Atmospheric Environment 173 (2018) 295–305

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Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

High-resolution spatiotemporal mapping of PM2.5 concentrations at T

Mainland China using a combined BME-GWR technique
Lu Xiaoa, Yichao Langa, George Christakosa,b,∗
a
Institute of Islands and Coastal Ecosystems, Ocean College, Zhejiang University, Zhoushan, China
b
Department of Geography, San Diego State University, San Diego, CA, USA

A R T I C L E I N F O A B S T R A C T

Keywords: With rapid economic development, industrialization and urbanization, the ambient air PM2.5 has become a
Particulate matter major pollutant linked to respiratory, heart and lung diseases. In China, PM2.5 pollution constitutes an extreme
Space-time analysis environmental and social problem of widespread public concern. In this work we estimate ground-level PM2.5
Remote sensing from satellite-derived aerosol optical depth (AOD), topography data, meteorological data, and pollutant emis-
Aerosol optical depth
sion using an integrative technique. In particular, Geographically Weighted Regression (GWR) analysis was
Bayesian Maximum Entropy
combined with Bayesian Maximum Entropy (BME) theory to assess the spatiotemporal characteristics of PM2.5
Geographically weighted regression
Meteorological fields exposure in a large region of China and generate informative PM2.5 space-time predictions (estimates). It was
found that, due to its integrative character, the combined BME-GWR method offers certain improvements in the
space-time prediction of PM2.5 concentrations over China compared to previous techniques. The combined BME-
GWR technique generated realistic maps of space-time PM2.5 distribution, and its performance was superior to
that of seven previous studies of satellite-derived PM2.5 concentrations in China in terms of prediction accuracy.
The purely spatial GWR model can only be used at a fixed time, whereas the integrative BME-GWR approach
accounts for cross space-time dependencies and can predict PM2.5 concentrations in the composite space-time
domain. The 10-fold results of BME-GWR modeling (R2 = 0.883, RMSE = 11.39 μg / m3 ) demonstrated a high
level of space-time PM2.5 prediction (estimation) accuracy over China, revealing a definite trend of severe PM2.5
levels from the northern coast toward inland China (Nov 2015–Feb 2016). Future work should focus on the
addition of higher resolution AOD data, developing better satellite-based prediction models, and related air
pollutants for space-time PM2.5 prediction purposes.

1. Introduction Peng et al., 2016).

China's atmospheric pollution is very serious. The main pollution
sources are fuel combustion, human activities and other natural pro-
cesses (e.g., dust). Ambient air pollutants that have a significant impact
on human health and the environment are composed of complex ma-
terials, including particulate matter, ozone, sulfur dioxide and nitrogen
dioxide. Fine particle particulate matter, PM2.5 (aerodynamic diameters
smaller than 2.5 μm), is the most problematic among these pollutants as
regards public health. PM2.5 particles can enter into the alveoli, sub-
sequently being retained in the lung parenchyma (Christakos and
Hristopulos, 1998; Dockery, 2009), thus causing severe heart disease,
cardiovascular diseases, respiratory diseases and even lung cancer
(Brook et al., 2010; Dhondt et al., 2011; Hoek et al., 2013). With rapid
economic development, PM2.5 pollution in China has become an ex-
treme environmental and social problem having an important impact
on the human body, the environment and the climate (Song et al., 2014;
Relatively small PM2.5 datasets are available in China. Ground-
based measurements are considered as the most reliable way of col-
lecting PM2.5 concentrations (Tao et al., 2017). Accordingly, most
pollutant concentration information has been obtained from ground-
level monitoring sites, a fact that has many limitations. Among them is
the considerable information bias, the limited credibility of the ex-
posure response results (Liu et al., 2007), and the sparsity and uneven
distribution of the monitoring stations (Gupta and Christopher, 2008).
These limitations affect the geographical and demographic range of a
study, so that it is usually impossible to determine the temporal and
spatial variation of PM2.5 concentrations over large geographic areas
(You et al., 2016b), For example, PM2.5 was not included in China's
national monitoring system until 2013 (Chu et al., 2016). So far, do-
mestic and foreign scholars have carried out PM2.5 variation analysis
and generated ground level PM2.5 concentration estimates using a
variety of statistical models. Christakos and Serre (2000) and Christakos

∗
Corresponding author. Institute of Islands and Coastal Ecosystems, Ocean College, Zhejiang University, Zhoushan, China.
E-mail address: gchristakos@zju.edu.cn (G. Christakos).

https://doi.org/10.1016/j.atmosenv.2017.10.062
Received 11 June 2017; Received in revised form 19 October 2017; Accepted 29 October 2017
Available online 21 November 2017
1352-2310/ © 2017 Elsevier Ltd. All rights reserved.
L. Xiao et al.
et al. (2001) have used Bayesian maximum entropy (BME) theory to
represent and predict spatiotemporal particulate matter distributions in
North Carolina and California, USA. Wang and Christopher (2003) used
linear regression models, whereas Liu et al. (2004) proposed a Chemical
Transport Model (CTM). Later, Reid et al. (2015) and Donkelaar et al.
(2011) also used the CTM. Lee et al. (2011) developed the day-specific
Mixed-Effect Model (MEM), Lee et al. (2012) used a space-time geos-
tatistical kriging model to estimate long-term ambient PM2.5 exposure
in U.S.A. Liu et al. (2009) and Kloog et al. (2011) proposed a two-stage
generalized additive model (GAM), and Ma et al. (2014) and (Xiao
et al., 2017) used Geographically Weighted Regression (GWR) tools.
Hence, remote sensing techniques, spatial and temporal modeling, and
statistical prediction theory have been individually or in combination
employed in the quantitative assessment of air pollution and environ-
mental health (Kim et al., 2015; Xiao et al., 2017).
In view of the above considerations, the objective of the present
work is to introduce and validate in terms of real data a new satellite-
based technique of composite space-time modeling and estimation of
PM2.5 concentrations in China during a four-month period: this is the
combined (or integrative) Bayesian Maximum Entropy-Geographically
Weighted Regression (BME-GWR) method. Advantages of the combined
BME-GWR method include its rigorous consideration of the physical
cross-space-time dependencies of pollutant distribution, the generation
of pollutant predictions in a realistic space-time domain rather than
separately, the inclusion of more general cases (non-linear and non-
Gaussian predictors), and its ability to jointly incorporate different
environmental predictors, including topography data (elevation) and
meteorological data (wind speed, precipitation, temperature, relative
humidity and pressure), as well as pollutant emission indicators (such
as NO2, CO, land use, population, and road network information).
2. Data and method
2.1. Study area
The present study focuses on the entire China, with the exception of
Fig. 1. Study area. The green dots represent the 1408 PM2.5 monitoring sites within the study area and the 43 sites in neighboring provinces. (For interpretation of the references to colour
in this figure legend, the reader is referred to the web version of this article.)
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Atmospheric Environment 173 (2018) 295–305
the Xinjiang, Tibet, Qinghai, Mongolia and Heilongjiang provinces
(Fig. 1), which were not included in the study because the PM2.5
monitoring sites in these areas are sparse (while these provinces cover a
total area of 5.33 million Km2 , they have only 89 monitoring sites, and
this monitoring limitation would seriously affect pollutant estimation
accuracy in provinces with serious pollution problems). On the other
hand, the study area covers about 4.18 million Km2 that include 1408
monitoring sites and 93% of the total population of China. For data
processing and mapping purposes, the study area is covered with a grid
consisting of 357,997 grid cells of 3 × 3Km2 size (Xiao et al., 2017).
2.2. Data
2.2.1. Ground-level pollutant measurements
The 24h-averaged PM2.5, NO2, and CO concentrations at nationally-
referenced monitoring stations during the period November 1, 2015 to
February 29, 2016 were downloaded from the China Environmental
Monitoring Center (CEMC, http://106.37.208.233:20035/). The ob-
served PM2.5 concentrations, which served as the dependent variable of
the pollutant space-time prediction (estimation) techniques used in this
work, include 1408 monitoring sites (Fig. 1) with a total of 3009 ob-
servations in the study area, and, also, 43 monitoring sites that were
evenly distributed in adjacent to the study area provinces to avoid any
edge-effects. PM2.5, NO2, and CO concentrations less than 2 μg / m3
(5.6% of total records) were discarded since they are below the estab-
lished detection limit (EPA, 2008). Also, stations where data were
available during less than 15 days per month were removed, according
to China National Ambient Air Quality Standards (CNAAQS). All 3009
observations were distributed during four months, i.e., there exist 953,
707, 529 and 820 observations during the months of November, De-
cember, January and February, respectively. Daily PM2.5, NO2, and CO
data were used to calculate the monthly average pollutant concentra-
tion at each site, and the monthly averages were obtained using the R
programming language (R version 3.3.2, https://www.r-project.org/).
Notice that most of the PM2.5 monitoring sites are clustered in urban
areas (rural areas have little coverage in China).
L. Xiao et al.
2.2.2. Aerosol optical depth data
MODIS (Kaufman et al., 1997) is an instrument aboard the Terra
and Aqua satellites operated by the U.S. National Aeronautics and
Space Administration (Remer et al., 2005). The aerosol optical depth
(AOD) data were obtained from the newly released MODIS collection of
six AOD products (http://ladsweb.nascom.nasa.gov/) with 3 km spatial
resolution. The 3 km AOD (MYD04_3k, MOD04_3k) were all retrieved
with the help of the same dark-target algorithm (a characteristic of the
algorithm is that its accuracy is slightly lower over land). The Dark-
Target (DT) aerosol retrieval algorithm is applied to satellite data to
derive aerosol properties, including aerosol optical depth (AOD) over
land and ocean, and aerosol size parameters over ocean. Products of the
DT aerosol retrieval algorithm are used to develop global and regional
AOD retrieval, to study the aerosols with clouds, and for air quality
assessment (Wu et al., 2016a,b; Levy et al., 2010). And the DT is better
for areas covered by green plants. And this is why we have carefully
selected the study area to meet this condition. Removed areas were
mostly deserts, mountains covered by snow etc. – such as Xinjiang
province and Tibet. During the study period (November 1, 2015 to
February 29, 2016) the 10:30am Terra and 1:30pm Aqua were used to
synthesize the Chinese regional daily AOD products. Technically, the
data processing steps were as follows: (a) the 550 nm wavelength
aerosol optical thickness data were selected following a geometric
correction; (b) after the geometric correction was embedded, the daily
550 nm wavelength aerosol optical thickness data were mosaicked to
obtain the daily product and the average AOD value of the overlapping
areas in the mosaic image was selected; and (c) MODIS Terra and
MODIS Aqua aerosol data were integrated in order to obtain the max-
imum usable range.
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Atmospheric Environment 173 (2018) 295–305
Fig. 2. The outline of BME-GWR.
2.2.3. Meteorological fields
As has been documented in the literature, weather conditions can
affect PM2.5 distributions (e.g., Liu et al., 2014). Daily data at the me-
teorological monitoring stations were collected, including precipita-
tion-Prec (0.1 mm), temperature-Temp (0.1 °C), relative humidity-RH
(%), air pressure-Pres (0.1Pa), and wind speed-WS (0.1 m/s), using the
China Meteorological Data Sharing Service System (http://cdc.cma.
gov.cn).
2.2.4. Land use information
Previous studies have showed that land-use information could affect
the relationship between PM2.5 concentrations and satellite AOD (Ma
et al., 2014, 2016, Kloog et al., 2015a; 2015b). For land-use informa-
tion, we downloaded 500m resolution surface classification data from
the Global Land Cover Facility-MODIS Land Cover (http://www.
landcover.org/data/lc/), and we measured the total grassland
(Green), water, urban, built-up (City) and forest areas covered by the
3 × 3Km2 AOD grid (the area was measured in m2 ).
2.2.5. Road network data monthly average
Road length data were extracted from the OpenStreetMap (http://
www.openstreetmap.org). Major roads, primary highways and railways
from all different layers were retained. The total road length (in m) was
calculated on the same 3 km grid of land-use data mentioned above.
2.2.6. Elevation data and population data
The 30m resolution digital elevation data (DEM) were downloaded
from the Shuttle Radar Topography Mission (SRTM, http://srtm.csi.
cgiar.org/SELECTION/inputCoord.asp). The 1 km population data
L. Xiao et al.
Fig. 3. Histogram and summary statistics of the GWR model variables for the four months during which PM2.5 monitoring took place (N = 3009 estimation points).
(Pop) were available from the Gridded Population of the World, Version
4 (GPWv4) (http://sedac.ciesin.columbia.edu/data/collection/gpw-
v4). Elevations and populations were subsequently averaged at each
3 × 3Km2 grid cell.
2.2.7. Data integration
For data integration purposes, at the data pre-processing stage: (a)
All meteorological data at a 3 km scale were interpolated using a spatial
interpolation software for climatic data (ANUSPLIN), whereas for the
NO2 and CO data at the 3 km scale (i.e., matching the AOD grid size) the
standard inverse distance weighted (IDW) interpolation software
(ArcGIS 10.3) was used. (b) All these data were integrated into records
appropriate for model fitting, validation and mapping purposes. (c) The
collected data were re-projected onto the Asia Lambert Conformal
Conic coordinate system. (d) Two square grids with 3 km and 30 km
spatial resolution were constructed, which consisted of a total number
of 357,997 and 3582 grid cells, respectively.
The 30 × 30Km2 grid data served as the soft information for BME-
GWR modeling purposes (for more details on the term “soft informa-
tion”, i.e., secondary information bases of various levels of uncertainty,
see sub-section 2.3.2 below). On the other hand, the 3 × 3Km2 grid
(AOD, NO2, CO and meteorological) data were used, together with the
3 × 3Km2 grid (land-cover, road length, elevation and population) data
to obtain the complete 3 km resolution dataset. The PM2.5 value at the
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center of each cell of the 30 × 30Km2 grid was calculated as the average
of the values on the 3 × 3Km2 grid nodes that fall within the 30 × 30Km2
grid cell. Finally, the complete PM2.5 sites dataset was extracted based
on all 3 × 3Km2 grid data in ArcGIS 10.3 (see, also, Xiao et al., 2017).
We notice that, due to the large number and variety of environmental
variables, they were standardized by using the z-score method fol-
lowing multiple linear regression (MLR). The purpose of MLR is to se-
lect the significant variables and eliminate any collinearity between
variables. MLR is the most common form of linear regression analysis.
As a predictive analysis, the multiple linear regression is used to explain
the relationship between one continuous dependent variable and two or
more independent variables. Each independent variable is given a
computed VIF and Tolerance value. When VIF value is large (> 10, for
example) and Tolerance < 0.1, collinearity is a problem and the of-
fending variables should be removed from the model.
2.3. Methods
2.3.1. The GWR model
Ordinary least squares (OLS) is a statistical technique for estimating
the unknown parameters of a linear regression model subject to the
condition of minimizing the sum of squares of the differences between
the observed responses (values of the variable being predicted) in the
given dataset vs. those predicted by a linear function of a set of
L. Xiao et al. Atmospheric Environment 173 (2018) 295–305

Table 1 sense, GWR is a refined moving windows approach where observations

Parameterization and model fitting of the GWR and OLS models. within the windows are weighted based on distance from the regression
point, rather than evaluated equally as in moving windows regression.
Statistical model OLS GWR
Like moving windows, the GWR technique calibrates the model at
Variables Coefficient Accuracy Value multiple points in the study space, using linear combinations of
indicators neighboring data points within a window surrounding the regression
point; as such, GWR is an enhanced version of moving windows re-
November AOD (unitless) 2.12 R2 0.779
Prec (0.1 mm) 0.91 RMSE 14.87 gression in which distance-based weights are added to neighboring
Pres (0.1Pa) 11.73 MPE −0.085 points, and bandwidth is allowed to vary across the study area. The
RH (%) −3.56 MAE 10.89 GWR method embeds spatial location in the regression parameters and
WS (0.1 m/s) −0.17 ME −0.614 considers local parameter estimates (Lin et al., 2015b). In more words,
Temp (0.1 °C) −17.97
8.12
instead of estimating global parameter values, by estimating the para-
NO2 ( μg / m3 )
3.61
meters at each location GWR generates a continuous surface of spatially
CO ( μg / m3 )
Road_Length (m) 0.5
varying parameter values (Hu et al., 2013). The GWR model can assess
DEM (m) −0.56 the influence of independent variables on dependent variables in terms
Pop (people) 0.44 of the location changes and the spatial heterogeneity of the relationship
Green (m2) −1.33 between an independent and a dependent variable (Bagheri et al.,
Forest (m2) −0.78
2009). Before the development of the GWR method, the OLS model was
City (m2) 1.66
Water (m2) −0.49 used to test the spatial homogeneity of the relationship between vari-
Intercept 41.61 ables. The Koenker (BP) Statistic is a test used to determine if the model
R2 0.69 explanatory variables have a consistent relationship with the dependent
variable (which we are trying to predict/understand) both in geo-
December AOD (unitless) −3.52 R2 0.828
Prec (0.1 mm) −2.07 RMSE 12.25 graphic space and in data space, that is, the Koenker (BP) statistic was
Pres (0.1Pa) 9.43 MPE −0.043 used to test non-stationarity (assuming that the test is statistically sig-
RH (%) −4.20 MAE 9.47 nificant, p < 0.01), in which case the relationship is characterized as
WS (0.1 m/s) −25.78 ME 0.254 non-stationary or heteroskedastic.
Temp (0.1 °C) −20.12
The GWR model can provide the spatial variance of the relationship
NO2 ( μg / m3 ) 10.89
8.53
between PM2.5 concentrations and other environmental variables.
CO ( μg / m3 )
Road_Length (m) 2.07
Mathematically, the GWR is a linear regression model expressed as
DEM (m) 4.40
Pop (people) −1.07 P2.5, i = β0 (s1, i, s2, i ) + ∑k βk (s1,i, s2,i) xik + εi (1)
Green (m2) 0.19
Forest (m2) −1.78
City (m2) -0.48 (i = 1,2, ...n) , where (s1, i, s2, i ) are the spatial coordinates of each sample
Water (m2) 1.25 point i , β0 (s1, i, s2, i ) is the intercept of sample i , βk (s1, i, s2, i ) is the re-
Intercept 37.84 gression coefficient of sample point i , x ik is an observation of the kth
R2 0.77
environmental variable of sample i , P2.5, i is the ground-level PM2.5
January AOD (unitless) 0.58 R2 0.803
concentration at sample i and εi is the random error. If β1 = β2 = ...=βn ,
Prec (0.1 mm) −37.83 RMSE 14.68 the GWR method reduces to the earlier OLS model (Fotheringham et al.,
Pres (0.1Pa) 7.61 MPE −0.055 2002). Notice that, in this work separate GWR models were fitted to the
RH (%) 0.38 MAE 11.14 data of each month, with the general structure.
WS (0.1 m/s) −17.97 ME −0.135
NO2 ( μg / m3 ) 11.18 PM2.5∼AOD+Prec+Pres+RH+WS+Temp+NO2+CO+DEM+Roa-
CO ( μg / m3 ) 6.05 d_Length + Pop + Green + Forest + City + Water, (2)
DEM (m) 2.38
Forest (m2) −2.45 where PM2.5 here refers to the monthly-averaged ground-level PM2.5
Intercept 49.35 concentrations ( μg / m3 ), and the symbol “∼” denotes that the PM2.5 is
R2 0.67
related to/can be predicted by the following environmental factors
February AOD (unitless) 5.96 R2 0.629 (seen as independent variables): the MODIS aerosol optical depth value
Pres (0.1Pa) 22.20 RMSE 17.67 AOD (unitless), the precipitation Prec (0.1 mm), the air pressure Pres
RH (%) −19.00 MPE −0.044 (0.1Pa), the relative humidity-RH (%), the WS is wind speed (0.1 m/s),
WS (0.1 m/s) 44.02 MAE 12.64 Temp denotes temperature (0.1°C), NO2 is nitrogen dioxide ( μg / m3 ), the
NO2 ( μg / m3 ) 6.56 ME 0.49
carbon monoxide CO ( μg / m3 ), the elevations DEM (m), the sum of road
CO ( μg / m3 ) 1.09
lengths Road_Length (m), the count of people Pop, and the land-use
City (m2) −1.57
Forest (m2) −1.88 cover the Green, Forest, City, and Water areas (m2 ).
Water (m2) −0.98 In this study, adaptive bandwidths were used due to the uneven
Intercept 63.40 distribution of the PM2.5 data points. These bandwidths were obtained
R2 0.53 by minimizing the corrected Akaike Information Criterion value (AICc).
There are other bandwidth selection criteria such as the standard
Akaike Information Criterion (AIC) and the Bayesian Information
explanatory variables. Using the OLS, the Koenker (BP) Statistic
Criterion (BIC). Compared to AIC, the AICc is less biased and can avoid
(Koenker's studentized Bruesch-Pagan statistic) is a test that determines
the large variability and under-smoothness tendency of AIC (Hurvich
whether the explanatory variables in the model have a consistent re-
et al., 1998). Unlike AIC, the BIC is not an estimator of the Kull-
lationship to the dependent variable both in geographic space and in
back–Leibler information distance that is used to decide which model is
data space.
closest to reality (Hu et al., 2013). Also, how the BIC could be extended
Based on OLS theory, Fotheringham et al. (1998) developed a
to non-parametric models with variable bandwidth and effective de-
method to explore spatial heterogeneity by means of local regression,
grees of freedom is yet not clear (Bekara et al., 2005).
termed the geographically weighted regression (GWR) method. In a

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Fig. 4. The spatiotemporal empirical covariance (in (μg / m3)2 ) and the fitted theoretical model used by the BME-GWR technique.

2.3.2. The BME technique economically developed area of China. The role of GWR in this in-
Bayesian Maximum Entropy (BME, Christakos, 1990, 2000) is a tegration was to generate soft data. The monthly GWR models involve
spatiotemporal modeling and prediction theory with very general fea- different variables after they are filtered by OLS (Table 2), where Eq (2)
tures (e.g., it provides non-linear estimators and allows non-Gaussian describes the general multi-variable structure of monthly GWR. And,
probability laws, it incorporates information from many different the role of BME is to use these soft data together with hard data to
sources, as well as core and site-specific knowledge bases-KB). Its im- produce space-time maps of PM2.5 distribution during four months
plementation is made possible in practice in terms of various software (3 × 3 Km2 resolution).
libraries, like the one used here, namely, the Spatiotemporal Epistemic Specifically, the hard data that served as input to the BME-GWR
Knowledge Synthesis Graphical User Interface software library (SEKS- technique included the measured PM2.5 concentration values at mon-
GUI, Yu et al., 2007). The basic set of BME equations of space-time itoring stations for all eligible station-days during the period November
PM2.5 estimation used in the present study are (Christakos, 2000, 1, 2015 to February 28, 2016 (all predictions are about monthly-
2010), averaged data). On the other hand, the soft data generated by the GWR
model and used in the GWR-BME technique consisted of PM2.5 esti-
∫ dG (g − g ) e μ ⋅ g = 0, mates and an associated variance at the center of each 30 × 30 Km2
∫ dSe μ ⋅ g − AfPM2.5 = 0 (3a-b) grid cell. The soft data obtained by the GWR model (in the form of
probability distributions with mean and variance estimated by GWR)
where g is a vector of functions expressing mathematically the available
serve as useful auxiliary information that can improve the accuracy of
core G-KB, including theoretical space-time covariance models, popu-
the predictions generated by BME at the unsampled points of the space-
lation exposure laws, and scientific theories, including the GWR model;
time grid. Notice that, four separate GWR models were fitted to the data
g denotes the mean value of g ; S denotes the available site-specific KB
during each month, and the BME-GWR method was applied for the
about the pollutant in the specific study region as described earlier (S-
entire four-month period. An outline of the combined BME-GWR
KB may include AOD, meteorological monitoring data, road networks
technique is shown in Fig. 2.
information, land-use data, DEM and population); μ is a vector of
coefficients representing the relative importance of each g -function ( μ⋅g
denotes the inner product of the vectors g and μ , which are both
2.3.4. 10-Fold cross-validation between spatiotemporal estimates and
functions of space-time); fPM2.5 is the probability law of the PM2.5 dis-
ground observations
tribution in space-time, where the distribution is considered as a
In order to assess the performance of the combined BME-GWR
random field model (Christakos, 2017); and A is a normalization
technique, the coefficient of determination (R2), the mean prediction
parameter. Technically, S-KB may represent both hard and soft data:
error (MPE), the mean error (ME), the mean absolute prediction error
hard data include site-specific measurements with negligible or no
(MAE), and the root mean squared prediction error (RMSE) were the
uncertainty associated with them, whereas soft data include site-spe-
accuracy indicators calculated in terms of the differences between the
cific information in the form of uncertain observations, auxiliary vari-
space-time PM2.5 predictions generated by the combined BME-GWR
ables, and probabilistic assessments (e.g., intervals of possible values
technique and the ground-level PM2.5 observations at a set of control
and probability distribution functions of any shape; He and Kolovos,
points.
2017). This allows BME to rigorously integrate any non-Gaussian soft
Since the sample-based, 10-fold cross validation (CV) procedure
data, such as soft data with a truncated Gaussian distribution (Reyes
(Diego Rodriguez et al., 2010; Lee et al., 2011; Hu et al., 2014; Ma
and Serre, 2014).
et al., 2014) has been more widely tested in previous PM2.5-AOD
Eq (3a-b) can be solved with respect to the PM2.5 probability law
modeling studies than other procedures (such as, e.g., the site-based CV
fPM2.5 at all pollutant mapping points (i.e., space-time points at which
technique, Chang et al., 2014), in this study we also chose the 10-fold
predictions of the PM2.5 concentrations are sought). Also, it has been
CV method to test the potential over-fitting of the BME-GWR technique.
proven in theory that Kriging is a special case of BME under limiting
Previous GWR studies that used the 10-fold cross validation method
conditions –linear estimation, Gaussian distribution and hard only site-
include Hu et al. (2013), Ma et al. (2014), Fang et al. (2016), You et al.
specific data are considered (Christakos, 2000). More technical details
(2016b), and Zou et al. (2016). In the present study, the data set was
concerning the BME approach above can be found in the relevant lit-
divided into k = 10 folds, a classifier learned using k-1 = 9 folds, and
erature. Software libraries have been developed dealing with the so-
an error value was calculated by testing the classifier in the remaining
lution of Eq (3a-b) in real-world conditions, including BMElib, SEKS-
fold. Then, the k-fold cross-validation classification (k-cv) error esti-
GUI, QuantumBME, and StarBME (Yu et al., 2007).
mator was calculated as the average value of the errors committed in
each fold. Note that the k-cv error estimator depends on two factors: the
2.3.3. The combined (integrative) BME-GWR technique
training set and the partition into folds (Diego Rodriguez et al., 2010).
In this work, we developed a combined (integrative) BME-GWR
technique to estimate space-time PM2.5 concentrations in the most

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Fig. 5. Scatter plots of model fitting and validation result. The solid line denotes the trend line: (a) CV results for the BME-GWR technique (N = 3009 estimation points, t = 4 months);
(b)–(e) are GWR model fitting results during the four months considered.

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Table 2 where c1 = 0.8, c2 = 0.2, a s1 = 1, a s2 = 14 (in °C), and at1 = 3.8, at2 = 13
10-fold cross-validation results of space-time BME-GWR estimation of monthly PM2.5 (in months). Using the above covariance model, we obtained BME es-
averages (k = 1408 monitoring stations, N = 3009 estimated points, t = 4 months).
timates of PM2.5 that are representative of the actual distribution.
Method R2 RMSE MPE MAE ME
3.3. Cross validation results
BME-GWR 0.883 11.39 −0.067 7.90 −1.065
Fig. 5 and Table 2 show the cross-validation (CV) results of the BME-
GWR estimation technique. The accuracy indicators of technique, in-
3. Results
cluding RMSE, MPE, MAE, and ME, are listed in Table 2. For model
validation purposes, the R2, RMSE, MPE, MAE and ME values of the
3.1. Descriptive statistics
BME-GWR technique were 0.883, 11.39, −0.067, 7.90, and
−1.065 μg / m3 , respectively.
Various simulations of the 16-variable model were initially gener-
ated using the GWR and OLS techniques. The histograms and summary
3.4. Spatial distributions of PM2.5 predictions
statistics of GWR variable fitting for the four months (Nov–Dec 2015,
Jan–Feb 2016) are plotted in Fig. 3. These plots show that all the
Fig. 6 presents ground-level PM2.5 measurements and the corre-
variables are roughly lognormally and unimodally distributed. The
sponding monthly-averaged PM2.5 predictions using the space-time
geometric mean, standard deviation, maximum, and minimum for all
BME-GWR technique. The first observation is that the fact that most of
variables for all days are also presented in Fig. 3. The mean PM2.5
the PM2.5 monitoring sites are clustered in urban areas (rural areas have
concentration over all monitoring sites is 63.75 μg / m3 , and the overall
little coverage in China), may impact the performance of a space-time
mean of the MODIS generated AOD is 0.41.
prediction technique that covers the entire China. Provinces (such as
On the basis of the OLS results, the Koenker (BP) Statistic tests were
Xinjiang, Tibet, Qinghai, Mongolia and Heilongjiang) with sparse and
found to be statistically significant (p < 0.01) during the four months
unevenly distributed PM2.5 monitoring sites were removed from the
considered in the present study, indicating that there is a non-stationary
present study. Also, the considerable number of missing PM2.5 data in
relationship between dependent variables and independent variables,
the Tibet and Xinjiang provinces can lead to substantial errors in PM2.5
that is, the local sublinearity between environmental variables and
concentration prediction (Ma et al., 2014; Fang et al., 2016). These
PM2.5 concentrations in a wide geographic area can be better inter-
provinces, also, were not included in the present study. The second
preted by the GWR model. This result is consistent with previous stu-
observation is that, while the Beijing, Tianjin and Hebei provinces were
dies (Hu et al., 2013; Song et al., 2014; Zou et al., 2016).
always highly polluted areas, in southern provinces the air quality has
Table 1 provides a summary of the parameters of the fitted GWR
been much better. The BME-GWR technique provided considerably
and OLS models. The overall mean adjusted R2 = 0.75 (GWR model) is
detailed maps of the space-time pollutant distribution due to its in-
greater than the overall mean adjusted R2 = 0.67 (OLS model). This
corporation of soft data.
result confirms the superiority of the GWR model over the OLS model in
As the maps of Fig. 6 reveal, the PM2.5 concentrations were high in
simulating site-based PM2.5 concentrations. These findings are con-
the northern part of the study area, especially in the Beijing, Tianjin,
sistent with previous GWR applications (Hu et al., 2013; Zou et al.,
Hebei and Shandong provinces. The spatial gradients of PM2.5 con-
2016). The GWR result for December was the most accurate among the
centrations showed a significant change during the four months con-
GWR results for the four months considered, with the highest R2 (=
sidered, and the overall PM2.5 concentration trend was high in the north
0.828) and the lowest RMSE (=12.25 μg / m3 ). As regards the OLS re-
and low in the south part of the study region. The temporal PM2.5
sults, the model with the highest R2 (=0.77) corresponds to December.
concentrations in the study region showed a clear monthly variation,
Different monthly OLS models have different variables, and the same
and there was a PM2.5 concentration trend from the northern coast
variable has different relationships (positive or negative) with PM2.5.
toward inland during the period November of 2015 to February of
For example, the AOD coefficients for December, November, January,
2016. A possible explanation may be the monsoon weather conditions
and February are, respectively, −3.52, 2.12, 0.58, and 5.96.
that caused the dispersion of the coastal PM2.5 pollution towards inland
China (Ainslie et al., 2008). The average PM2.5 concentration during
3.2. Covariance model fitting December 2015 (reaching 76.1 μg / m3 ) was significantly higher than
that during the other three months, while the most widely distributed
The covariance function (Kolovos et al., 2004; Ma, 2008) is a sta- PM22.5 concentrations were observed during January 2016 (with spa-
tistical tool that offers information about the variation of PM2.5 con- tially distributed values that exceeded the 85 μg / m3 level).
centrations across space-time, when is mathematically represented by a
spatiotemporal random field (Christakos, 2017). Concerning the em- 4. Discussion
pirical space-time covariance presented in Fig. 4, we noticed that the
PM2.5 covariance used by the combined BME-GWR technique had a From a methodological perspective, this work presented a combined
linear shape at the space-time origin (in random field modeling terms, BME-GWR technique of space-time pollutant modeling and mapping. In
this covariance shape is interpreted as characterizing considerable this setting, the role of GWR was to generate “soft” data, and that of
PM2.5 concentration changes both in space and in time), followed by a BME to use these data together with the available “hard” data to pro-
sharp PM2.5 covariance drop along space, and a very slow decline along duce space-time maps of PM2.5 distribution over China during a four-
the time axis (this dual behavior indicates a short PM2.5 correlation month period. In particular:
range in space and a long PM2.5 correlation range in time). Given that
four months are considered in this study, the temporal correlation of (a) The BME approach is able to integrate general or core KBs (theo-
adjacent months is strong. retical covariance models, trend functions, physical laws, and sci-
In light of these empirical PM2.5 covariance features, the following entific relationships) about the attribute of interest with site-spe-
theoretical covariance model was fitted to the empirical one of Fig. 4, cific KBs (hard or accurate data, such as monthly-averaged PM2.5
concentrations, and soft data in the form of uncertain measure-
cPM2.5 (h, τ ) = c1 ⎛⎜1 −
3h
+
h3 ⎞ ⎛
3 ⎟⎜
1−
3τ
+
τ3 ⎞
3 ⎟
+ c2 e
−3 ( ah + aτ )
s2 t2 ments, probabilistic assessments and auxiliary information) to
⎝ 2a s 2a s1 ⎠ ⎝ 2a t 2a t1 ⎠
1 1 generate space-time PM2.5 prediction maps and the associated
(4) prediction accuracy maps.

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Fig. 6. (a)–(d) Ground measurements and (e)–(h) spatial distribu-

tions of monthly PM2.5 concentrations generated by the BME-GWR
space-time technique during November 2015, December 2015,
January 2016, and February 2016.

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L. Xiao et al. Atmospheric Environment 173 (2018) 295–305

Table 3
Summary of previous GWR, improved GWR, and Bayesian models PM2.5 results in China.

Publication Study period Model 10-fold CV-R2 and RMSE

Ma et al. (2014) 2012–2013 GWR R2 = 0.64, RMSE = 32.98(N = 835), China.

Song et al. (2014) 2012–2013 GWR R 2 = 0.738, RMSE = 32.98(N = 37), PRD.
You et al. (2016b) 2014 GWR R 2 = 0.760, RMSE = 20.85 (MODIS, N = 943); R 2 = 0.850, RMSE = 24.86 (MISR, N = 943), China.
Lv et al. (2016) 2014 Bayesian R 2 = 0.780, RMSE = 33.39 (N = 298), North China.
You et al. (2016a) 2014 GWR R 2 = 0.79, RMSE = 18.6 (N = 943), China.
Zou et al. (2016) 2013 GWR, OLS R 2 = 0.750, RMSE = 10 (GWR, N = 52), R2 = 0.530, RMSE = 16 (OLS, N = 52), BTH
Fang et al. (2016) 2013/1–2014/6 TSAM R2 = 0.80, RMSE = 22.75 (TSAM, N = 509–945), China

(1) N denotes the number of PM2.5 monitoring sites.

(2) Model: GWR (Geographically Weighted Regression); Bayesian model, Bayesian hierarchical framework; OLS (ordinary least square); TSAM (timely structure adaptive modeling) based
on GWR.
(3) PRD (Pearl River Delta region); BTH (Beijing City, most of Tianjin City, and parts of Hebei Province).

(b) The GWR model, on the other hand, explores spatial heterogeneity
by means of local regression. Instead of estimating global parameter
values, by estimating the parameters at each location GWR gen-
erates a continuous surface of spatially varying parameter values.
Also, GWR can assess the influence of independent variables on
dependent variables in terms of location changes and spatial het-
erogeneity of the relationship between an independent and a de-
pendent variable.
As regards (b), many earlier studies have used various versions of
GWR-based models, as wells as Bayesian models. Each one of these
studies exhibited different characteristics because of the different con-
ditions, PM2.5 concentration levels, and geological and meteorological
environments considered (Table 3). By accounting for cross space-time
correlations, allowing more general assumptions (non-linear and non-
Gaussian predictors), and incorporating a sufficient number of key
environmental factors (capable of explaining a large proportion of the
PM2.5 concentration variance) the model used in this work performed
better than the earlier ones, because of its advantages as outlined in the
Introduction section and in other parts of the paper. In particular, it
provided the best 10-fold cross-validating results (R2 = 0.883,
RMSE = 11.39).
As regards (a), it was shown that the combination of the BME
technique with the GWR model offers certain improvements in the
space-time prediction (estimation) of PM2.5 concentrations over China.
In particular, we compared the combined BME-GWR technique pro-
posed in this work with seven previous studies of satellite-derived PM2.5
concentrations in China. The combined BME-GWR technique generated
realistic maps of space-time PM2.5 distribution, and its performance was
superior to these techniques, in terms of prediction accuracy.
Other important differences and advantages of BME-GWR over the
previous techniques include the following. First, due to sparse sites and
AOD missing data, Ma et al. (2014) obtained higher PM2.5 concentra-
tion estimates in rural regions and slightly lower concentration esti-
mates in the Sichuan basin. The study by Fang et al. (2016) was char-
acterized by a considerable number of missing PM2.5 data in the Tibet
and Xinjiang provinces, which generated substantial errors in the PM2.5
concentration estimates they derived. Second, in the present study we
collected and processed more data of environmental factors than in
previous studies, such as 3 km AOD, pollutant emissions, meteor-
ological data and land use. Furthermore, for the first time, we in-
corporated a GWR model into the BME estimation technique in a high
spatial/temporal resolution setting. The calculated accuracy indicators
of the combined GWR-BME technique showed a considerable im-
provement compared to the existing techniques. As was mentioned
throughout the paper, the limited number of monitoring sites is a
limitation of this work, as well as the lack of information about other
environmental variables. When more monitoring stations are estab-
lished in certain rural areas, the BME-GWR can be used to improve the
study of air pollution in these areas. And, we hope that data about more
environmental variables will become available, such as wind directions,
in this case.
The findings of this study are useful for exposure assessment and
health risk management purposes, as well as for air pollution control
strategies and environmental protection related studies. Accordingly,
future work on the combined GWR-BME technique should consider (i)
adding higher resolution data sources, such as 1 km AOD data (Lin
et al., 2015a; Wu et al., 2016a,b), (ii) focusing on developing satellite-
based models for the prediction of historical PM2.5 and other air pol-
lutants, (iii) visualizing exposure estimates in ArcEngine 10 in order to
properly assess the long-term effects of PM2.5 exposure on human
health and facilitate better prevention and control of PM2.5 exposure in
China.
Acknowledgments
This research was supported by the National Science Foundation of
China (Grant No. 41671399).
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