Environmental Pollution 258 (2020) 113659

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Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Spatio-temporal patterns of air pollution in China from 2015 to 2018

and implications for health risks*
Mireadili Kuerban a, Yizaitiguli Waili b, Fan Fan a, Ye Liu a, Wei Qin a, Anthony J. Dore c,
Jingjing Peng a, Wen Xu a, *, Fusuo Zhang a
a
College of Resources and Environmental Sciences, National Academy of Agriculture Green Development, Key Laboratory of Plant-Soil Interactions of MOE,
China Agricultural University, Beijing, 100193, China
b
College of Resources and Environmental Science, Xinjiang University, Urumqi, 830046, China
c
Centre for Ecology and Hydrology, Edinburgh, Bush Estate, Penicuik, Midlothian, EH26 0QB, UK

a r t i c l e i n f o a b s t r a c t

Article history: China has been seriously affected by particulate matter (PM) and gaseous pollutants in the atmosphere.
Received 25 May 2019 In this study, we systematically analyse the spatio-temporal patterns of PM2.5, PM10, SO2, CO, NO2, and O3
Received in revised form and the associated health risks, using data collected from 1498 national air quality monitoring sites. An
19 November 2019
analysis of the averaged data from all the sites indicated that, from 2015 to 2018, annual mean con-
Accepted 20 November 2019
centrations of PM2.5, PM10, SO2 and CO declined by 3.2 mg m
3, 3.7 mg m
3, 3.9 mg m
3, and 0.1 mg m
3,
Available online 23 November 2019
respectively. In contrast, those of NO2 and O3 increased at rates of 0.4 and 3.1 mg m
3, respectively. Except
for O3, the annual mean concentrations of all pollutants were generally the highest in North China and
Keywords:
Air pollution
lowest in the Tibetan Plateau. The concentrations were generally higher in the north of the country than
Emission control in the south. In all regions of China, the pollutant concentrations were the highest in winter and lowest in
PM2.5 summer, except for O3, which showed an opposite seasonal pattern. Overall, the seasonal mean con-
Ozone centrations of all the pollutants (except for O3) significantly decreased between the same seasons in 2018
Human health and 2015, whereas the seasonal mean O3 concentrations generally significantly increased, and/or
China remained at stable levels in all four seasons except for winter. Diurnal variations of all pollutants (except
for O3) exhibited a bimodal pattern with peaks between 8:00 and 11:00 a.m. and 9:00 and 12:00 p.m.,
whereas O3 exhibited a unimodal pattern with maximum values between 5:00 and 7:00 p.m. No sig-
nificant differences in the daily mean concentrations of all pollutants were found between weekdays and
weekends in all regions, except for PM2.5 and PM10 in Northeast China. In Northwest China and Southeast
China, PM2.5 showed stronger correlations with NO2 relative to SO2, suggesting that NOx emission control
may be more effective than SO2 emission control for alleviating PM2.5 formation. Compared with 2015,
the total PM2.5-attributable mortality, number of respiratory and cardiovascular diseases, and incidence
of chronic bronchitis decreased overall by 23.4%e26.9% in 2018. In contrast, for O3-attributable deaths,
there was an increase of 18.9%. Our study not only improves the understanding of the spatial and
temporal patterns of air pollutants in China, but also highlights that synchronous control of PM2.5 and O3
pollution should be implemented to achieve dual benefits in protecting human health.
© 2019 Elsevier Ltd. All rights reserved.

1. Introduction growing health risk is mainly growing because of an increase in

Air pollution has become one of the top environmental issues in
China, and threatens both human health (Cohen et al., 2017) and
the natural environment (Li et al., 2017a, b; Yue et al., 2017). The
*
This paper has been recommended for acceptance by Eddy Y. Zeng.
* Corresponding author.
E-mail addresses: hi.xuwen@163.com, wenxu@cau.edu.cn (W. Xu).
pollution caused by particulate matter (PM) pollution, such as
PM2.5 (particles with an aerodynamic diameter of 2.5 mm) and
PM10 (particles with an aerodynamic diameter of 10 mm) (Lu et al.,
2017; Xie et al., 2016). Globally, 3.2 million people died from air
pollution in 2010; of those, 1.3 million people were from China
(Lelieveld et al., 2015). Gaseous pollutants such as CO, SO2, NO2, and
O3, have significant impacts on human health and the well-being of
natural ecosystems (Heal et al., 2012, 2013; Liu et al., 2016, 2018a,

https://doi.org/10.1016/j.envpol.2019.113659
0269-7491/© 2019 Elsevier Ltd. All rights reserved.
2 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
b). For example, PM2.5-attributable premature mortalities in China
totalled 1.37 million, of which 50%, 28%, 9%, and 12% could be
attributed to stroke, ischemic heart disease, lung cancer, and
chronic obstructive pulmonary disease, respectively (Liu et al.,
2016). Liu et al. (2018a, b) showed that an increase of 1 mg m
3
in the average CO concentrations can cause significant increases in
mortality from cardiovascular diseases (1.12%), coronary heart
disease (1.75%) and stroke (0.88%). There is solid evidence indi-
cating the importance of improving air quality for human health
(Lai et al., 2013; Zheng et al., 2015; Liu et al., 2016; Xie et al., 2016;
Lu et al., 2018). For example, Zheng et al. (2015) reported that the
average total mortality in urban Beijing caused by PM2.5 was
approximately 5100 individuals each year from 2001 to 2012. At a
regional scale, Xie et al. (2016) demonstrated that premature
deaths attributed to ambient PM2.5 grew 42% in China from 2000 to
2010. As for O3, Lu et al. (2018) showed that on a regional scale, the
exposure of humans to O3 is higher in China than in other devel-
oped countries such as the US, Europe, Japan, and South Korea.
However, updated information on the impact of air quality im-
provements on human health in recent years is very limited, owing
to the lack of long-term monitoring of PM2.5 and O3.
To mitigate air pollution, the Chinese government has imposed
stringent air quality standards and strengthened emission controls,
and has also introduced a nationwide air quality monitoring
network with hourly measurements of major atmospheric pollut-
ants (PM2.5, PM10, SO2, NO2, CO, and O3). Various studies have
focused on the spatio-temporal variations of air pollutants on na-
tional and regional scales (Chai et al., 2014; Wang et al., 2014; Wang
et al., 2015; Zhang and Cao, 2015; Liu et al., 2017a; Zhao et al., 2016).
Nevertheless, most of these studies were limited to either a single
city and/or to a short-term period of investigation. For instance, an
analysis of the spatio-temporal variation of six air pollutants in 31
provincial capital cities between March 2013 and February 2014
was reported by Wang et al. (2014), and later by Zhao et al. (2016).
Thus far, very little attention has been paid to annual, seasonal,
monthly, and daily variations of ambient pollutants based on
analysis of a long-term dataset, on the correlations between air
pollutants in different regions, or on variations in weekday/week-
end concentrations. Advancing our understanding of the spatial
and annual variations of air pollutants in different regions of China,
as well as the correlations among different pollutants, is helpful for
supporting the implementation of control measures for air pollu-
tion, and the establishment of region-oriented air quality stan-
dards. Investigation of the diurnal patterns of air pollutant
concentrations and the differences in behaviour between weekdays
and the weekend is also important as it aids in the understanding of
specific emission sources and pollutant formation mechanisms
(Zheng et al., 2014). In summary, it is imperative to obtain detailed
information, based on long-term and continuous observation of
airborne pollutant trends and their variability.
The objectives of the present study are: (1) to explore the spatial
and temporal (annual, monthly, seasonal and diurnal) patterns of
six air pollutants (PM2.5, PM10, CO, SO2, NO2, and O3) in different
regions of China; (2) to detect the regional weekday/weekend air
concentration differences, as well as the correlations among the six
pollutants, and (3) to investigate the impacts of PM2.5 and O3 on
human health across China. We used a 4-year (2015e2018) dataset
of the hourly concentrations of the aforementioned six critical air
pollutants, which was officially released from 1498 monitoring
sites (located in 367 cities and counties) across China. To the best of
our knowledge, this is the first time that such a large dataset has
been used to systematically probe the variations in characteristics
of the six critical air pollutants, and their associated health effects in
China.
2. Data and methods
2.1. Data collection
The hourly mean concentrations of PM2.5, PM10, CO, O3, NO2, and
SO2 were measured at 1498 sites in 367 cities and counties between
1 January 2015 and 23 December 2018, and were acquired from a
large network operated by the China National Environmental
Monitoring Center (CNEMC) (http://106.37.208.233:20035/). The
location of all 1498 monitoring sites is shown in Fig. S1 in the
Supplement. Information regarding the sampling instruments,
sampling method, and data quality control for the six measured
pollutants is provided in Text S1. Although the sampling methods
were not uniform across the sites, other studies have confirmed
that the ambient concentrations of particulate matter measured
using the different methods were comparable (Chung et al., 2001;
Schwab et al., 2006). In addition, other previous work has
demonstrated that the quality and validity of the officially-released
data are statistically reliable (Xie et al., 2015). A dataset similar to
the one chosen for this study has been utilised in previous studies
(Yin et al., 2016; Zhou et al., 2016). Furthermore, to make a com-
parison between China and other countries, we collected the
available air quality datasets of the annual concentration of PM2.5,
PM10, NO2, and SO2 from 2015 to 2016 for Europe (https://projects.
nilu.no//ccc/reports.html), and from 2015 to 2017 for East Asia
(https://monitoring.eanet.asia/document/public/index) and the US
(https://www.epa.gov/outdoor-air-quality-data/air-quality-
statistics-report). The annual mean concentrations of the four
pollutants at the corresponding monitoring sites in those three
countries are provided in Table S1 in the Supplement.
2.2. Analytical methods
To investigate the annual, seasonal, monthly, and daily varia-
tions of the six air pollutants, as well as their weekday and weekend
differences, the 1498 monitoring sites located in 367 cities were
grouped into six regions: North China (n ¼ 369 sites), Northeast
China (n ¼ 173 sites), Northwest China (n ¼ 137 sites), Southeast
China (n ¼ 556 sites), Southwest China (n ¼ 234 sites), and the
Tibetan plateau (n ¼ 29 sites). These six areas represent various
socio-economic and geo-climatic regions within China (for details,
refer to Xu et al., 2015; Fig. S1). The provinces and monitoring sites
in each region are listed in Table S2. The monthly and daily con-
centrations of each pollutant were calculated for each of the six
different regions. Weekday (Monday-Friday) and weekend (Satur-
day and Sunday) concentrations were also calculated with a
method analogous to that used for the monthly calculations clas-
sified by region. In addition, seasonal average statistics were
defined for spring (MarcheMay), summer (JuneeAugust), fall
(SeptembereNovember) and winter (DecembereFebruary). The
time period from 6:00 a.m. to 5:00 p.m. was defined as daytime,
and from 6:00 p.m. to 5:00 a.m. the next day was defined as night-
time. The calculation of daily, monthly, and annual mean concen-
trations of the six pollutants is described in detail in Text S2 of the
Supplement. In this study, we estimated the potential public health
impacts of PM2.5 and O3 on the Chinese population, aiming to
provide insights into the impacts of air quality changes on human
health. We only considered the populations in the cities and/or
counties where the monitoring sites were located. A detailed
description of health impact assessment is provided in Text S3 of
the Supplement. The excess risks of mortality (per increase in
1 mg m
3 of PM2.5 or 10 mg m
3 O3) for the four endpoints of PM2.5
(mortality, respiratory diseases, cardiovascular diseases, and
chronic bronchitis) and the one endpoint of O3 (cardiovascular
 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
mortality) are listed in Table S3.
2.3. Statistical analyses
A one-way analysis of variance (ANOVA) and paired-sample t
tests were used to examine the significance of the differences in the
mean concentrations of the six air pollutants for the same seasons
across years and between weekdays and weekends. Pearson cor-
relations and linear regression analyses were conducted for all
pollutants. Statistically significant differences were set at p < 0.05,
unless otherwise stated.
3. Results and discussion
3.1. Spatial distribution of six ambient pollutant concentrations in
China
As averaged over 2015e2018, the annual mean PM2.5 concen-
trations in the 367 cities ranged from 9.4 to 148.5 mg m
3 and
averaged 41.3 ± 17.4 mg m
3 across China (Fig. 1a). 1491 of the 1498
sites exceeded the Chinese Ambient Air Quality Standard (CAAQS)
Grade I of 15 mg m
3, whereas 80% of the 1491 sites exceeded the
Grade II standard of 35 mg m
3. The highest and lowest PM2.5
concentrations both occurred in Western China, with the highest
value (148.5 mg m
3) in Kashgar, and the lowest in Altay city
(9.4 mg m
3; Fig. 1a). The annual mean PM2.5 concentration over
China was extremely high as compared with that from 2015 to 2016
in Europe (average 7.8 ± 3.8 mg m
3), and that from 2015 to 2017 in
East Asia (19.0 ± 13.0 mg m
3) and the US (average 7.9 ± 2.9 mg m
3)
(Fig. 2a). The average PM2.5 concentrations for Europe and the US
were lower than the lowest concentration at a Chinese site. The
annual mean PM10 concentrations ranged from 25.0 mg m
3
(Lijiang) to 380.0 mg m
3 (Hetian) (on average 83.2 ± 34.4 mg m
3)
(Fig. 1b). The concentrations in 53% of the cities exceeded the Grade
II standard of the CAAQS (70 mg m
3). The averaged PM10 concen-
tration in China (83.2 mg m
3) was approximately 2.6e7 times
higher than those in Europe (12.0 ± 5.9 mg m
3), East Asia
(31.7 ± 20.4 mg m
3), and the US (20.7 ± 9.5 mg m
3) (Fig. 2b).
The annual mean SO2 concentrations ranged from 2.7 mg m
3 in
Sanya to 133.1 mg m
3 in Puzhong (on average 20.4 ± 13.7 mg m
3)
(Fig. 1c). The SO2 concentrations exceeded the Grade I CAAQS
standard (20 mg m
3) at 578 sites, with 23 sites (primarily located in
the Hebei and Shanxi provinces) exceeding the Grade II standard
(60 mg m
3). Although the average annual concentration of SO2
over China was only 0.4 mg m
3 higher than the Grade I CAAQS
standard, this value was approximately 20 times higher than the
average SO2 concentrations in Europe (0.86 ± 1.4 mg m
3) and 4e5
times higher than those in East Asian (2.5 ± 3.9 mg m
3) and the US
(1.0 ± 1.7 mg m
3) (Fig. 2c). The annual mean NO2 concentrations
ranged from 5.9 mg m
3 (Nanping) to 64.4 mg m
3 (Changzhi) and
averaged 31.1 ± 11.8 mg m
3 (Fig. 1d). There were 236 sites that had
NO2 concentrations lower than the Grade I standard (20 mg m
3).
However, at 411 of the remaining 1263 sites, NO2 concentrations
exceeded the Grade II standard (40 mg m
3). The average annual
mean NO2 concentration across all sites (31.1 mg m
3) was signifi-
cantly higher than those in Europe (5.6 ± 4.7 mg m
3), East Asia
(15.7 ± 15.1 mg m
3), and the US (9.4 ± 6.1 mg m
3) (Fig. 2d). The
annual mean concentrations varied from 0.3 (Yichun) to
2.7 mg m
3 (Lvliang) for CO (1.0 ± 0.3 mg m
3) (Fig. 1e), and from
52.0 (Haerbin) to 140.9 (Zaozhuang) mg m
3 for O3
(59.9 ± 12.2 mg m
3) (Fig. 1f). To date, the CAAQS has not defined
standard values for annual CO and O3 concentrations. Therefore, we
cannot make an official assessment of the impacts of the average
annual concentrations of these pollutants in China.
Generally, Northwest China (e.g. Xinjiang) and North China have
3
higher concentrations of PM2.5, PM10, and gaseous pollutants
(except for O3), whereas the Tibet Plateau and some parts of
Northeast China have lower concentrations of all measured pol-
lutants (Fig. 1). For example, the Xinjiang, Inner Mongolia, Hebei,
and Shanxi provinces showed the highest concentrations of PM2.5,
PM10, and SO2 (Fig. 1aec, Table S2). The NO2 concentrations were
highest in Xinjiang in Northwest China, and Hebei, and parts of
Shandong and Henan provinces in North China (Fig. 1d). The Xin-
jiang, Shanxi, and Henan Provinces (in North China) had higher CO
concentrations than other provinces (Fig. 1d). Overall, our results
demonstrated that air pollution is heavier in the north of the
country than in the south, owing to the geographic distributions of
specific emissions sources, topographic features, and climate. Two
possible explanations for the pollution gradient are 1) the large
number of coal-fired energy plants located in Northern China; and
2) the fact that Northern China is more economically dependent on
industry than Southern China and requires domestic heating in
winter owing to the cold weather (Bao et al., 2015; Zhang et al.,
2016). These condition resulted in high emissions and concentra-
tions of air pollutants (e.g. SO2, NOx CO, and PM2.5) in Northern
China (Chai et al., 2014; Liu et al., 2017a, b; Wang et al., 2014; Yang
et al., 2013; Zhang et al., 2009). High concentrations of SO2 and NO2,
as coupled with high atmospheric NH3, can accelerate PM2.5
pollution in Northern China, owing to enhanced formation of sec-
ondary aerosols (Huang et al., 2014; Xu et al., 2015, 2018). In
contrast, electricity generated from hydroelectric power is the
dominant energy source in Southern China (accounting for
approximately 80% of China’s total hydroelectric power in 2017,
http://news.bjx.com.cn/html/20180313/885159.shtml), and pro-
duces lower levels of air pollutants (Zhan et al., 2017).
In addition to the anthropogenic emissions of primary pollut-
ants (e.g. PM2.5, PM10, SO2, NO2, CO, and nonmethane volatile
organic compounds) from six source sectors (e.g. power, industry,
residential, transportation, agriculture, and solvent use) (Zheng
et al., 2018), temperature and wind speed are the main meteoro-
logical factors influencing the spatial distributions of particulate
matter and gaseous pollutants at a national scale in China (Li et al.,
2019a). The frequent presence of unfavourable meteorological
conditions (e.g. low temperature, shallow mixing layers, low pre-
cipitation, and low wind speed) in winter in the north are condu-
cive to the accumulation of air pollutants (Wang et al., 2017a, b).
The Tibeten plateau and Northwest China experienced higher O3
pollution as compared with the other four regions (Fig. 1f). This is
mainly owing to enhanced photochemical formation caused by
strong solar radiation and a long duration of sunshine (Ran et al.,
2014), as well as a strong stratosphere-troposphere exchange
process in the context of the low height of the troposphere (Yin
et al., 2017).
3.2. Inter-annual variation of air pollutants
From 2015 to 2018, the annual mean concentrations of PM2.5,
PM10, SO2, and CO decreased at annual rates of 3.2 mg m
3,
3.7 mg m
3, 3.9 mg m
3, and 0.1 mg m
3, respectively, whereas the
annual mean concentrations of NO2 and O3 increased at annual
rates of 0.4 and 3.1 mg m
3, respectively (Fig. S2, Supplement).
China’s anthropogenic emissions of SO2, NOx, CO, PM2.5, and PM10
decreased by 17e62% from 2013 to 2017 (Zheng et al., 2018), which
can partially explain the downward trends of their respective
annual mean concentrations, except for NO2. The spatial variation
in the annual differences in concentrations can be mainly attrib-
uted to differences from a combination of anthropogenic emissions
and meteorology (An et al., 2019). For example, as compared to the
88% contribution from anthropogenic emissions, 12% of the PM2.5
decrease from 2013 to 2018 in China is contributed by the
4 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659

Fig. 1. Spatial patterns of annual mean concentrations of a) PM2.5, b) PM10, c) SO2, d) NO2, e) CO, f) O3 at the 1498 sites average over 2015e2018, with annual averages for the six
regions shown in the boxes inside the corresponding figures (NC: North China; NEC: Northeast China; NWC: Northwest China; SEC: Southeast China; SWC: Southwest China; TP:
the Tibetan Plateau).
 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
Fig. 2. Comparison of annual mean concentrations of a) PM2.5, b) PM10, c) SO2, and d) NO2 in China and other countries worldwide (n on the bar denotes the number of monitoring
sites in corresponding regions, with details shown in Table S1 in the Supplement).
meteorology (e.g. wind speed, precipitation, relative humidity, and
temperature). The positive effect from meteorology is the greatest
in the Sichuan Basin and the Fenwei Plain, followed by Beijing-
Tianjin-Hebei, and the meteorology slightly favoured an increase
in PM2.5 in the Yangtze River Delta (Zhai et al., 2019). In addition,
the regional differences in NH3 emissions in China can also lead to
an evident spatial variability in the air concentrations of SO2, NO2,
and PM2.5 in China (Liu et al., 2018a, b, 2019). The increased annual
mean NO2 concentrations from 2015 to 2018 might reflect the
rebound of NOx emissions in some areas of China in 2018. In
contrast, the upward trend of annual mean O3 concentrations can
be ascribed to reduced PM2.5 concentrations, as a decrease of PM2.5
can slow down the aerosol sink of hydroperoxyl radicals, and thus
speed up O3 generation (Li et al., 2019b). In addition, Chinese
megacity clusters shifted from a volatile organic compound (VOC)-
limited O3 production regime to a mixed regime, owing to declines
in NOx emissions. This has lessened the NOx titration effect,
resulting in an increase in O3 concentration from 2005 to 2013 (Jin
and Holloway, 2015).
The annual mean PM2.5 concentrations decreased from
52.2 ± 18.5 mg m
3 in 2015 to 41.5 ± 14.1 mg m
3 in 2018 across all
sites in 31 provinces (Fig. S3a), whereas the annual PM10 concen-
tration decreased from 89.3 ± 60.6 mg m
3 in 2015 to
77.0 ± 32.6 mg m
3 in 2018 (Fig. S3b). The decrease in PM con-
centration can mainly be attributed to effective control measures
implemented by the Chinese government, e.g. using nuclear and
hydroelectric power, eliminating small coal-fired power generation
units, and setting up stringent emission standards for industrial
factories (Fu et al., 2014). While the annual average PM concen-
trations decreased overall, they displayed notable spatial hetero-
geneity. For example, the PM10 concentrations increased in some
provinces in Northwest China (e.g. Xinjiang) and North China (e.g.
Shanxi), likely owing to high emissions of coarse particulate matter
from sand and soil during the dry and dusty conditions in that
5
region (Song et al., 2017). In addition, the frequency of dust storms
in the Xinjiang provinces has increased slightly in recent years
(http://www.cma.gov.cn/), which may have promoted the elevation
of PM10. Overall, however, PM2.5 concentrations declined signifi-
cantly across China.
The SO2 concentrations decreased from 26.2 ± 16.3 mg m
3 in
2015 to 14.7 ± 7.7 mg m
3 in 2018 (Fig. S3c). Power plants are the
major source of SO2 and contribute more than 50% of the total
annual SO2 emissions in China (Lu et al., 2010). The decreases in
mean SO2 concentration across China are mainly owing to the
application of flue gas desulfurization technology, and the phasing
out of low-efficiency power generation units (Lu et al., 2010).
Additionally, electrostatic precipitators were previously widely
used in steel making and cement production processes, and their
reduced use has resulted in a major decrease in SO2 emissions (Hua
et al., 2016). The mean concentrations of NO2 showed minor
changes between 2015 (31.8 ± 12.5 mg m
3) and 2018
(30.2 ± 11.0 mg m
3). However, some provinces still showed an
increase in NO2 concentrations (Fig. S3d). Geographically, the
provinces with increasing NO2 concentrations were mainly located
in Southwest China (e.g. Sichuan, Yunnan, and Guangxi provinces),
Southeast China (e.g. Anhui and Guangdong provinces), and part of
Northwest China (e.g. Ningxia province), as well as some parts of
North China (e.g. Shanxi and Shaanxi). The increases in NO2 con-
centrations in the aforementioned provinces could be partially
explained by a growth in population density, traffic emissions, and
newly built power plants in less-developed regions. Transportation
has been the main contributor of NOx emissions in Chinese cities
(van der A et al., 2017). With Chinese economic development and
improvements to living standards, the 59.4 million private cars on
the roads in 2010 increased to 185.2 million in 2017, with a growth
rate of 18.0 million cars yr
1 (http://www.stats.gov.cn/tjsj/ndsj/).
The elevated NOx concentrations in the Ningxia province are
probably caused by enhanced NOx emissions from newly built
6 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
power plants, which were put into operation in 2010 (van der A
et al., 2017). The average CO concentration decreased slightly,
from 1.1 ± 0.4 mg m
3 in 2015 to 0.9 ± 0.3 mg m
3 in 2018 (Fig. S3e),
likely owing to changes in the structure of energy consumption
(Lindner et al., 2013).
In contrast, the annual mean O3 concentration increased from
55.6 ± 13.2 mg m
3 in 2015 to 65.0 ± 11.4 mg m
3 in 2018 (annual
rate of 2.3 mg m
3; Fig. S3f). In that regard, 22 of the 30 provinces
exhibited an increase in O3 concentration, with the Anhui province
showing the greatest amount of increase (þ18.8 mg m
3), and the
Qinghai province showing the greatest amount of decrease
(
9.4 mg m
3). Enhanced O3 pollution poses a threat to human
health and food security. For example, in cities in the Pearl River
Delta region an increases of 10 mg m
3 in O3 concentration over the
preceding two days could lead to a 0.81% increase in the mortality
rate (Tao et al., 2012). A review of the published data by Feng et al.
(2015) indicated that the current level of O3 pollution can cause a
6.4e14.9% loss of yield for wheat. Thus, the long-term and short-
term health endpoints associated with high O3 concentrations in
these provinces should be analysed in future studies.
3.3. Seasonal mean concentrations of six pollutants
The monthly mean concentrations of the six pollutants varied
greatly and showed a similar variation in all regions. Generally, the
concentrations of PM2.5, PM10, SO2, NO2, and CO show low values
from April to August, and high values from September to March,
whereas O3 exhibited the opposite behaviour (details are presented
in Text S4 and Fig. S4a in the Supplement). Based on an analysis of
the monthly data, the average PM2.5 concentrations show a large
seasonal variability across China, with the highest values occurring
during the winter (70.1 ± 27.0 mg m
3) and the lowest in summer
(30.0 ± 10.3 mg m
3) (Fig. S5a). A similar seasonal pattern is also
observed in all regions (Table S4). On a national scale, there were no
significant differences between the mean concentrations of PM2.5
in the spring and autumn (45.3 ± 15.2 versus 43.1 ± 14.5 mg m
3),
whereas the values were significantly higher in spring than in
autumn in Northwest China and Southern China (Table S4).. The
higher PM2.5 concentrations in winter were probably caused by the
combined effects of coal combustion for domestic heating, weak
photochemical reactions, and adverse diffusion conditions (e.g. low
boundary layer height, less precipitation and low wind speed) in
winter (Chai et al., 2014; Wang et al., 2014).
The seasonal variation of PM10 was generally in agreement with
PM2.5 in all regions, with the exception of Northwest China
(Fig. S5b, Table S4), where the PM10 concentration peaked in spring.
This was probably due to the higher contribution of wind-blown
dust in Northwest China. Wang et al. (2006) reported that
different dust events, such as storms, floating dust and blowing
dust contribute to PM10 pollution in Northwest China. The PM10
concentration in spring in North China was as high as that in
Northwest China. This mainly occurred because strong winds
transported dust from Mongolia and the QinghaieGansu regions to
North China (Wang et al., 2014). These suspended dust particles
were transported along a certain route: Taklimakan Desert - Hexi
Corridor - Loess Plateau - North China Plain. As a result, the areas
along this transmission route suffered from serious PM10 pollution
(Chen et al., 2017). Chen et al. (2015) found that the PM10 concen-
trations increased by 344.0%e2562.1% in northern Chinese cities
along the transportation pathways of dust derived from the Takli-
makan Desert and their outer edges. Ma et al. (2019) reported that
the relatively high PM10 mass concentration over the Beijing-
Tianjing-Hebei region in spring is also caused by the trans-
portation of dust from Northwest China and Inner Mongolia. With
regard to the differences in seasonal means over the 4 years, the PM
concentrations, especially of PM2.5, significantly decreased in all
four seasons in 2018 as compared with those in the former 3 years
(2015e2017), despite the opposite phenomenon sometime occur-
ring in winter in some regions such as North China, Northwest
China, Southwest China, and Southeast China (Table S4).
Seasonal variations of gaseous pollutants have been reported at
different temporal and spatial scales in many previous studies
(Wang et al., 2014; Li et al., 2017a, b, 2019a; Ma et al., 2019; Yin
et al., 2019). Generally, SO2, CO, and NO2 exhibited the highest
concentrations in winter and the lowest in summer, whereas the O3
concentration peaked in spring and/or summer. Yet, it is still un-
known whether seasonal differences reach a statistically significant
level. Although these studies provide valuable insights, most of
them only considered one-year monitoring data, and/or focused on
capital cities in China. Thus, there are unanswered questions. For
example, what are the seasonal patterns of air pollutants for
different regions of China, based on years of monitoring? Moreover,
what are the differences in seasonal means over the years? As
shown in Table S4 and Figs. S5cef, in the six regions, the seasonal
mean concentrations of all gaseous pollutants (except for O3)
showed similar variations to those of the previous studies, namely,
the highest concentrations in winter and the lowest in summer. The
difference is that we found significant seasonal variations in the
concentrations of all gaseous pollutants in all regions (Table S4). In
addition, the seasonal mean concentrations of SO2 showed a sig-
nificant decreasing trend among the same seasons from 2015 to
2018. In contrast, those of NO2 and CO generally declined signifi-
cantly in all four seasons in 2018 as compared with those in 2015,
despite some opposite behaviour occurring in some regions such as
autumn and/or winter in North China, Northwest China, Southwest
China, and Southeast China (Table S5). As for O3, the seasonal mean
concentrations in winter generally decreased significantly in 2018,
whereas those in the other three seasons generally increased
significantly, and/or remained at stable levels in all regions
(Table S5).
The main reasons for the high concentrations of SO2, NO2, and
CO in winter are the same as those for the high concentrations of
PM in winter as mentioned earlier. In contrast, the weather con-
ditions in summer (e.g. strong solar radiation, turbulent eddies, and
precipitation scavenging) favour the removal of near-surface pol-
lutants, causing lower summer concentrations (Antony et al., 2001).
The differences in SO2 concentrations between winter and summer
were much more pronounced in North China and parts of the
northwest (e.g. Inner Mongolia) than for other pollutants. This re-
flects the fact that local residential heating had a large impact on air
quality, as a high level of production and consumption of coal
during winter occurred in those regions. Additionally, the com-
bustion of fossil fuels for heating is also a pivotal factor influencing
the seasonal variation of CO concentrations (Li et al., 2019a).
However, the concentration of O3 shows an opposite seasonal trend
to SO2, NO2, and CO, i.e., it is highest in summer and lowest in
winter. Ground-level O3 is produced rapidly in polluted air by the
photochemical oxidation of VOCs catalysed by NOx radicals and
hydrogen oxide radicals (HOx ¼ OH þ HO2 þ organic peroxy radi-
cals (RO2)) (Li et al., 2017a, b). VOCs and NOx are mainly derived
from fuel combustion and industrial sources (Zheng et al., 2018),
and biogenic sources also contribute to VOC emissions (Wang et al.,
2017a, b). HOx originates mainly from the photochemical oxidation
of water vapour and the photolysis of carbonyls (Brasseur and
Jacob, 2017). Many meteorological parameters can affect the
photochemical formation of O3, but the dominant variable is the air
temperature. An increase in temperature can accelerate photo-
chemical reactions and increase the emissions of biogenic VOCs
(Pusede et al., 2015; Ma et al., 2016). In certain regions, temperature
is also closely linked with the intensity of solar radiation, which
 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659 7

plays a vital role in the photochemical formation of O3. Thus, the
weak sunlight and low temperature in winter can inhibit the for-
mation of O3, whereas the strong solar radiation and high tem-
peratures in summer are responsible for the enhanced O3
concentrations (Zhao et al., 2016).
3.4. Diurnal variation of air pollutants
The diurnal variation of air pollutants gives insight into the in-
teractions of pollutants with different emission sources, with both
chemical and physical processes operating on a diurnal variation.
Generally, the daily mean concentrations of all six pollutants
(except for O3) displayed a bimodal distribution across all six re-
gions, with maxima observed from 8:00 to 11:00 and 21:00 to 0:00,
and minima from 4:00 to 7:00 and 14:00 to 17:00 (Fig. 3aee). PM2.5
showed a pronounced diurnal pattern in the Tibetan plateau, with a
maximum of 41.6 ± 19.5 mg m
3 at 11:00. The PM2.5 concentration
gradually decreased between 00:00 and 05:00, and then increased
just after sunrise. After peaking at approximately 11:00, the PM2.5
concentration decreased until reaching a minimum of
20.5 ± 9.5 mg m
3 at 17:00, then gradually increased from 18:00 to
3:00 (beginning just after the end of typical working hours). As for
PM2.5, PM10, NO2, SO2, and CO, The diurnal peaks in the morning
and evening were mainly ascribed to elevated traffic emissions in
rush hours, and a decreased boundary layer height during and after
sunset (Lee et al., 2014; Zhang et al., 2014). As reported by Zhou
et al. (2014), the traffic volume was greatest near 9:00e10:00 and
19:00e22:00, resulting in high emissions of air pollutants from
vehicle exhaust. In addition, the concentrations of the six pollutants
(except for O3) decreased in the afternoon, likely owing to the
combined effect of a raised boundary layer height and photo-
chemical oxidation reactions for CO and NO2 (Han et al., 2011). In

Fig. 3. Diurnal variation of air pollutants in six regions (a. PM2.5; b. PM10; c. SO2; d. NO2; e. CO; f. O3).
8 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
contrast, the O3 concentrations showed opposite diurnal trends to
those of CO and NO2, with the maximum and minimum values
observed from 17:00 to 19:00, and 8:00 to 10:00, respectively
(Fig. 3f). These results, in turn, suggest that the highest O3 con-
centration in the afternoon was mainly the result of photochemical
reactions in the present of intense solar radiation, resulting in the
consumption of NO2 and CO (Yin et al., 2019).
3.5. Weekday and weekend efficiency
The weekend effect is calculated by the difference of pollutant
concentration ¼ (weekend e weekdays)/weekdays  100%. The
weekend/weekday differences of PM2.5, PM10, SO2, NO2, CO, and O3
across China were 2.29%, 1.76%, 0.97%, 0.61%, 0.56%, and
0.64%,
respectively (Table S6). These results suggest that air pollutants
displayed a positive weekend effect except for O3, which showed a
negative effect. However, the differences in the daily mean con-
centrations of the six pollutants between weekdays and weekends
are not significant at the 0.05 level. At the city level, air pollutants
generally displayed the obvious weekend effect in Beijing during
2013e2014 (Huang et al., 2015). Across China, the concentrations of
PM2.5, PM10, SO2, NO2, and CO from 2015 to 2016 were significantly
higher on weekdays than on weekends, whereas no significant
difference was found for O3 (Li et al., 2019a). One possible expla-
nation for the findings in this study is that human activities such as
travel for recreation are probably more intensive during the
weekend, resulting in the air pollutant concentration being similar
to that on weekdays.
On a spatial scale, the concentrations of PM2.5 and PM10 in
Northeast China showed positive and significant weekend effects
(p < 0.05), whereas the gaseous pollutants in Northeast China and
all pollutants in the other five regions revealed non-significant
weekend effects (Table S6). Our findings for Northeast China are
consistent with that of Du (2018) who systematically investigated
influencing factors of haze pollution in Northeast China, and they
stated that higher traffic intensity at weekends relative to week-
days is responsible for significantly heavier particulate matter
pollution on weekends in Northeastern China. Generally, the con-
centrations of PM2.5, PM10, SO2, NO2, and CO on weekdays were
slightly lower as compared with weekend values in North China,
Northeast China, and Southeast China, whereas Northwest China,
Southwest China, and the Tibetan Plateau showed the opposite
trend. However, the weekend effects of O3 generally showed an
opposite behaviour to other five pollutants, namely, higher O3
concentrations on weekdays than on weekends in all regions, with
the exception of Southeast China and the Tibetan Plateau.
3.6. Correlation between six air pollutants
To understand the relationships between the six air pollutants,
Pearson correlation coefficients (R) were calculated for each region,
based on their monthly mean concentrations from 2015 to 2018
(Fig. 4). PM2.5 values were strongly correlated (R > 0.82, p < 0.001)
with PM10 (p < 0.01) in six regions. Furthermore, both PM2.5 and
PM10 were positively correlated with SO2, NO2, and CO. suggesting
fossil fuel combustion was a common source for all six pollutants.
According to Zheng et al. (2018), coal consumption in China has
significantly decreased since 2013, owing to the more stringent
pollution control requirements implemented in the ‘Clean Air Ac-
tion’. As a result, the total anthropogenic emissions decreased by
59% for SO2 and by 21%e36% for the other four air pollutants (i.e.,
NOx, CO, PM2.5, and PM10). Therefore, our results demonstrate that
fossil fuel (including coal-based and oil-based fuels) combustion
was a common primary emission source for all six pollutants.
Similar results have also been reported in previous studies (Wang
et al., 2014; Song et al., 2017). In addition, gaseous SO2 and NOx
are precursors of secondary aerosols (Huang et al., 2014). This can
also explain the significant correlations between acidic gases (SO2
and NO2) and PM2.5 (or PM10, which includes PM2.5). From 2011 to
2015, the reduction of SO2 and NOx emissions by 38% and 21%,
respectively, resulted in a 14% reduction in secondary aerosol pro-
duction (Lachatre et al., 2019). In Northwest China and Southeast
China, the PM2.5 concentration showed stronger correlations with
NO2 (p < 0.001, R ¼ 0.44 and 0.52, respectively) than with SO2
(p < 0.001, R ¼ 0.27 and 0.19, respectively) (Fig. 4a, e), whereas in
the other four regions, the correlations between PM2.5 and NO2
(p < 0.001, R ¼ 0.47e0.59) were comparable to those between PM2.5
and SO2 (p < 0.001, R ¼ 0.43e0.65) (Fig. 4b, c, d, f). These results
imply that relative to SO2 emission control, more stringent control
of NOx emission should be implemented in Northwest China and
Southeast China to reduce PM2.5 pollution, whereas synchronous
control of NOx and SO2 emissions is vital for the improvement of air
quality in the other four regions. For example, in North China,
alkaline aerosol components (e.g. NH3) can capture gaseous SO2,
which is oxidised by NO2 to form sulphate, thereby aggravating
severe haze pollution (Cheng et al., 2016; Wang et al., 2016).
In addition, ammonia (NH3) emission reduction has been
proven to be a feasible option for alleviating haze pollution (Xu
et al., 2019). Using a chemical transport model with a high-
resolution NH3 emission inventory, Liu et al. (2019) demonstrated
that a 50% reduction in total NH3 emissions in China, along with a
15% reduction of total SO2 and NOx emissions, can lower PM2.5
concentrations by 11e17% in Northern China, south-central China,
and the Sichuan Basin. Similarly, An et al. (2019) showed that a 50%
reduction in the NH3 concentration accomplished a 10% reduction
in PM2.5. Ozone (p < 0.01) was significantly negatively correlated
with the other five pollutants in all regions (Fig. 4). One possible
explanation for this is that gaseous pollutants and aerosols weaken
the intensity of solar radiation (Pochanart, 2015), which is not
conducive to O3 formation. In addition, as compared with South-
west China, Southeast China, and Northeast China
(R ¼
0.18e0.23), O3 was significantly and negatively correlated
with NO2 in Northwest China, North China, and the Tibetan Plateau
(p < 0.001, R ¼
0.3e0.43). This indicates that NO2, as an important
precursor of O3, more actively participated in O3 formation in those
regions. Nevertheless, O3 the formation mechanisms also differed
between different land use types in the same region. For example,
the summer O3 formation in the plain and mountain areas situated
in Northern China was sensitive to VOCs and NOx, respectively
(Tang et al., 2012). In large urban areas in the Yangtze River Delta,
North China Plain, Pearl River Delta, O3 formation is VOC-limited
(Tie et al., 2013; Xue et al., 2014). A recent study by Li et al.
(2019c) showed that the chemistry of PM2.5 makes O3 pollution
less sensitive to NOx emission controls in the North China Plain,
underlining the need for reducing VOC emissions. Unfortunately,
such scientific information is still scarce, which limits our under-
standing of O3 formation from a broad perspective. Thus, the O3-
VOC-NOx chemistry over China merits further exploration through
more field measurements and modelling studies as well as mining
existing data, and is crucially important for developing effective
strategies for ground-level O3 pollution control.
3.7. Implications for health risk, uncertainty, and recommendations
PM2.5 and O3 are two air pollutants which threaten human
health (Li et al., 2017a, b; Feng et al., 2019). Changes in annual
concentrations of these two pollutants can lead to different heath
impacts (detailed descriptions of the resulting human risks and
spatial patterns are provided in Text S5 and Fig. S6, Supplement).
Comparing 2018 with 2015, the mortality, respiratory diseases,
 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659 9

Fig. 4. Correlations between air pollutants in six regions of China (a. Northwest China; b. North China; c. Northeast China; d. the Tibetan Plateau; e. Southeast China; f. Southwest
China). Shown are correlation coefficients, with two asterisk denoting significant correlation at p < 0.01.

cardiovascular diseases, and chronic bronchitis caused by PM2.5
decreased by 23.4%, 26.9%, 24.8%, and 26.5%, respectively, when the
PM2.5 concentration declined by 20% over China (Fig. 5aed,
Figs. S6aeh, and Table S7). In contrast, the total cardiovascular
mortality caused by O3 over China increased by 18.9% (Fig. 5e,
Figs. S6i and j, and Table S7). These results reflect the benefit of
PM2.5 reduction and highlight the importance of O3 pollution
control for the protection of human health. While China has
experienced a substantial improvement in PM2.5 air quality, the
regions with greater population density, such as North China and
Southeast China, produce a larger overall PM2.5-related mortality
benefit. At the same time, however, the largest rates of O3-attrib-
utable cardiovascular mortality also occurred in North China, and
some regions (e.g. the Yangtze River Delta) in Southeast China.
Some limitations should be noted in interpreting the results of
the present study: 1) the sampling methods used at all the sites
were not uniform. This may affect the data accuracy and the pre-
sented regional or countrywide estimates; 2) most of the PM2.5 and
O3 concentrations were only obtained from urban areas. The
exposure and health situations of rural populations were not
investigated. Substantial urban and rural disparities in mortality
can exist even within the same province, owing to differences in
social economics, social environments, and health services; 3) the
present study did not consider province-, age-, and disease-specific
mortality, and 4) improved health outcomes may also be based on
factors unrelated to air pollution (e.g. changes in the health system
and improved living standards). These factors were not analysed in
this study. With the updating of health data, future studies can
further improve on these aspects. In addition, although this is not
the intention of this study, there is a significant seasonal variation
10 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
Fig. 5. Differences in the number (on the y-axis of panels aee) of a) mortality caused by PM2.5, b) respiratory diseases caused by PM2.5, c) cardiovascular diseases caused by PM2.5, d)
chronic bronchitis caused by PM2.5, and e) cardiovascular mortality caused by O3) between 2015 and 2018.
in the acute effects of PM2.5 and O3 pollution on mortality in China
(Huang et al., 2012; Qin et al., 2017). With high temporal resolution
and full spatial coverage, the reanalysed data provides great po-
tential for future research to explore the acute effects of PM2.5 and
O3 in China (Liu et al., 2016).
4. Conclusions
The highest concentrations of regional air pollution were
observed in North China, followed by Northwest and Northeast
China, Southeast China, Southwest China, and the Tibetan plateau.
The annual mean concentrations of PM2.5, PM10, SO2, and CO
decreased between 2015 and 2018, whereas the O3 concentrations
increased substantially. This suggests that current air pollution
controls should be optimised to mitigate O3 pollution, to avoid
offsetting the benefits from reduced air pollution by other pollut-
ants. At a national scale, the annual average NO2 concentrations
showed a minor decrease in 2018 as compared with 2015, but the
NO2 concentrations increased in most provinces. Except for O3, the
concentrations of all pollutants were generally the highest in
winter and lowest in summer in all regions; in contrast, O3 showed
an opposite seasonal pattern.
The diurnal cycles of PM2.5, PM10, SO2, CO, and NO2 showed a
bimodal pattern (8:00e11:00 in the morning and 21:00e0:00 in
the evening) in all regions. However, O3 peaked between
17:00e19:00, and its lowest levels occurred between 8:00e10:00.
The daytime concentrations of PM2.5, PM10, CO, NO2, and O3 were
lower than at night-time, but SO2 was higher during the day. The
weekdays/weekend differences of the six pollutants were not sig-
nificant in all regions, with the exception of Northeast China where
PM2.5 and PM10 were at significantly higher concentrations on
weekends than on weekdays. Negative correlations were found
between O3 and the other five pollutants, suggesting that enhanced
pollution by other pollutants is unfavourable to O3 formation. NOx
controls were more beneficial than SO2 controls for mitigation of
PM2.5 pollution in Northwest China and Southeast China, The
mortality rate, respiratory diseases, cardiovascular diseases, and
chronic bronchitis caused by PM2.5 pollution decreased signifi-
cantly in 2018 as compared to 2015, in contrast to the significant
increase in the total number of O3-attributable deaths.
Based on our results, we propose that a region-oriented emis-
sion control strategy (e.g. targeting different pollutants/emission
sources in different regions) is needed to support further
improvement of air quality in China. Additionally, future emission
control measures should work toward synchronous mitigation of
PM2.5 and O3 pollution, to maximise the protection of human health
in China.
Author contributions
Wen Xu designed the study. Wen Xu, Mireadili Kuerban, Yizai-
tiguli Waili, and Ye Liu performed the data analysis and prepared
the figures and tables. Wen Xu and Mireadili Kuerban wrote the
manuscript with comments from Fan Fan, Jingjing Peng, Wei Qin,
Anthony J. Dore, and Fusuo Zhang.
Declaration of competing interest
The authors declare that they have no conflict of interest.
Acknowledgements
This work was supported by the National Natural Science
Foundation of China (41705130, 41977038), and China Postdoctoral
 M. Kuerban et al. / Environmental Pollution 258 (2020) 113659
Science Foundation (2019T120156, 2018M641531), and Beijing
Advanced Discipline.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.envpol.2019.113659.
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