Sie sind auf Seite 1von 8
Article pubs.acs.org/est Improving the Accuracy of Daily PM 2 . 5 Distributions Derived from the
Article

Article

Improving the Accuracy of Daily PM 2.5 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 fi ne particulate matter concentrations (PM 2 . 5 ),

ABSTRACT: The accuracy in estimated ne particulate matter concentrations (PM 2.5 ), 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-speci c linear regression model was rst developed to ll in missing AOD data. A novel interpolation-based variable, PM 2.5 spatial interpolator (PMSI 2.5 ), was also introduced to account for the spatial dependence in PM 2.5 across grid cells. A Bayesian hierarchical model was then developed to estimate spatiotemporal relationships between AOD and PM 2.5 . These methods were evaluated through a city-speci c 10-fold cross-validation procedure in a case study in North China in 2014. The cross validation R 2 was 0.61 when PMSI 2.5 was included and 0.48 when PMSI 2.5 was excluded. The gap- lled AOD values also e ectively improved predicted PM 2.5 concentrations with an R 2 = 0.78. Daily ground-level PM 2.5 concentration elds 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.

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 μ m or less (PM 2.5 ), has been a major component of the severe air pollution levels experienced in many cities in China in recent years. PM 2.5 is the dominant pollutant of concern, especially during the winter. 1 3 Since PM 2.5 can eciently penetrate into human lungs and bronchi, 4 , 5 long-term and short-term exposures to PM 2.5 can increase premature mortality and morbidity. 5 One major limitation with ground-level measurements of PM 2.5 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 PM 2.5 concentrations. 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 PM 2.5 particle mass scatter sunlight, leading to a strong association between the mass of PM 2.5 and observed AOD. 10 All else being equal, as the number (and mass) of particles increases, light scattering increases, leading to

9

,

6

8

light scattering increases, leading to 9 , 6 − 8 © 2016 American Chemical Society 4752

© 2016 American Chemical Society

4752

an increase in AOD. While the association between PM 2.5 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 PM 2.5 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 eect (LME) model, 12 , 13 geo- graphically weighted regression (GWR) model, 14 , 15 remote

sensing formula,

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 PM 2.5 . 8 , 19 Among all these studies, treating the linear slopes and intercepts between AOD

16

Received: December 10, 2015

Revised: March 23, 2016

Accepted: April 4, 2016

Published: April 4, 2016

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759

Environmental Science & Technology

Article

Environmental Science & Technology Article Figure 1. Study area and the locations of PM 2 .

Figure 1. Study area and the locations of PM 2.5 monitoring stations as shown by points. The right panel depicts the average satellite-based AOD values in 2014.

and PM 2.5 at di erent locations and at di erent time points as spatially and temporally correlated random e ects has been shown to be promising in a study conducted in the southeast

However, to our knowledge, such a statistical

United States.

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 albedos 21 (e.g., snow and ice), and potentially, very high PM 2.5 pollutant levels. 22 , 23 If the missing AOD values are related to high PM 2.5 pollution levels, the average PM 2.5 concentrations estimated

using only the retrieved AOD elds can be underestimated. Several attempts have been made to solve this issue. Kloog et al. lled in missing AOD values by smoothing the mean PM 2.5 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 speci c, 19 , 27 such that the bias could not be e ectively corrected when calculating the mean in a small number of days. Just et al. predicted PM 2.5 levels within the grid cells with missing AOD by using PM 2.5 levels in the neighboring grid cells, based on season-speci c spatial

Ma et al. used ordinary Kriging to interpolate the

patterns.

available retrieved AOD values. 14 However, their method could have signi cant 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 coe cients in a linear regression setting. We also considered using spatially interpolated PM 2.5 concen- trations as a predictor and lled 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- lling method are introduced in the Materials and Methods . Model estimation, performance evaluation, and PM 2.5 pre- diction results are presented in the Results and Discussion .

20

28

MATERIALS AND METHODS

Study Area. Figure 1 shows the North China study area. This region includes ve 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 PM 2.5 and its precursors. 30 Increasing vehicular population and electricity demand also worsen the air quality in this region. 31 The annual mean PM 2.5 concentrations in this region was 93

4753

μ g/m 3 in 2014, about nine times the World Health Organization (WHO) recommended standard of 10 μ g/m 3 . 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 PM 2.5 Data. Hourly ground-level PM 2.5 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 PM 2.5 concentrations from monitors that are located in a same grid cell. It is worth noting that point measurements of PM 2.5 concentrations were used to represent the area-average PM 2.5 levels over a grid cell. This may cause potential bias due to a change of support. Specically, the grid- average concentrations may not fully re ect the spatial variation in PM 2.5 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 PM 2.5 concentrations were computed among

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759

Environmental Science & Technology

Article

Environmental Science & Technology Article Figure 2. (a) Average PM 2 . 5 concentrations; (b) daily

Figure 2. (a) Average PM 2.5 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 PM 2.5 concentrations in that grid cell. It is clear that mean PM 2.5 concentrations were consistently higher on days when AOD observation were missing than when AOD data were present ( Figure 2 a). To quantitatively measure the spatial and temporal pattern of AOD missing values, SVVR (spatial valid value ratio, de ned in SI) and TVVR (temporal valid value ratio, de ned in SI) were used. Daily SVVR values, shown in Figure 2 b, indicate that missing AOD was more signi cant 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 2 a), negative bias in long-term PM 2.5 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-speci c formula was introduced, based on a linear assumption of the relationship between PM 2.5 and AOD: 10

AODe = a

ij

,

s

PM

i

, j

PM

s

, j

AODo + b

,

s j

s

(1)

AODe i, , j refers to the estimated AOD value on day i in grid cell j. PM i,j refers to the daily mean PM 2.5 concentration observed on day i in grid cell j. AODo s ,j refers to the average retrieved AOD values in grid cell j and in season s , where s = 1 denotes warm season from Apr 16Oct 15 and s = 2 denotes cold seasons as the remaining days in a year. PM s,, j refers to the average PM 2.5 concentrations in grid cell j in season s. The linear relationship was tted separately in 53 cities. The city- specic models were then used to predict missing AOD values in grid cells containing PM 2.5 monitors. Second, we combined the estimated and retrieved AOD values to interpolate missing AOD values in the other grid cells without PM 2.5 monitors using ordinary Kriging (OK) with exponential covariance function and obtained a nal AOD data set with complete spatial coverage for each day. Interpolated Ground PM 2.5 Data. We proposed a novel variable based on the interpolation of PM 2.5 observations to be used in combination with AOD. A spatial interpolation utilizes the spatial dependence among observations to obtain optimal

4754

weights for predicting PM 2.5 levels at unobserved locations. The uncertainties (prediction standard errors) of the interpolated PM 2.5 concentration eld 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 PM 2.5 (PMI 2.5 ) value using the OK method. Specically, we rst randomly removed the monitors in 10% of 53 cities within the study area. PMI 2.5 values at the removed sites were obtained from kriging the monitors from the remaining cities. This procedure was repeated 10 times to obtain interpolated PMI 2.5 values at all monitors. To further control the uncertainties with the variable PMI 2.5 , we de ned the nal PM 2.5 spatial interpolator (PMSI 2.5 ) as follows

P MSI

and

f ( x )

2.5

=

=

PMI

10%

×

σ

t

2.5

σ (PMI )

2.5

1

(

x

α

+ 1

)

= PMI

2.5

PMI

2.5

× f

(PMI )

2.5

SE(PMI )

2.5

(2)

(3)

where σ(PMI 2.5 ) and σ t refer to, respectively, the uncertainties of PMI 2.5 and the target uncertainties in that grid cell. The

function f is a continuous inverse proportional function to constrain the uncertainties of PMI 2.5 to be a relatively small proportion of the original interpolated values (PMI 2.5 ). The proportion begins with 10% and decreases with increasing PMI 2.5 . The parameter α determines rate of decrease. When PMI 2.5 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 PMSI 2.5 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 classi cation of the

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759

Environmental Science & Technology

Article

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 PM 2.5 measurements 20 ( eq 4)

P M( st, ) = α ( st, ) ×+AOD αε( st, ) + ( st, )

0

1

(4)

where PM( s , t ) denotes the PM 2.5 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 speci c slope and intercept are, respectively, designated as α 0 ( s , t) and α 1 ( s , t). The residual errors ε( s, t ) are assumed to be normally distributed with mean zero and variance σ 2 . Model coe cients have both a temporal and spatially dependent structure. The coecients of the linear regression are separated into a second level

α (,st ) =++β ()s

0

0

β ()t

0

and

α (,st ) =++β ()s

1

1

β ()t

1

λ Z

0

0

λ Ζ

1

1

(5)

(6)

where β i ( s) and β i ( t ), respectively, refer to the underlying independent spatial and temporal processes that determine the spatiotemporal variations of the slope (for i = 0) and intercept (for i = 1). The parameter vectors λ i represent xed eects for meteorological, land cover variables: Z 0 for the slopes (for i = 0) and Z 1 for the intercepts (for i = 1). Speci cally, eq 5 models the relationships between AOD and PM 2.5 , with potential interactions between AOD and other predictors, and eq 6 models the underlying processes that have direct eects on the PM 2.5 levels. PMSI 2.5 is a predictor variable included in Z 1 to capture addition variation in PM 2.5 not explained by AOD and the other predictors. In this study, we used a tapered conditional Kriging method to interpolate the spatial coe cients β i ( s) in eq 2 for spatial dependence. 20 For those days without PM 2.5 AOD pairs, we used a linear autocorrelation function to model the temporal coecients β i ( t ), which speci es that β i ( t) is proportional to the weighted average between the neighboring days. 20 There- fore, we could obtain, with complete coverage, the spatially and temporally dependent coecient elds through interpolating the tted AOD eld. We used the Markov Chain Monte Carlo (MCMC) method for model tting under the Bayesian framework. One advantage of employing a Bayesian hierarchical framework is that the model could account for uncertainties in parameter estimates and PM 2.5 predictions. This facilitates the model outputs being incorporated in human exposure and health impact evaluations that considers exposure uncertain- ties. 36 , 37 It is worth noting that the tted model can only be used to predict AOD values within the temporal extent of the available data, as day-speci c AOD PM 2.5 relationships beyond the time scope (i.e., temporal extrapolation) were not estimated in our model structure. Model Evaluation Workow. We evaluated the eective- ness and performance of the AOD gap- lling method, the novel variable PMSI 2.5 as an additional predictor, and the statistical

model formulation based on out-of-sample prediction. We designed a work ow (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 ll the missing AOD values and to t two AOD PM 2.5 models ( eq 4 ), with and without the variable PMSI 2.5 . The remaining group served as the test data set where the predicted PM 2.5 values were compared to the observed measurements. The PM 2.5 concentrations in the test data set could be predicted by either the retrieved AOD values or the lled AOD values. The evaluation was done by withholding a di erent 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 Specically, 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 condence 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), R 2 , and the linear regression coecients (along with their standard errors). NME and RMSE are de ned in the SI .

RESULTS AND DISCUSSION

Model Parameters Estimation. The mean PM 2.5 concen- trations from monitors for the nal data set was 58.8 μ g/m 3 , which is 1.7 times that of the China Class I standard. On average, AOD and PMSI 2.5 were signi cantly associated with their 95% posterior intervals not including zero (Table 1 ), with

Table 1. Statistical Assessment of the Estimated Coe cients

terms in λ 1

eEst c

SE d

Low95 e

 

Up95 f

intercept

23.44

18.80

13.19

60.99

AOD

21.66

3.93

15.34

30.81

PMSI 2.5

1.16

0.016

1.12

1.19

Green.fac

a

0.21

0.31

0.4

0.82

Urban.fac

b

0.64

1.82

2.97

4.20

elevation

0.012

0.004

0.02

0.0044

temperature

0.04

0.062

0.084

0.163

PBL

0.0013

0.00047

0.0022

0.00035

RH

0.033

0.016

0.065

 

0.000065

a Green.fac refers to the fraction of green land in each of the grid cells.

Urban.fac refers to the fractions of urban area in each of the grid cells. c Est denotes the estimated coe cients. d SE denotes the standard errors of the estimated coe cients. e Low95 denotes the lower bound of 95% posterior interval. f Up95 denotes the upper bound of 95% posterior interval.

b

a positive coe cient indicating a positive linear relationship with the PM 2.5 levels. The mean uncertainty of the variable PMSI 2.5 was less than 5 μ g/m 3 . Hence, due to the presence of PMSI 2.5 , an average uncertainty of approximately 5 μ g/m 3 was incorporated into the estimations considering its coe cient being close to 1 ( Table 1 ). Both PBL and terrain height were

4755

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759

Environmental Science & Technology

Article

negatively associated with PM 2.5 levels. Regarding the daily speci c random intercepts and slopes ( β 0 ( t ) and β 1 ( t ), respectively, in eq 5 and eq 6), they are larger in winter because the PM 2.5 concentrations were higher (Figure S3, SI). Model Comparisons and PMSI 2.5 Evaluations. In model tting, R 2 improved by 0.07 (from 0.66 to 0.73) when the variable PMSI 2.5 was considered in the model. In the 10-fold leave-10%-cities-out cross validation procedure, the R 2 improved from 0.48 ( Figure 3 b) to 0.61 (Figure 3c) by a

from 0.48 ( Figure 3 b) to 0.61 ( Figure 3 c) by a Figure 3.

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) + PMSI 2.5 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- lling was performed in these models.

large margin of 0.13. The RMSE also decreased by 3.46 μ g/m 3 , from 26.99 μ g/m 3 to 23.53 μ g/m 3 . In general, the model with PMSI 2.5 predicted PM 2.5 more accurately. The variable PMSI 2.5 explained more variance of PM 2.5 than AOD values by comparing the model s performance without using AOD values and that without PMSI 2.5 (Figure 3 a). In summary, PMSI 2.5 contains additional spatial information PM 2.5 that is not

captured by the spatiotemporal predictors, including AOD. When using the random leave-10%-monitors-out cross- validation method, the R 2 was 0.68 (Figure 3 d), which is similar to the R 2 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 PM 2.5 levels were calculated by averaging the estimated PM 2.5 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 PMSI 2.5 better characterized this belt-shape pollution zone ( Figure S4). Moreover, the full model with PMSI 2.5 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 PM 2.5 pairs. However, an estimation bias was apparent in the predictions even by the full model. The annual means of the observed PM 2.5 concentrations in the heavily polluted Hebei cities were approximately 120 μ g/m 3 . However, the highest estimated PM 2.5 concentrations (full model) were no larger than 100 μg/ m 3 ( Figure S4c ). Spatially, the estimated PM 2.5 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 PM 2.5 concentrations only when AOD values were available. The observed mean PM 2.5 levels with available AOD values were lower than the annual mean PM 2.5 levels ( Figure 2 a), which accounts for the underestimations. AOD Gap-Filling Evaluation. There were approximately 40000 missing AOD values in the grid cells with PM 2.5 monitors. Our missing AOD imputation method was eective at improving PM 2.5 predictions. In the model-tting procedure, the model overestimated AOD when the retrieved AOD values were low ( Figure 4a). Although the R 2 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 eld, we found that the spatial variations of the AOD values were well captured. There were almost no abnormal spatial patterns in

captured. There were almost no abnormal spatial patterns in Figure 4. (a) Scatterplots of the AOD

Figure 4. (a) Scatterplots of the AOD values tted by eq 1 and retrieved AOD values; (b) prediction performance using the reconstructed AOD with full model; (c) annual average AOD values with gap- lling.

4756

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759

Environmental Science & Technology

Article

Environmental Science & Technology Article Figure 5. Annual and seasonal mean estimations of the PM 2

Figure 5. Annual and seasonal mean estimations of the PM 2.5 concentrations ( μ g/m 3 ) using the full model and reconstructed AOD data set.

the daily AOD. When used in predicting PM 2.5 , the full model performed well with the reconstructed data set, giving an R 2 of 0.78, an NME of 0.27, and an RMSE 33.39 μ g/m 3 in the cross- validation experiment (Figure 4 b). 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 PM 2.5 enabled our model to leverage additional extra spatial information from PM 2.5 monitors. PM 2.5 Concentration Estimation. The model using the fullAOD data set predicted the seasonal and annual average of the PM 2.5 concentrations well ( Figure 5 ). The PM 2.5 concentrations were much higher in winter compared to those using the retrieve d AOD only. The mean PM 2.5 concentration in winter was approached 200 μ g/m 3 . The heavy pollution mainly occurred in the middle and southern Hebei province, the western Shandong province, Tianjin, and Beijing. The PM 2.5 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 PM 2.5 concentrations were generally lower than 40 μ g/m 3 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 PM 2.5 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 PM 2.5 level of nearly 50 μ g/m 3 . The successful prediction of this pollution hotspot among clean surroundings further demonstrated the model s e ectiveness. The PM 2.5 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 R 2 = 0.64 in the 10-fold cross validation method, while we obtained an R 2 = 0.61 by our stricter evaluation process that

4757

accounts for spatial clustering. They predicted the mean PM 2.5 concentrations in southern Hebei province at around 90 μ g/m 3 in 2013 and 130 μ g/m 3 in the winter. In contrast, for 2014, we predicted improved PM 2.5 levels to be at around 120 μ g/m 3 overall and 180 μ g/m 3 in the winter, which were closer to observations. Zheng et al. 27 evaluated their LME model in Beijing Tianjin Hebei area with an R 2 = 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 PM 2.5 concentrations well by using a correction factor. Xie et al. predicted PM 2.5 levels in Beijing, with an R 2 = 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 signi cantly under- estimated annual mean PM 2.5 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 PM 2.5 concentrations in North China. First, we used a Bayesian hierarchical framework to model the daily grid cell-speci c linear relationships between the AOD and PM 2.5 concentrations. Second, we used the spatial dependence in all the observed PM 2.5 levels by developing an interpolated PM 2.5 variable PMSI 2.5 . The new variable PMSI 2.5 can signi cantly improve the model s prediction performance. The R 2 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 PM 2.5 pollution maps with complete spatial and temporal coverage, which was shown to be useful for capturing the evolution of PM 2.5 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

Article

prediction performance. In our case, using a completely random, exhaustive leave-10%-monitors-out procedure led to an R 2 , NME, and RMSE of 0.68, 0.26, and 21.40 μ g/m 3 , 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 μ g/m 3 , 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 S1S6 ( 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 nancial 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 ocial 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).

REFERENCES

(1) Wang, L.; Wei, Z.; Yang, J.; Zhang, Y.; Zhang, F.; Su, J.; Meng, C.; Zhang, Q. The 2013 severe haze over southern Hebei, China:

model evaluation, source apportionment, and policy implications. Atmos. Chem. Phys. 2014 , 14 , 31513173. (2) Zhang, R.; Jing, J.; Tao, J.; Hsu, S.-C.; Wang, G.; Cao, J.; Lee, C.; Zhu, L.; Chen, Z.; Zhao, Y. Chemical characterization and source apportionment of PM 2.5 in Beijing: seasonal perspective. Atmos. Chem. Phys. 2013 , 13 (14), 7053 7074. (3) He, K.; Yang, F.; Ma, Y.; Zhang, Q.; Yao, X.; Chan, C. K.; Cadle, S.; Chan, T.; Mulawa, P. The characteristics of PM 2.5 in Beijing, China. Atmos. Environ. 2001 , 35 (29), 4959 4970. (4) Nel, A. Air pollution-related illness: effects of particles. Science 2005 , 308 (5723), 804 806. (5) Pope, C. A., III; Dockery, D. W. Health effects of fine particulate air pollution: lines that connect. J. Air Waste Manage. Assoc. 2006 , 56 (6), 709 742. (6) Lin, J.; Nielsen, C. P.; Zhao, Y.; Lei, Y.; Liu, Y.; McElroy, M. B. Recent changes in particulate air pollution over China observed from

4758

space and the ground: effectiveness of emission control. Environ. Sci. Technol. 2010 , 44 (20), 7771 7776. (7) Van Donkelaar, A.; Martin, R. V.; Levy, R. C.; da Silva, A. M.;

Krzyzanowski, M.; Chubarova, N. E.; Semutnikova, E.; Cohen, A. J. Satellite-based estimates of ground-level fine particulate matter during extreme events: A case study of the Moscow fires in 2010. Atmos. Environ. 2011 , 45 (34), 62256232. (8) Van Donkelaar, A.; Martin, R. V.; Park, R. J., Estimating ground- level PM 2.5 using aerosol optical depth determined from satellite remote sensing. J. Geophys. Res. 2006 , 111 , (D21). 10.1029/

(9) Kahn, R.; Banerjee, P.; McDonald, D.; Diner, D. J. Sensitivity of multiangle imaging to aerosol optical depth and to pure-particle size distribution and composition over ocean. J. Geophys. Res. 1998 , 103 (D24), 32195 32213. (10) Liu, Y.; Sarnat, J. A.; Kilaru, V.; Jacob, D. J.; Koutrakis, P. Estimating ground-level PM 2.5 in the eastern United States using satellite remote sensing. Environ. Sci. Technol. 2005 , 39 (9), 3269

3278.

(11) Wang, J.; Christopher, S. A., Intercomparison between satellite- derived aerosol optical thickness and PM 2.5 mass: implications for air quality studies. Geophys. Res. Lett. 2003 , 30 , (21). 10.1029/

(12) Lee, H.; Liu, Y.; Coull, B.; Schwartz, J.; Koutrakis, P. A novel calibration approach of MODIS AOD data to predict PM 2.5 concentrations. Atmos. Chem. Phys. 2011 , 11 (15), 7991 8002. (13) Xie, Y.; Wang, Y.; Zhang, K.; Dong, W.; Lv, B.; Bai, Y. Daily estimation of ground-level PM 2.5 concentrations over Beijing using 3 km resolution MODIS AOD. Environ. Sci. Technol. 2015 , 49, 12280. (14) Ma, Z.; Hu, X.; Huang, L.; Bi, J.; Liu, Y. Estimating ground-level PM 2.5 in China using satellite remote sensing. Environ. Sci. Technol. 2014 , 48 (13), 7436 7444. (15) Song, W.; Jia, H.; Huang, J.; Zhang, Y. A satellite-based geographically weighted regression model for regional PM 2.5 estimation over the Pearl River Delta region in China. Remote Sensing of Environment 2014 , 154 , 17. (16) Lin, C.; Li, Y.; Yuan, Z.; Lau, A. K.; Li, C.; Fung, J. C. Using satellite remote sensing data to estimate the high-resolution distribution of ground-level PM 2.5 . Remote Sensing of Environment 2015 , 156 , 117 128. (17) Zheng, Y.; Liu, F.; Hsieh, H.-P. In U-Air: When urban air quality inference meets big data. Proceedings of the 19th ACM SIGKDD international conference on Knowledge discovery and data mining, 2013; ACM, 2013; pp 14361444. (18) Lary, D. J.; Faruque, F. S.; Malakar, N.; Moore, A.; Roscoe, B.;

Adams, Z. L.; Eggelston, Y. Estimating the global abundance of ground level presence of particulate matter (PM 2.5 ). Geospatial Health 2014, 8 (3), 611 630. (19) Geng, G.; Zhang, Q.; Martin, R. V.; van Donkelaar, A.; Huo, H.; Che, H.; Lin, J.; He, K. Estimating long-term PM 2.5 concentrations in China using satellite-based aerosol optical depth and a chemical transport model. Remote Sensing of Environment 2015 , 166 , 262 270. (20) Chang, H. H.; Hu, X.; Liu, Y. Calibrating MODIS aerosol optical depth for predicting daily PM 2.5 concentrations via statistical downscaling. J. Exposure Sci. Environ. Epidemiol. 2014 , 24 (4), 398

404.

(21) Levy, R. C.; Remer, L. A.; Kleidman, R. G.; Mattoo, S.; Ichoku, C.; Kahn, R.; Eck, T. Global evaluation of the Collection 5 MODIS dark-target aerosol products over land. Atmos. Chem. Phys. 2010 , 10 (21), 10399 10420. (22) Tao, M.; Chen, L.; Su, L.; Tao, J., Satellite observation of regional haze pollution over the North China Plain. J. Geophys. Res. 2012 , 117 , (D12). 10.1029/2012JD017915 (23) Engel-Cox, J. A.; Holloman, C. H.; Coutant, B. W.; Hoff, R. M. Qualitative and quantitative evaluation of MODIS satellite sensor data for regional and urban scale air quality. Atmos. Environ. 2004 , 38 (16),

2495 2509.

(24) Kloog, I.; Chudnovsky, A. A.; Just, A. C.; Nordio, F.; Koutrakis,

P.; Coull, B. A.; Lyapustin, A.; Wang, Y.; Schwartz, J. A new hybrid

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759

Environmental Science & Technology

Article

spatio-temporal model for es timating daily multi-year PM 2.5 concentrations across northeastern USA using high resolution aerosol optical depth data. Atmos. Environ. 2014 , 95, 581 590. (25) Kloog, I.; Koutrakis, P.; Coull, B. A.; Lee, H. J.; Schwartz, J. Assessing temporally and spatially resolved PM 2.5 exposures for epidemiological studies using satellite aerosol optical depth measure- ments. Atmos. Environ. 2011 , 45 (35), 6267 6275. (26) Van Donkelaar, A.; Martin, R. V.; Pasch, A. N.; Szykman, J. J.; Zhang, L.; Wang, Y. X.; Chen, D. Improving the accuracy of daily satellite-derived ground-level fine aerosol concentration estimates for North America. Environ. Sci. Technol. 2012 , 46 (21), 11971 11978. (27) Zheng, Y.; Zhang, Q.; Liu, Y.; Geng, G.; He, K. Estimating ground-level PM 2.5 concentrations over three megalopolises in China using satellite-derived aerosol optical depth measurements. Atmos. Environ. 2016 , 124 , 232 242. (28) Just, A. C.; Wright, R. O.; Schwartz, J.; Coull, B. A.; Baccarelli,

A. A.; Tellez-Rojo, M. M.; Moody, E.; Wang, Y.; Lyapustin, A.; Kloog, I. Using high-resolution satellite aerosol optical depth to estimate daily PM 2.5 geographical distribution in Mexico City. Environ. Sci. Technol. 2015 , 49 (14), 8576 8584. (29) Oliver, M. A.; Webster, R. Kriging: a method of interpolation for geographical information systems. International Journal of Geographical Information System 1990 , 4 (3), 313 332. (30) Zhang, Q.; Streets, D. G.; Carmichael, G. R.; He, K.; Huo, H.; Kannari, A.; Klimont, Z.; Park, I.; Reddy, S.; Fu, J. Asian emissions in 2006 for the NASA INTEX-B mission. Atmos. Chem. Phys. 2009 , 9 (14), 5131 5153. (31) Lv, B.; Zhang, B.; Bai, Y. A systematic analysis of PM 2.5 in Beijing and its sources from 2000 to 2012. Atmos. Environ. 2016 , 124 , 98108. (32) Yang, L.; Cheng, S.; Wang, X.; Nie, W.; Xu, P.; Gao, X.; Yuan, C.; Wang, W. Source identification and health impact of PM 2.5 in a heavily polluted urban atmosphere in China. Atmos. Environ. 2013 , 75 ,

265 269.

(33) Madaniyazi, L.; Nagashima, T.; Guo, Y.; Yu, W.; Tong, S. Projecting Fine Particulate Matter-related Mortality in East China. Environ. Sci. Technol. 2015 , 49 (18), 11141 11150. (34) Jiang, J.; Zhou, W.; Cheng, Z.; Wang, S.; He, K.; Hao, J. Particulate matter distributions in China during a winter period with frequent pollution episodes (January 2013). Aerosol Air Qual. Res. 2015 , 15 (2), 494. (35) Remer, L. A.; Kaufman, Y.; Tanre ,́ D.; Mattoo, S.; Chu, D.; Martins, J. V.; Li, R.-R.; Ichoku, C.; Levy, R.; Kleidman, R. The MODIS aerosol algorithm, products, and validation. J. Atmos. Sci. 2005 , 62 (4), 947 973. (36) Gryparis, A.; Paciorek, C. J.; Zeka, A.; Schwartz, J.; Coull, B. A. Measurement error caused by spatial misalignment in environmental epidemiology. Biostatistics 2009 , 10 (2), 258 274. (37) Szpiro, A. A.; Paciorek, C. J.; Sheppard, L. Does more accurate exposure prediction necessarily improve health effect estimates? Epidemiology (Cambridge, Mass.) 2011 , 22 (5), 680.

4759

DOI: 10.1021/acs.est.5b05940 Environ. Sci. Technol. 2016, 50, 4752 4759