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Environmental Science & Technology Letters is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036

Energy Golden Triangle, Northwest China

Yanjie Shen, Xiaodong Zhang, Jeffrey Robert Brook, Tao Huang, Yuan Zhao, Hong Gao, and Jianmin Ma

Environ. Sci. Technol. Lett., Just Accepted Manuscript • DOI: 10.1021/acs.estlett.6b00182 • Publication Date (Web): 07 Jun 2016 Downloaded from http://pubs.acs.org on June 7, 2016

Just Accepted

“Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

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Satellite Remote Sensing Of Air Quality In The Energy Golden Triangle In 1

Northwest China 2

Yanjie Shen1, Xiaodong Zhang1, Jeffrey R. Brook2, Tao Huang1, Yuan Zhao1,Hong 3

Gao1*, Jianmin Ma1,3*

4

Affiliation:

5

1Key Laboratory for Environmental Pollution Prediction and Control, Gansu Province, 6

College of Earth and Environmental Sciences, Lanzhou University, Lanzhou 730000, 7

China 8

2Air Quality Research Division, Atmospheric Science and Technology Directorate, 9

Environment Canada, 4905 Dufferin St., Toronto, Ontario, Canada M3H 5T4 10

3CAS Center for Excellence in Tibetan Plateau Earth Sciences, Beijing 100101, China 11

12

*Corresponding author: Jianmin Ma, Hong Gao 13

Tel: +86 15293166921, fax: +86-931-8911843, email: [email protected]14

[email protected] 15

Word account: 2632; Figures: 3 16

Abstract 17

This article presents the first assessment of air quality in the Energy Golden Triangle 18

(EGT) in northwest China. Using the planetary boundary layer (PBL) column density 19

(PCD) of SO2 and the tropospheric column density (TCD) of NO2 retrieved from the 20

Ozone Monitoring Instrument (OMI), we show that the column densities of both SO2

21

and NO2 exhibit an increasing trend from 2005 to 2014 in the Ningdong energy and 22

chemical industrial base (NECIB) within the EGT,in contrast to the rapid and 23

widespread decrease of SO2 emissions in northern China. This is largely attributed to 24

the rapid development of the energy industry in this region. It is expected that SO2

25

and NO2 emitted from the EGT would increasingly contribute to the totalemissions of 26

these two air pollutants in northern China.

27 28 29 30 31 32 33

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TOC Art 34

35

1. Introduction 36

Fossil fuel industries are major sources of air pollutants,1 Due to rapid 37

industrialization and urbanization over the past decades, the increasing demands for 38

energy supply in China have imposed serious adverse effects on air quality,

39

particularly in northern China where most of the heavy industry is located. Under the 40

national strategy for energy development and safety during the 21st century, oil, 41

natural gas, coal mining industries,and thermal power generators have been relocated 42

towards energy-abundant northwest China,2,3 Consequently, the Energy Golden 43

Triangle (EGT), which is located in this region (Figure S1 of Supporting Information, 44

SI), is now the largest new energy and chemical industry base in China providing 25%

45

of the country’s energy production,4 The total fossil fuel resources in the EGT are 46

equivalent to 2 trillion tons of standard coal and account for approximately 40% of the 47

(4)

country's total. In particular, the Ningdong energy and chemical industrial base 48

(NECIB) in the Ningxia Hui Autonomous Region,5 a sub-region in the EGT (Figure 49

S1), is a nationally prioritized region for the promotion of the development of 50

large-scale coal mining bases, thermal power generation, and the chemical industry.

51

To guarantee national energy security and to promote the regional economy,the EGT 52

energy program has been accelerating since 2010 reaching the national goals for coal 53

production of 1.45×109 tons, oil output of 5.4×107 tons, and natural gas production of 54

5.5×1010 m3 in 2015.4 ,6Given the low annual precipitation ranging from 100 mm to 55

400 mm and sparse vegetation coverage,7,8 the poor ecological environments in the 56

EGT region are uniquely susceptible to atmospheric pollution. It is hypothesized that 57

the increased release of pollutants to the air, water and land that is associated with 58

rapid development in the EGT will have a considerable impact on the local 59

environment. These effects can also be expected to extend to the downstream regions 60

in eastern China via atmospheric transport and river flows. In particular, the EGT 61

region is located in the upper reaches of the Yellow River, the second largest river in 62

China, which passes through the EGT and has been the main source of water supply 63

not only to local industries, but also to a vast region of eastern and central China.

64

Knowledge of the magnitude and extent of the environmental contamination and 65

impact associated with EGT development is very limited. No detailed air quality 66

monitoring data are available and the limited local government reports and air quality 67

assessments indicate that air quality in the EGT has been improving over the past 68

decade. These assessments state that levels of most criteria air pollutants were well 69

(5)

below the national standard.5,9 Here we attempt to independently assess the air quality 70

in the NECIB and EGT using satellite remote sensing data to quantify the influence of 71

the rapid development in the EGT on the local environment since 2005. Through the 72

use of satellite-based observations, it is possible to obtain valuable information on 73

emissions, spatial-temporal patterns, and annual trends of many air contaminants10-12. 74

In particular, air quality remote sensing with relatively high spatial resolution has 75

been improved rapidly in the last several years. Notably, the Ozone Monitoring 76

Instrument (OMI) on the NASA EOS Aura platform provides daily global coverage in 77

combination with small ground pixel sizes (nominally 13 × 24 km2 at nadir, 78

minimum 13 × 12 km2 at nadir),12-15 and the Infrared Atmospheric Sounding 79

Interferometer.15,16 This article presents the satellite retrieved column densities of 80

sulfur dioxide (SO2) and nitrogen dioxide (NO2) as well as their trends from 2005 to 81

2014 over the EGT and NECIB with a high spatial resolution, aiming to fill critical 82

knowledge gaps and understand air quality in the EGT given the shifting energy base 83

in northern China. Awareness of the implications of these large scale national policies 84

are important for assessing and minimizing impacts.

85

2. Materials and Methods 86

The OMI-derived PCD ( DU) of SO2 and TCD (1015 molec cm-2) of NO2 with a fine 87

spatial and temporal resolution were collected from the NASA EOS and KNMI 88

(Koninklijk Nederlands Meteorologisch Instituut), respectively.15,18 The operational 89

OMI PBL data are processed using the highly sensitive band residual difference (BRD) 90

algorithm to facilitate the acquisition of information on near-surface SO2 emission16. 91

(6)

The NO2 vertical column densities are obtained using a differential optical absorption 92

spectroscopy (DOAS) algorithm that converts NO2 slant column densities to vertical 93

columns.19,20 The SO2 PCD and NO2 TCD have been validated against their respective 94

monitored air concentrations in northern China.14,20 In the present study, the 95

OMI-retrieved column densities of SO2 and NO2 have been compared with the 96

available daily and monthly ambient air concentration data of these two chemicals at 97

official air quality monitoring stations and in the China National Environmental 98

Monitoring Center (http://106.37.208.233:20035/) near the central NECIB region.

99

Details of the comparisons are presented in the SI (text and Figures S2 and S3).

100

Two emission inventories for SO2 and NOx (nitrogen dioxide, NOx=NO+NO2 101

where NO is nitric oxide) are available in China. The first one covers East Asia with 102

gridded emission data before 2006.21 The other provides gridded SO2 and NOx 103

emission data from four emission sectors (industry, residential, power generation, and 104

transportation) for every two years from 2008 to 2012.22 Figures S4 and S5 display 105

the SO2 and NOx annual emissions from different emission sectors in 2008, 2010, and 106

2012,22 averaged over the NECIB and over a selected region of northern China (see 107

below for description of this region).

108

3. Results and Discussion 109

3.1 OMI-retrieved SO2 and NO2 in EGT and NECIB 110

Figure 1 shows the spatial distribution of SO2 PCD and NO2 TCD over the EGT and 111

four bordering provinces (inner map), averaged over 2005-2014 at a 0.25°×0.25°

112

latitude/longitude resolution. Higher SO2 PCDs (Figure 1a) and NO2 TCDs (Figure 113

(7)

1b) can clearly be observed in Ningdong (Yinchuan), Erdos, and the north of Yulin 114

(also seeing Figure S1). The higher 2005-2014 mean SO2 PCD and NO2 TCD extend 115

from the central NECIB region to Shizuishan in Ningxia and Wuhai in Inner 116

Mongolia. Wuhai and Shizuishan are traditional coal mining areas in northwest China.

117

The energy industries in these two regions have rapidly expanded since the early 118

2000s to provide raw coal to the Ningdong chemical and thermal power industries.

119

Due to SO2 emissions from coal mining industry, the daily ambient air 120

concentrations of SO2 in Wuhai were considerably higher than in Yinchuan (Figure 121

S6a). Conversely there were relatively higher levels of NO2 over Yinchuan compared 122

to Wuhai (Figure S6b), which was likely due to the larger number of motor vehicles 123

in Yinchuan (population 2.1 million) compared with that in Wuhai (population 0.56 124

million).

125

Since the coal mining and power generation industries in the NECIB sub-area 126

of the EGT have been experiencing the fastest expansion in recent several years, we 127

compared the monthly mean PCD of SO2,averaged over the NECIB with northern 128

China (Figure 2a, the NECIB and northern China are marked in Figure S1), where 129

air pollution levels, especially fine particulate matter (PM2.5), have received 130

significant international attention during the past three decades. Here we include in 131

northern China two mega cities (Beijing, Tianjin) and three provinces ( Liaoning, 132

Shangdong, and Hebei), which make up one of China's most populated and 133

industrialized regions. This region will be referred to as the northern China region 134

hereafter. Result from 2005 to 2014 shown in Figure 2a indicate that the SO2 PCDs in 135

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the northern China region were much higher than those in the NECIB before 2011.

136

However, since 2011, the monthly SO2 PCDs over the NECIB have been similar to 137

and higher than the northern China region in magnitude. This is attributed to 138

decreasing SO2 emissions in the northern China region and increasing emissions in 139

the NECIB. The strong decline of SO2 emission from power generation after 2006 in 140

the northern China region (Figure S4c) was a result of regulations to reduce SO2

141

emission in this region,21,22 including application of flue-gas desulfurization, and the 142

relocation of oil and coal mining industries as well as thermal power generations to 143

northwest China.23,24 144

The 2005-2014 mean SO2 PCDs and NO2 TCDs are generally consistent with the 145

mean SO2 and NOx emissions over 2008, 2010, and 201222 in the same region, as 146

shown in Figure 2b, c and Figure S7. The annual SO2 emissions from different 147

emission sectors averaged over the NECIB and the northern China region are 148

illustrated in Figure S4. Although the emissions from the residential and 149

transportation sectors in the northern China region were considerably higher than 150

those averaged over the NECIB in the later 2000s because of much higher population 151

density in the northern China region (Figure S4b and d), the emissions from these 152

two sectors accounted for less than 10% of the total SO2 emission. In contrast to the 153

continuously declining SO2 emission in the northern China region, for the major 154

emission sectors of industry and power generation (Figures 2a, b and Figure S4a, c), 155

the SO2 emissions averaged over the NECIB increased after 2006 and became much 156

higher than the domain-averaged emissions from power plants over the northern 157

(9)

China region, in line with the SO2 PCD changes, as illustrated in Figure 2a and b. As 158

a result, the domain-averaged total SO2 emission over the NECIB has exceeded the 159

mean emission averaged over the northern China region in 2012 (Figure 2b and S4e).

160

Similarly, the domain-averaged NOx emissions from power generation in the NECIB 161

increased rapidly and was 2.2 times higher than the emissions averaged over the 162

northern China region in 2012 (Figure 2c and S5). Although the mean NOx emissions 163

in the NECIB from the other three emission sectors were still lower than those 164

averaged over the northern China region, the total NOx emission from all emissions 165

sectors in the NECIB increased more rapidly than those averaged over the northern 166

China region due to markedly increasing NOx emission from power generation in the 167

NECIB (Figure S5e).

168

Figure S8a and b further compare the annual emissions of SO2 and NOx from 169

power generation21 with annually averaged column densities of SO2 and NO2

170

retrieved from OMI over the EGT in 2008, 2010, and 2012, showing agreement 171

between the emissions and column densities of SO2 and NO2. Knowing that the 172

thermal power industry contributed primarily to the NECIB and EGT development6, 173

the association between SO2 and NOx emission patterns and the column densities of 174

these two criteria air pollutants confirmed that the coal mining and thermal power 175

industry in this region likely played a significant role worsening local air quality.

176

3.2 Trends of OMI-retrieved column densities of SO2 and NO2

177

Table S1 presents the non-parametric Mann-Kendall statistical test (Z)25 and Sen’s 178

estimated slopes (Q)26 for the monthly mean SO2 PCD and NO2 TCD in the NECIB, 179

(10)

EGT, and the northern China region. The statistically significant declining trend of 180

SO2 PCD in the northern China region is indicated by the negative Z value (-6.698, 181

p<0.01) for the time series of the monthly mean SO2 PCDs, in line with its linear 182

trend in this region (Figure 2a). The SO2 PCD in the EGT also exhibits a decreasing 183

trend, characterized by the negative Z value of -3.62 (p<0.01) and the negative linear 184

trend (slope=-0.0002, R2=0.089, p=0.0009). While the positive Z value (1.626) and 185

the slope of the linear trend (slope=0.0002, R2=0.022, p=0.1013, Figure 2a) of the 186

monthly mean SO2 PCD in the NECIB suggests an increasing trend, , these positive 187

trends are not statistically significant using the p<0.05 and |Z|>Z1-α/2=1.96 criteria 188

(Table S1). Accordingly, Sen's slope Q revealed the faster decreasing rate of the 189

monthly SO2 PCD time series in the northern China region (-0.0019) as compared 190

with that in the EGT (-0.0002), whereas a positive Sen's slope Q for the SO2 PCD 191

(0.0002) was estimated in the NECIB.

192

Figure 3a shows the gridded trends of the annual mean SO2 PCDs (DU) from 193

2005 to 2014 across the four provinces (Figure 1 inner map) where the EGT is 194

located. These trends were estimated from the linear regression of SO2 PCDs against 195

the time sequence from 2005 to 2014 for each grid square. Overall the SO2 PCDs 196

exhibited negative trends in the EGT. We would expect the decline of SO2 emissions 197

in the EGT from 2012 onward. Conversely, as shown in Figures 2a and 3a, the SO2 198

PCDs increased in the NECIB during 2005-2014, in agreement with the increasing 199

SO2 emissions in this sub-region in the EGT (Figures 2b and S4), particularly from 200

power generation and industry. The increasing SO2 emission in the NECIB can also 201

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offset the declining emission over the EGT.

202

Figure 3b illustrates the spatial pattern in the trend of SO2 PCDs for the same 203

period but for the EGT only. The positive trend of SO2 PCDs can now be more clearly 204

seen to only be over the NECIB,in contrast to the decline of SO2 emissions in the 205

northern China region and other EGT regions. Among the three areas in the EGT, 206

intensive coal and oil mining in Yulin and Ordos was initiated in the early 1990s and 207

has slowed down considerably since 2008 partly due to decreasing demands to raw 208

coal in China,27 whereas the energy industry in the NECIB has been accelerating since 209

the mid-2000s under strong support from provincial and central governments28 to 210

provide electric power to eastern China. These geographic patterns in socioeconomic 211

change are clearly reflected in the PCD values (Figure 3b). Compared with SO2, the 212

NO2 TCDs over the NECIB did not exhibit a declining trend after 2008 (Figure S3).

213

The measured annual mean NO2 air concentrations in Yinchuan (40 km west of the 214

NECIB) decreased from 2005 to 2008 and increased thereafter, showing an overall 215

increasing trend, somewhat consistent with NO2 column densities. This is attributable 216

to more difficulties in the control of NO2 emissions from industry, power generation, 217

and transportation. Differing from the SO2 measurements (Figure S6a), Figure S6b 218

shows the relatively higher NO2 levels in Yinchuan than in Wuhai in most cases, 219

which is likely due to the proximity of Yinchuan to the NECIB and more motor 220

vehicles in Yinchuan.

221

Following the shift of energy industries, fossil fuel mining, and chemical 222

industries to northwest China and stricter emission control regulations in the 223

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traditional industrialized regions in China, significant emission reductions are 224

reported for the northern China region and these are being reflected in the observed 225

vertical column densities of SO2. It is anticipated that such reductions will continue in 226

the coming years. In localized areas of the EGT/NECIB, where emission activities 227

have been expanding, there have been modest increases in SO2, particularly since 228

2010. As a national energy base for the 21st century, the development of the 229

EGT/NECIB also is projected to continue for many years. Considering the potentially 230

fragile ecological environments in this area, the impact in the EGT (NECIB) due to 231

degraded air quality and higher levels of related contaminants on a range of 232

environmental media needs to be carefully monitored. More investigations are 233

required to fill knowledge gaps in the emissions of toxic chemicals, greenhouse gases, 234

and the responses of eco-sensitive environments in order to minimize future impacts.

235

ASSOCIATED CONTENT 236

Supporting Information. Additional material as noted in the text. This material is 237

available free of charge via t http://pubs.acs.org.

238

ACKNOWLEDGMENTS 239

This work is supported by the National Natural Science Foundation of China through 240

grants 41371478 and 41371453. We acknowledge the free use of SO2 PBL column 241

density and tropospheric NO2 column density data from OMI,and SO2 and NOx

242

emission data from Multi-resolution Emission Inventory for China (MEIC). We thank 243

Dr. S. Venkatesh for his helpful comments and edits to the manuscript.

244

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Figure captions 328

Figure 1. OMI-retrieved column densities of SO2 and NO2 averaged from 2005 to 329

2014 in the EGT and four bordering provinces (Inner Mongolia, Shaanxi, Ningxia, 330

and Gansu) at the spatial resolution of 0.25o×0.25o lat/lon. (a) Gridded annual mean 331

SO2 PBL column density (DU), and (b) NO2 tropospheric column density (1015 molec 332

cm-2). The EGT is encircled by Ordos, Yulin, NECIB, and includes their respective 333

extended areas (coal mine, power generators, and chemical industry). The inner map 334

on the up-left corner highlights the location of the four bordering provinces of the 335

EGT relative to all of China.

336

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Figure 2. (a) Monthly mean OMI SO2 PBL column density (DU) from 2005-2014 337

averaged over the northern China region (the one of China's economic engine) and the 338

NECIB (Figure S1). Blue and red dashed lines in Figure 2a represent linear trend of 339

SO2 PCDs in the NECIB (slope=0.0002, R2=0.022, p=0.1013) and the northern China 340

region (slope=-0.002, R2=0.328, p=0.0003), respectively; (b) annual mean SO2 PCD 341

and its emissions (ton yr-1) over the NECIB in 2008, 2010, and 2012; (c) annual mean 342

NO2 TCD and NOx emissions (ton yr-1) over the NECIB in 2008, 2010, and 2012.

343

Figure 3. Linear trends (slopes) of OMI retrieved SO2 PCD (DU) across (a) 4 344

provinces (Inner Mongolia, Shaanxi, Ningxia, and Gansu as shown in Figure 1), and 345

(b) EGT.

346 347

348

Figure 1 349

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350

Figure 2.

351

352

Figure 3 353

. 354

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