 concentrations measured at
location s and time t. Location s is the index of a monitor-
contained grid cell, which is georeferenced as in Figure 1, and
time t is the index of a day within the study period. The
location and time specific slope and intercept are, respectively,
designated as α0(s,t) and α1(s,t). The residual errors ε(s,t) are
assumed to be normally distributed with mean zero and
variance σ2. Model coefficients have both a temporal and
spatially dependent structure.
The coefficients of the linear regression are separated into a
second level
α0(s , t ) = β0(s) + β0(t ) + λ0 Z0 (5)
and
α1(s , t ) = β1(s) + β1(t ) + λ1Ζ1
(6)
where βi(s) and βi(t), respectively, refer to the underlying
model formulation based on out-of-sample prediction. We
designed a workflow (depicted as the Figure S2) to evaluate the
three methods using both 10-fold and spatial cross-validation
experiments. For the 10-fold cross-validation, the data were
randomly divided into 10 groups. For a particular experiment,
nine groups were used to fill the missing AOD values and to fit
two AOD− PM2.5 models (eq 4), with and without the variable
PMSI2.5. The remaining group served as the test data set where
the predicted PM2.5 values were compared to the observed
measurements. The PM2.5 concentrations in the test data set
could be predicted by either the retrieved AOD values or the
filled AOD values. The evaluation was done by withholding a
different group each time for 10 times.
We performed a 10-fold spatial cross-validation by leaving
10% of the cities out each time or 10% of the monitors out each
time. We considered leaving all observations out by cities
instead of by individual monitors to address a weakness that has
been reported in the literature.14,27 Specifically, given the dense
number of monitors in cities, there were typically one or more
monitors near any monitor. Hence, removing individual
monitors one-at-a-time in a cross-validation experiment may
falsely show that the model can perform spatial predictions
well. Results from removing monitors by a group of cities,
however, provide confidence in the model’s ability to predict at
locations far away from monitors.
Model prediction performance was evaluated using the
normalized mean absolute error (NME), root mean square
error (RMSE), R2, and the linear regression coefficients (along
with their standard errors). NME and RMSE are defined in the
SI.

■
independent spatial and temporal processes that determine the
spatiotemporal variations of the slope (for i = 0) and intercept
(for i = 1). The parameter vectors λi represent fixed effects for RESULTS AND DISCUSSION
meteorological, land cover variables: Z0 for the slopes (for i = Model Parameters Estimation. The mean PM2.5 concen-
0) and Z1 for the intercepts (for i = 1). Specifically, eq 5 models trations from monitors for the final data set was 58.8 μg/m3,
the relationships between AOD and PM2.5, with potential which is 1.7 times that of the China Class I standard. On
interactions between AOD and other predictors, and eq 6 average, AOD and PMSI2.5 were significantly associated with
models the underlying processes that have direct effects on the their 95% posterior intervals not including zero (Table 1), with
PM2.5 levels. PMSI2.5 is a predictor variable included in Z1 to
capture addition variation in PM2.5 not explained by AOD and Table 1. Statistical Assessment of the Estimated Coefficients
the other predictors.
terms in λ1 eEstc SEd Low95e Up95f
In this study, we used a tapered conditional Kriging method
to interpolate the spatial coefficients βi(s) in eq 2 for spatial intercept 23.44 18.80 −13.19 60.99
dependence.20 For those days without PM2.5−AOD pairs, we AOD 21.66 3.93 15.34 30.81
used a linear autocorrelation function to model the temporal PMSI2.5 1.16 0.016 1.12 1.19
coefficients βi(t), which specifies that βi(t) is proportional to Green.faca 0.21 0.31 −0.4 0.82
the weighted average between the neighboring days.20 There- Urban.facb 0.64 1.82 −2.97 4.20
fore, we could obtain, with complete coverage, the spatially and elevation −0.012 0.004 −0.02 −0.0044
temporally dependent coefficient fields through interpolating temperature 0.04 0.062 −0.084 0.163
−0.0013 −0.0022 −0.00035
the fitted AOD field. We used the Markov Chain Monte Carlo PBL 0.00047
−0.033 −0.065
(MCMC) method for model fitting under the Bayesian a
RH 0.016 0.000065
framework. One advantage of employing a Bayesian hierarchical Green.fac refers to the fraction of green land in each of the grid cells.
b
framework is that the model could account for uncertainties in Urban.fac refers to the fractions of urban area in each of the grid cells.
c
parameter estimates and PM2.5 predictions. This facilitates the Est denotes the estimated coefficients. dSE denotes the standard
errors of the estimated coefficients. eLow95 denotes the lower bound
model outputs being incorporated in human exposure and of 95% posterior interval. fUp95 denotes the upper bound of 95%
health impact evaluations that considers exposure uncertain- posterior interval.
ties.36,37 It is worth noting that the fitted model can only be
used to predict AOD values within the temporal extent of the
available data, as day-specific AOD−PM2.5 relationships beyond a positive coefficient indicating a positive linear relationship
the time scope (i.e., temporal extrapolation) were not estimated with the PM2.5 levels. The mean uncertainty of the variable
in our model structure. PMSI2.5 was less than 5 μg/m3. Hence, due to the presence of
Model Evaluation Workflow. We evaluated the effective- PMSI2.5, an average uncertainty of approximately 5 μg/m3 was
ness and performance of the AOD gap-filling method, the novel incorporated into the estimations considering its coefficient
variable PMSI2.5 as an additional predictor, and the statistical being close to 1 (Table 1). Both PBL and terrain height were
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Environmental Science & Technology
negatively associated with PM2.5 levels. Regarding the daily
specific random intercepts and slopes (β0(t) and β1(t),
respectively, in eq 5 and eq 6), they are larger in winter
because the PM2.5 concentrations were higher (Figure S3, SI).
Model Comparisons and PMSI2.5 Evaluations. In model
fitting, R2 improved by 0.07 (from 0.66 to 0.73) when the
variable PMSI2.5 was considered in the model. In the 10-fold
leave-10%-cities-out cross validation procedure, the R 2
improved from 0.48 (Figure 3b) to 0.61 (Figure 3c) by a
Figure 3. Model evaluations using the 10-fold leave-10%-cities-out
cross-validation method for the (a) Meteo (Meteorological variables)
+ LU (land use variables) + PMSI2.5 model, (b) AOD + Meteo + LU
model, and (c) full model. Model evaluation using the 10-fold leave-
10%-monitors-out cross-validation method for the full model (d). No
AOD gap-filling was performed in these models.
large margin of 0.13. The RMSE also decreased by 3.46 μg/m3,
from 26.99 μg/m3 to 23.53 μg/m3. In general, the model with
PMSI2.5 predicted PM2.5 more accurately. The variable PMSI2.5
explained more variance of PM2.5 than AOD values by
comparing the model’s performance without using AOD values
and that without PMSI2.5 (Figure 3a). In summary, PMSI2.5
contains additional spatial information PM2.5 that is not
Figure 4. (a) Scatterplots of the AOD values fitted by eq 1 and retrieved AOD values; (b) prediction performance using the reconstructed AOD
with full model; (c) annual average AOD values with gap-filling.
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captured by the spatiotemporal predictors, including AOD.
When using the random leave-10%-monitors-out cross-
validation method, the R2 was 0.68 (Figure 3d), which is
similar to the R2 of 0.69 reported by Zheng et al.27 using the
leave-one-monitor-out validation method but is 0.07 larger than
that using the leave-10%-cities-out cross validation method in
this study. Hence, performing cross-validation at the individual
monitor level could exaggerate the model’s prediction perform-
ance.
The annual PM2.5 levels were calculated by averaging the
estimated PM2.5 concentrations by retrieved AOD values. The
pollution levels in the cities in Hebei province along the foot of
the Taihang Mountains were much higher than those in other
cities. The full model with PMSI2.5 better characterized this
belt-shape pollution zone (Figure S4). Moreover, the full model
with PMSI2.5 predicted the lower pollution levels in the
northern part of study area than the partial model, with lower
prediction standard errors (Figure S4b,d). The standard errors
in the urban area were generally lower due to the greater
density of AOD−PM2.5 pairs.
However, an estimation bias was apparent in the predictions
even by the full model. The annual means of the observed
PM2.5 concentrations in the heavily polluted Hebei cities were
approximately 120 μg/m3. However, the highest estimated
PM2.5 concentrations (full model) were no larger than 100 μg/
m3 (Figure S4c). Spatially, the estimated PM2.5 concentrations
were not smooth, especially in the winter (Figure S5d).
Moreover, the full model using retrieved AOD values failed to
estimate the increased pollution area in the southern Hebei in
the autumn and winter (Figure S5). In all of these cases, the
model predicted PM2.5 concentrations only when AOD values
were available. The observed mean PM2.5 levels with available
AOD values were lower than the annual mean PM2.5 levels
(Figure 2a), which accounts for the underestimations.
AOD Gap-Filling Evaluation. There were approximately
40000 missing AOD values in the grid cells with PM2.5
monitors. Our missing AOD imputation method was effective
at improving PM2.5 predictions. In the model-fitting procedure,
the model overestimated AOD when the retrieved AOD values
were low (Figure 4a). Although the R2 was low (0.36), the
constructed AOD and retrieved AOD showed a good linear
relationship when the retrieved AOD was less than 1.5. By
visually checking the interpolated full AOD data field, we found
that the spatial variations of the AOD values were well
captured. There were almost no abnormal spatial patterns in
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Figure 5. Annual and seasonal mean estimations of the PM2.5 concentrations (μg/m3) using the full model and reconstructed AOD data set.
the daily AOD. When used in predicting PM2.5, the full model
performed well with the reconstructed data set, giving an R2 of
0.78, an NME of 0.27, and an RMSE 33.39 μg/m3 in the cross-
validation experiment (Figure 4b). It is interesting that the
cross-validation performance with the constructed AOD was
better than the model with retrieved AOD. In part, this is
because the linear relationship between AOD and PM2.5
enabled our model to leverage additional extra spatial
information from PM2.5 monitors.
PM2.5 Concentration Estimation. The model using the
“full” AOD data set predicted the seasonal and annual average
of the PM2.5 concentrations well (Figure 5). The PM2.5
concentrations were much higher in winter compared to
those using the retrieved AOD only. The mean PM 2.5
concentration in winter was approached 200 μg/m3. The
heavy pollution mainly occurred in the middle and southern
Hebei province, the western Shandong province, Tianjin, and
Beijing. The PM2.5 levels were also high in the middle of
Liaoning province around Shenyang, its capital city. This area is
part of the Northeast plain, which is traditionally a zone of
heavy industry. The PM2.5 concentrations were generally lower
than 40 μg/m3 in northwest Hebei Province and in the Inner
Mongolia portion within the domain, which is mainly covered
by grassland and forests. It is worth noting that there is a small
area of higher PM2.5 levels in the east of Inner Mongolia and
near Liaoning Province. The area is the location of an industrial
city, Chifeng, which is the second most polluted city in Inner
Mongolia, with an annual mean PM2.5 level of nearly 50 μg/m3.
The successful prediction of this pollution hotspot among clean
surroundings further demonstrated the model’s effectiveness.
The PM2.5 levels were also lower in Shandong and the
Liaodong peninsula and in the middle south of Shandong
Province.
A previous study by Ma et al.14 used the GWR method with
2
R = 0.64 in the 10-fold cross validation method, while we
obtained an R2 = 0.61 by our stricter evaluation process that
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accounts for spatial clustering. They predicted the mean PM2.5
concentrations in southern Hebei province at around 90 μg/m3
in 2013 and 130 μg/m3 in the winter. In contrast, for 2014, we
predicted improved PM2.5 levels to be at around 120 μg/m3
overall and 180 μg/m3 in the winter, which were closer to
observations. Zheng et al.27 evaluated their LME model in
Beijing−Tianjin−Hebei area with an R2 = 0.77 and NME =
0.22 using the more optimiztic leave-one-monitor-out cross
validations method. They did not give estimated seasonal
variations, even though they predicted annual mean PM2.5
concentrations well by using a correction factor. Xie et al.
predicted PM2.5 levels in Beijing, with an R2 = 0.75 in cross-
validation.13 Their performance being better than that in this
study is partially owing to its smaller study area. Without
considering missing AOD values, they significantly under-
estimated annual mean PM2.5 levels. In our study, the data set
with complete spatial coverage could well characterize the
evolution of serious pollution episodes on a regional scale, and
a case pollution episode is presented in the SI (Figure S6).
In summary, our revised model and reconstructed AOD data
set accurately predicts ground PM2.5 concentrations in North
China. First, we used a Bayesian hierarchical framework to
model the daily grid cell-specific linear relationships between
the AOD and PM2.5 concentrations. Second, we used the spatial
dependence in all the observed PM2.5 levels by developing an
interpolated PM2.5 variable PMSI2.5. The new variable PMSI2.5
can significantly improve the model’s prediction performance.
The R2 was improved by 0.13, to 0.61, in the cross-validation
study. Third, we reconstructed the AOD values, and thus, we
obtained daily estimated PM2.5 pollution maps with complete
spatial and temporal coverage, which was shown to be useful
for capturing the evolution of PM2.5 pollution episodes that
occurred in North China.
This study also demonstrates the potential misinterpretation
of model accuracy when a completely random, leave-one (or
10%) cross-validation method is used to evaluate model
DOI: 10.1021/acs.est.5b05940
Environ. Sci. Technol. 2016, 50, 4752−4759
Environmental Science & Technology
prediction performance. In our case, using a completely
random, exhaustive leave-10%-monitors-out procedure led to
an R2, NME, and RMSE of 0.68, 0.26, and 21.40 μg/m3,
respectively. Using a process where monitors were removed
after being grouped by city led to similar performance statistics
of 0.61, 0.28, and 23.53 μg/m3, respectively. In cases where the
air quality monitors are not uniformly distributed (as is almost
always the case because monitors are preferentially located in
cities), the random removal of monitors will typically lead to
having one or more other monitors near the one removed.
Hence, the values to be predicted can often be captured by
measurements from an adjacent monitor that was not removed.
Thus, model prediction performance should be assessed by
accounting for geographical monitor clustering.
■
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acs.est.5b05940.
Variables NME, RMSE, SVVR, and TVVR, Table S1, and
Figures S1−S6 (PDF)
■
AUTHOR INFORMATION
Corresponding Authors
*Tel: +1-404-894-3079. E-mail: ted.russell@gatech.edu.
*Tel: +86-10-62795269. E-mail: yuqibai@tsinghua.edu.cn.
Notes
The authors declare no competing financial interest.
■ ACKNOWLEDGMENTS
Y.H. and A.G.R.’s work for this publication was made possible
in part by funding from the USEPA under Grant Nos.
RD834799, RD833866, and RD835217. H.C.’s work for the
Bayesian model was supported by National Institutes of Health
Grant No. R21ES023763. Its contents are solely the
responsibility of the grantee and do not necessarily represent
the official views of the supporting agencies. Further, the US
Government does not endorse the purchase of any commercial
products or services mentioned in the publication. This study
was also supported by the State Environmental Protection Key
Laboratory of Sources and Control of Air Pollution Complex
(No. SCAPC201406) and by Tsinghua University (Nos.
20131089277 and 553302001).
■
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4759 DOI: 10.1021/acs.est.5b05940

Environ. Sci. Technol. 2016, 50, 4752−4759