Abstract
In recent years, ozone (O3) pollution in China has shown a worsening trend. Due to the vast territory of China, O3 pollution is a widespread and complex problem. It is vital to understand the current spatiotemporal distribution of O3 pollution in China. In this study, we collected hourly data on O3 concentrations in 338 cities from January 1, 2016, to February 28, 2019, to analyze O3 pollution in China from a spatiotemporal perspective. The spatial analysis showed that the O3 concentrations exceeded the limit in seven geographical regions of China to some extent, with more serious pollution in North, East, and Central China. The O3 concentrations in the eastern areas were usually higher than those in the western areas. The temporal analysis showed seasonal variations in O3 concentration, with the highest O3 concentration in the summer and the lowest in the winter. The weekend effect, which occurs in other countries (such as the USA), was found only in some cities in China. We also found that the highest O3 concentration usually occurred in the afternoon and the lowest was in the early morning. The comprehensive analysis in this paper could improve our understanding of the severity of O3 pollution in China.
Subject terms: Environmental impact, Sustainability
Introduction
Air pollution has rapidly increased over the last few decades due to urbanization and industrialization, and this increase has attracted attention around the world, including in China. In 2012, the National Ambient Air Quality Standards (NAAQS) (GB 3095-2012) was published by the Chinese Ministry of Environmental Protection, which identified six environmental pollutants: sulfur dioxide (SO2), nitrogen dioxide (NO2), carbon monoxide (CO), ozone (O3), and particulate matter (PM2.5 and PM10)1–3. Several air pollution control policies and programs have been established by the Chinese government4–6. However, there is still a gap between China’s ambient air quality and the air quality guidelines (AQG) of the World Health Organization (WHO)7. In recent years, although the concentrations of most pollutants, including NO2, SO2, particulate matter, and CO, decreased in the period of 2013–2016, O3 concentrations have increased by 10.79%8. O3 has become a secondary pollutant after PM2.5, which introduces new challenges to pollution control9.
In the past few years, many studies have investigated the impact, formation, and sources of O3 pollution. For instance, Khaniabadi et al.10 found that inhaling high concentrations of O3 or exposure to O3-polluted environments for a long period of time had a negative impact on health. Inhaling high concentrations of O3 can increase the risk of cardiovascular and respiratory diseases, which contribute to the overall mortality rate. Huang et al.11 found that ambient O3 exposure was related to the tremendous disease burden of chronic obstructive pulmonary disease in Ningbo, China, and the elderly comprised a more susceptible population. Existing evidence also reveals the adverse effects of O3 on mental health12. O3 pollution will not only have a negative impact on human health13 but also have a variety of adverse effects on plants, such as declines in crop yields and quality14–16. Because O3 has a negative impact on the transfer of nitrogen to grain, O3 pollution will reduce the fertilizer efficiency of wheat17, leading to the inhibition of net photosynthesis of wheat18. Additionally, O3 is a secondary pollutant that is formed by other pollutants through reactions19–21. Therefore, the formation of O3 pollution is affected by many factors22–24. Studies have shown that volatile organic compounds (VOCs) and NOx are key precursors of O3 formation23. Aromatic hydrocarbons and olefins are considered the main contributors to O3 formation in many cities or regions in China. Ethylene, trans-pentene, propene, and BTEX (benzene, ethylbenzene, toluene, m-, p-, and o-xylene), as well as warm weather and low wind speeds, are also major contributors to O3 formation25. Given that China is currently plagued by complex O3 pollution problems, understanding the spatiotemporal pattern of O3 pollution in China is of great significance for conducting environmental epidemiological studies and drafting appropriate regional O3 pollution control strategies.
Some scholars have launched investigations on the spatiotemporal pattern of O3. In Nanjing, a unimodal peak was observed with the highest O3 levels occurring from 14:00 to 15:00, and the O3 concentration reached its maximum and minimum levels in the summer and winter, respectively3. Wang et al.26 studied the ground-level O3 concentrations of 6 major Chinese cities located on both sides of the Heihe-Tengchong line, and they found that ground-level O3 concentrations exhibited monthly variability, peaking in summer and reaching the lowest levels in winter. The diurnal cycle reached a minimum in the morning and peaked in the afternoon. Some research has found that the O3 distribution pattern is also related to terrain features9,27.
As previously mentioned, most of the studies on O3 spatiotemporal patterns are carried out with a short time scale and low spatial resolution and generally focus on a specific city or a limited spatial region. To the best of our knowledge, there has been a lack of research on the spatiotemporal pattern of O3 in China using a higher spatial resolution and long time-series datasets. Recently, China established a large-scale ground real-time air quality monitoring network, which provides data we can use to conduct research on the spatiotemporal distribution pattern of O3 pollution nationwide.
In brief, this research makes the following contributions. First, we obtained the O3 concentration data of 338 cities across China for more than three years, covering 1-Jan-2016 to 28-Feb-2019. In terms of spatial perspective, we investigated the O3 concentrations in seven major geographic regions and three major urban agglomerations to conduct a more in-depth analysis and discussion. In terms of temporal perspective, we studied the annual, seasonal, monthly, weekly, daily, and diurnal and nocturnal variations in the O3 concentrations. Second, the reasons for different patterns in different regions were briefly analyzed. The research results from this large dataset can not only help us elaborate on the spatiotemporal distribution pattern of O3 concentration in China with a better spatiotemporal resolution and increase public awareness of the current O3 pollution situation in China but also assist the relevant departments in formulating more targeted O3 pollution prevention and control policies to meet the NAAQS and even the AQG standards in the future.
Results and Discussion
The NAAQS and the WHO set concentration limits for the maximum daily 8-hour average (MDA8) O3 concentration. Two levels of limits are specified in the NAAQS (Grade 1 and Grade 2), and three levels of limits are specified in the WHO standard (AQG, Interim target 1 and High level) (see Table 1).
Table 1.
NAAQS | Who | |||
---|---|---|---|---|
Grade 1 | Grade 2 | Air Quality Guidelines (AQG) | Interim target 1 | High level |
100 | 160 | 100 | 160 | 240 |
Spatial distribution of O3 in China
Figure 1 shows the spatial distributions of the O3 concentrations in 338 cities in China in 2016–2018. The regions with the most O3 pollution were mainly concentrated in North China and Central China, especially in the Beijing-Tianjin-Hebei region (BTH) region. In addition, the O3 pollution in the Chengdu-Chongqing and the Pearl River Delta region (PRD) regions was significantly higher than that of their neighboring regions. O3 pollution in China has shown a trend of outward expansion. As shown in Table 2, based on the statistical results of the 90th percentile of the maximum daily 8-hour average urban O3 concentration, the top 10 cities with severe O3 pollution are mainly located in North China, Central China and the East China.
Table 2.
2016 | 2017 | 2018 |
---|---|---|
1. Beijing (Beijing Municipality) 2. Tai’an (Shandong Province) 3. Dezhou (Shandong Province) 4. Hengshui (Hebei Province) 5. Dongying (Shandong Province) 6. Wuxi (Jiangsu Province) 7. Jinzhou (Liaoning Province) 8. Jinan (Shandong Province) 9. Panjin (Liaoning Province) 10. Heze (Shandong Province) |
1. Linfen (Shanxi Province) 2. Baoding (Hebei Province) 3. Jincheng (Shanxi Province) 4. Anyang (Henan Province) 5. Jiaozuo (Henan Province) 6. Tai’an (Shandong Province) 7. Xingtai (Hebei Province) 8. Langfang (Hebei Province) 9. Tangshan (Hebei Province) 10. Luoyang (Henan Province) |
1. Baoding (Hebei Province) 2. Jinan (Shandong Province) 3. Liaocheng (Shandong Province) 4. Binzhou (Shandong Province) 5. Jincheng (Shanxi Province) 6. Dezhou (Shandong Province) 7. Shijiazhuang (Hebei Province) 8. Xingtai (Hebei Province) 9. Cangzhou (Hebei Province) 10. Handan (Hebei Province) |
Fig. 2 displays the over-standard rate of the O3 concentration in seven geographical regions in China. None of the cities in North China met the AQG or Grade 1 limit, and nearly 70% exceeded the Grade 2 limit. In East and Central China, nearly 40% of urban O3 concentrations exceeded the Grade 2 limit. The O3 pollution in other regions was not so prominent; however, there were still considerable gaps from the AQG standard.
O3 is a secondary pollutant, which is generally formed in the atmosphere through photochemical pathways of NOx and volatile organic compounds (VOCs)28–32. Most of the NOx and VOCs come from heavy industries, such as coal-fired power plants, the steel industry, and the cement industry. Some studies found that the local photochemical reaction process has made an important contribution to the formation of O333, including the consumption of NO2 during the photochemical reaction process23, which has been observed in regions such as North China and Yangtze River Delta (YRD) region34,35.
Additionally, PM pollution control in these regions has achieved certain results, and the reduction in haze has led to increased visibility, which in turn, has promoted the process of photochemical reactions and promoted the formation of O3 pollution. It is worth noting that some cities in western China, where industrial activities are infrequent, sometimes have high concentrations of O3. In these high-altitude regions, the increase in O3 concentration may be related to the transport of O3 from the stratosphere to the troposphere36. In addition, meteorological environments with a high ultraviolet intensity and low humidity are conducive to O3 formation. In general, the formation of O3 pollution is affected by many factors, including prerequisite pollutant concentrations and meteorological conditions.
Annual variation in O3 in China
Figure 3 shows the change in ozone concentration in all cities in China in 2016-2018. The top and bottom whiskers extend from the hinges to the largest values by no more than 1.5* IQR (interquartile range). The upper and lower bounds of the box represent the 75th and 25th quartiles, respectively. The line in the middle of the box represents the median. The cross points indicate the mean values, and the square points outside the whisker indicate outliers. From 2016 to 2018, the O3 concentration showed an upward trend, and the ozone levels were roughly the same in 2017 and 2018. Figure 1 shows that the scope of heavy O3 pollution has gradually expanded. This phenomenon is also depicted in Fig. 4. In 2016, more than 95% of cities failed to meet the Grade 1 standard, and nearly 20% failed to meet the Grade 2 standard. In 2017 and 2018, these values increased to 99% and 30%, respectively.
Seasonal variation in O3 in China
The distributions of O3 in different seasons were heterogeneous, exhibiting significant seasonal variations. In general, O3 pollution in the summer is significantly higher than that in winter (Fig. 5). Because the photochemical reaction process is affected by meteorological conditions such as light and temperature, the meteorological conditions in summer are more suitable for photochemical reactions. In contrast, the UV intensity in winter is low, and the photochemical reaction is not enough to form heavy O3 pollution.
Seasonality is also reflected in spatial variation. In the spring and summer, O3 pollution is highest in North, East, and Central China. In autumn, O3 pollution gradually shifts to the south. In winter, national O3 pollution is relatively mild, and only a small part of South China suffers from O3 pollution. Overall, the problem of O3 pollution in the eastern areas is more serious than that in the western areas. The seasonality of O3 concentration changes in the BTH region and the YRD region is relatively high. However, the seasonality of O3 concentration changes in the PRD region is not as obvious. In the BTH region and the YRD region, the maximum and minimum O3 concentrations were observed in the summer and winter, respectively. In the PRD region, the maximum O3 concentration was observed in autumn, and the minimum was observed in winter.
The formation of O3 pollution varies based on factors such as the overall NOx and VOC emissions37–39, topography40, and atmospheric circulation in the region31,41. Evidence suggests that the high O3 pollution in the BTH region may be related to the emissions of precursor pollutants and the transportation of VOCs in neighboring provinces42,43. In the YRD region, the high temperatures in summer and the lower humidity can easily induce O3 pollution. The O3 concentration in the PRD region throughout the year is close and at a high level because the temperature throughout the year is similar and the annual average temperature exceeds 20°C in this region.
Monthly variation in O3 in China
Figure 6 illustrates the highest maximum, upper-quartile, median, lower-quartile, and minimum values of the monthly variations in O3 concentration from January to December in the seven regions and the total for all cities. The data confirm that the O3 concentration changes periodically depending on the month. Except for South and Southwest China, the trends in the O3 concentration variations in other regions are consistent with the national trend, showing an inverted V-shaped curve. The O3 concentration gradually increases from January to June, reaching the highest value in June, and then gradually decreases from June to December. The trend of O3 concentration variations in South China and Southwest China is relatively stable. The variation in the O3 concentration in South China shows an M-shaped curve, and the O3 concentration is higher in May and October. O3 pollution in Southwest China is “coming early and going fast”. The O3 concentration peaks around May and then falls sharply starting in June.
The monthly pattern of O3 can be attributed to changes in meteorological conditions and seasonal variations in precursor emissions. The decrease in the O3 concentration in South China in summer may be attributed to the climatic characteristic of the southwest monsoon that prevails in summer. The change in the O3 concentration in Southwest China is strongly affected by ultraviolet radiation. In addition, the penetration of stratospheric ozone into the troposphere is another reason supporting the high O3 concentration in the region.
Weekly variation in O3 in China
The weekly variation in the O3 concentration is shown in Fig. 7. The trends in different regions are not the same, but in general, they follow a W-shape. In North, Central, South, and Southwest China and in the BTH and PRD regions, the O3 concentration showed a valley on Tuesday. In North China, the YRD region, and the BTH region, the O3 concentration showed another valley on Saturday. Some scholars have studied the weekend effect of O3 that was first reported in New York in 1974, which suggested that the O3 concentration was higher during the weekend than on weekdays44. The weekend effect has been investigated in many other cities in the United States45–47, Europe48–50, and Asia51–53. The weekend effect of urban O3 is related to the decrease in human activities.
As shown in Fig. 8, the weekly variation in O3 concentration varies greatly in different regions and seasons. In our study, the valley value of O3 concentration often occurs on Tuesday. The weekend effect of O3 is more evident in the Northeast China, South China, Central China in summer, and Northwest China, Southwest China in winter to a certain degree. However, the general weekend effect of O3 pollution is not significant, from a national scale. The weekly variation in O3 concentration is affected by complex factors, the most likely of which is characteristics of urban resident activities. At present, no natural process has been found to produce climate change with a cycle of about 7 days, so Dominique et al.54 believe that the existence of such a cyclic process is manifestation of human impact on climate. Due to the obvious weekly cycle of human activities, many meteorological elements in many regions have corresponding weekly cycle characteristics55. Meteorological elements of some cities have been observed to have varying degrees of weekly cycle characteristics, such as temperature56,57, precipitation frequency58,59, etc., which have a significant cycle with 7-day. The change of these climate factors will further affect the generation of O3 in the photochemical reaction process, and thus affect the weekly variation. In general, the weekly variations in O3 concentration are not very prominent, which shows that the weekly changes in human activities have limited effects on O3 concentration.
Daily variation in O3 in China
Figure 9 shows the daily O3 concentration from January 1, 2016, to December 31, 2018. As shown in the figure, the daily variation in the O3 concentration is usually continuous. The change from high concentration to low concentration, or from low concentration to high concentration, is often a gradual process rather than a sudden change. In most parts of the country, the daily variation of O3 concentration shows an inverse U-shaped trend during each year, i.e., gradually increasing first and then decreasing. Except for South China, including the Pearl River Delta, the daily variation process of O3 concentration has volatility. When observing horizontally from three years, the three cycles of O3 variation can be clearly distinguished. We also found that for at least 1/3 of the days in the three years in each region, the O3 concentration exceeded the AQG, while for more than 1/3 of the days in North China, the O3 concentration exceeded Grade 1 of the NAAQS. When observing vertically, during the days with O3 pollution, the BTH, YRD, and PRD regions usually had even higher O3 concentrations than their neighboring areas. In short, the figure simultaneously shows the seasonal variation pattern as well as the spatial distribution characteristic of O3 concentration.
Diurnal and nocturnal variation in O3 in China
The hourly data on O3 concentration are shown in Fig. 10 and were used to investigate the diurnal and nocturnal variations in O3 pollutants in seven regions and three urban agglomerations in China. All regions showed a similar overall trend of O3 concentration, with a single peak. The O3 concentration was relatively lower at night, but as the sun rose, the O3 concentration gradually increased. The peak appeared between 14:00 and 16:00 (i.e., in the afternoon). After 16:00, the O3 concentration gradually decreased. The change in O3 concentration was affected by the temperature, solar radiation intensity, and various emissions from the surrounding environment. At night, due to the absence of solar radiation and the precursor of the photochemical reaction, the reaction was weakened and the O3 concentration decreased.
There are still some differences in the diurnal and nocturnal variations in the O3 concentration in various regions. For example, the variations in Southwest and Northwest China have a hysteresis phenomenon relative to other regions. The phenomenon is attributed to China’s vast territory, with more than 60° of east-west longitude, spanning 5,200 km and five time zones. Although Beijing time is uniformly used in China, there are actually time differences between the eastern and western regions.
O3-NOx-VOC sensitivity regimes and influencing factors
O3 is a secondary pollutant, and it is mainly produced by a series of photochemical reactions among precursors. Therefore, the formation of O3 pollution is affected by many factors in addition to meteorological factors. The most important factors are its precursors NOx and VOCs. The relationship between O3 and its precursor concentrations is generally nonlinear60. The decrease in precursor concentration does not necessarily result in a corresponding decrease in O3 concentration, and the sensitivity of O3 to NOx and VOCs will be different under different environmental conditions in the same region. The O3-NOx-VOC sensitivity regimes can describe the relationship between O3 and its local precursors (NOX and VOCs). The sensitivity relationship between O3 and its precursors determines the controlled types of O3 pollution in different regions. In brief, when the concentration of NOx in the atmosphere is high, the generation of O3 is controlled by VOCs; however, when the VOC concentration in the atmosphere is high, O3 generation is controlled by NOx. For example, in VOC-sensitive areas, the O3 concentration may increase with the reduction of the NOx concentration23. Clarifying whether O3 generation in a region is VOC-sensitive or NOx-sensitive is one of the important issues related to O3 generation mechanisms, which will be helpful in determining the control of targeted emissions to reduce O3 pollution61 and formulating O3 pollution control strategies.
In this paper, we summarize the O3-NOx-VOC sensitivity regimes in major cities in China that have been studied, and the results are shown in Supplementary Table S1. In the urban districts of most cities, including Beijing, Tianjin, Shanghai and Guangzhou, O3 generation is VOC-sensitive, mainly because human intervention in urban districts has greatly affected the emissions of precursors. Industry and transportation caused a large amount of NOx emissions, and the titration effect suppressed the increase in the O3 concentration in urban areas. In these areas, the priority control of VOC emissions is more helpful in controlling local O3 pollution. However, in the suburban areas of some cities, such as Lanzhou, Guiyang, Chongqing, and Xuzhou, the generation of O3 is NOx-sensitive. The suburbs are less affected by anthropogenic emissions, and the migration of pollutants caused by the wind will affect O3 pollution in the suburbs. In these areas, to suppress O3 generation more effectively, priority should be given to the control of NOx emissions.
In addition, the meteorological influencing factors in major cities in China are provided in Supplementary Table S1. The main meteorological factors that affect O3 generation include temperature, relative humidity, wind speed, wind direction, solar radiation, atmospheric pressure, cloud cover, sunshine duration, precipitation, ultraviolet radiation, visibility, and geopotential height. The statistics of their frequency are shown in Supplementary Fig. S1. In different regions, meteorological factors have heterogeneous effects on O3 generation. In general, O3 has a significant correlation with temperature and relative humidity. High temperature and low relative humidity are more conducive to the formation of O3, while meteorological factors such as sunshine duration, wind direction and wind speed have a crucial impact on the changes in O3 concentration.
Combined with the results of previous statistical analyses, we found that the O3 pollution affecting other cities is often caused by the synergistic effects of precursors and meteorological factors. For example, MDA8 in Beijing and its surrounding areas mainly occur at conditions of high temperature, low cloud cover, low relative humidity, weak southeast wind, low planetary boundary layer height, and the presence of a large amount of NOx and VOCs62. In Taiyuan, when the wind direction is southerly or southwesterly, the concentration of O3 is higher, which indicates that the increase in O3 concentration in Taiyuan is not only related to the local generation but also related to the external transport from the south63,64. The O3 volume fraction and its generation rate in Langfang showed a significant positive correlation with air temperature and a significant negative correlation with total cloud cover. It is also susceptible to transmission in the southern region of Hebei and Tianjin.
From a long-term perspective, according to the characteristics of different O3 pollution in different regions, priority should be given to strengthen the coordinated control of the sensitive precursor emissions in the region. Forecasting in advance when meteorological conditions are adverse and taking timely NOx and VOC control measures are important ways to solve regional O3 pollution problems.
Conclusions
This study analyzed the spatiotemporal distributions of O3 concentrations in 338 prefecture-level cities in China from January 2016 to February 2019. The purpose was to understand the current status of O3 pollution in China with a higher spatial resolution and a longer time series. Our study has the following findings:
O3 had obvious spatial heterogeneity. Only a few cities met the AQG standard of the WHO. O3 pollution in North, East, and Central China was more serious, especially in the BTH region. The O3 concentrations in the BTH, YRD, and PRD regions were usually higher than those in their neighboring cities. In the spring and summer, O3 pollution in the north was more serious; in autumn, O3 pollution shifted toward the south. In winter, the O3 pollution problem was relatively mild across China.
O3 showed a significant temporal variation pattern. The O3 concentration increased each year from 2016 to 2018. For the monthly variation in O3, except for South and Southwest China, other regions showed an inverted-V curve. Although the weekly variation in O3 concentration was not exactly the same in different areas, some cities showed a W-shape. The O3 concentration was lower on Tuesday and Saturday, and no obvious weekend effect was found. The study also characterized the diurnal and nocturnal variation pattern of O3 concentration. The O3 concentration was significantly higher during the day because of factors such as solar radiation, temperature, and precursor emissions. Due to the different time zones in different cities, the western region had a remarkable lag effect compared with the eastern region.
At present, China has made some achievements in the control of PM, NOx and other pollutants; however, the problem of O3 pollution has become increasingly prominent. Against the background of China’s severe composite air pollution, the need for the coordinated control of multiple pollutants is becoming increasingly apparent. According to our understanding, there is coexistence of VOC control and NOx control in China’s O3 pollution, and the reduction of particulate matter pollution has exacerbated the problem of O3 pollution in China. The government should strengthen the monitoring of VOCs and combine the characteristics of O3 pollution in different regions to formulate more targeted O3 pollution control strategies to achieve a win-win situation of haze governance and O3 control.
Data and methods
The regional division of China
A total of 338 cities, including prefecture-level cities and municipalities, are used as basic study units to investigate the spatial and temporal distribution of O3 in China. To analyze the results more clearly, China was divided into seven geographical regions: Northeast China (NEC), North China (NC), East China (EC), Central China (CC), South China (SC), Northwest China (NWC), and Southwest China (SWC), and three urban agglomerations: Beijing-Tianjin-Hebei region (BTH), the Yangtze River Delta region (YRD), and the Pearl River Delta region (PRD) (Fig. 11).
Ground-level O3 monitoring data
The China National Environmental Monitoring Center (CNEMC) continuously operates and maintains the national air quality monitoring network of China. The network has comprised 496 stations in 74 cities since 2012, and the network was extended to 1436 monitoring stations in 338 cities after 2016. The real-time concentration of O3 was measured by the ultraviolet absorption spectrometry method and differential optical absorption spectroscopy at each monitoring site. The instrumental operation, maintenance, data assurance and quality control were properly conducted based on the most recent revisions of China Environmental Protection Standards2. The real-time hourly O3 concentration data are continuously recorded by the CNEMC in China and are provided to the public. The data for this study were obtained during the period from 1-Jan-2016 to 28-Feb-2019.
Maximum daily 8-hour average O3 and the annual average O3 concentration
In view of the impact of long-term O3 exposure on animals and plants, limits of the maximum daily 8-hour average O3 concentration are specified in the NAAQS. Therefore, the average hourly O3 concentration is calculated every 8 hours, which should include at least 6 hourly values within a given 8-hour period; otherwise, the average value is considered to be invalid. Invalid values are not accepted in subsequent analysis. Finally, the maximum daily 8-hour average O3 concentration in a day is used to represent the O3 level of that day. Additionally, the ‘technical regulation for ambient air quality assessment of China’ (on trial) (HJ 633-2013) published by the Ministry of Ecology and Environment of China (MEE) determined that the O3 annual assessment standard for a city is equal to the 90th percentile of MDA8.
Statistical method
The spatial distribution of O3 is analyzed by calculating the average MDA8 data of all cities in each region. The annual, seasonal, monthly, weekly and daily variations in O3 are represented by the average of the MDA8 of each city. Diurnal and nocturnal O3 variation is calculated using the hourly O3 concentration of each city.
Supplementary information
Acknowledgements
This work is supported by the National Natural Science Foundation of China (71671024, 71601028, 71421001), Fundamental Research Funds for the Central Universities (DUT20JC38, DUT20RW301), Humanity and Social Science Foundation of the Ministry of Education of China (15YJCZH198), Social Planning Foundation of Liaoning (L17AGL012), and Scientific and Technological Innovation Foundation of Dalian (2018J11CY009). The authors would like to thank the reviewers for their constructive comments.
Author contributions
G.F.Y. and Y.H.L. designed and performed the research. G.F.Y. and Y.H.L. wrote the manuscript and checked the Analysis. X.N.L. reviewed the analysis and revised the manuscript.
Competing interests
The authors declare no competing interests.
Footnotes
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
is available for this paper at 10.1038/s41598-020-64111-3.
References
- 1.China, M. Ambient air quality standards. GB 3095-2012. China Environmental Science Press, Beijing (2012).
- 2.Zhang Y, Cao F. Fine particulate matter (PM 2.5) in China at a city level. SCI REP-UK. 2015;5:14884. doi: 10.1038/srep14884. [DOI] [PMC free article] [PubMed] [Google Scholar]
- 3.An J, Shi Y, Wang J, Zhu B. Temporal Variations of O3 and NOxin the Urban Background Atmosphere of Nanjing, East China. Arch Environ Con Tox. 2016;71:224–234. doi: 10.1007/s00244-016-0290-8. [DOI] [PubMed] [Google Scholar]
- 4.Jin Y, Andersson H, Zhang S. Air pollution control policies in China: a retrospective and prospects. Int J Env Res Pub He. 2016;13:1219. doi: 10.3390/ijerph13121219. [DOI] [PMC free article] [PubMed] [Google Scholar]
- 5.Zhang H, et al. Air pollution and control action in Beijing. J Clean Prod. 2016;112:1519–1527. doi: 10.1016/j.jclepro.2015.04.092. [DOI] [Google Scholar]
- 6.Feng L, Liao W. Legislation, plans, and policies for prevention and control of air pollution in China: achievements, challenges, and improvements. J Clean Prod. 2016;112:1549–1558. doi: 10.1016/j.jclepro.2015.08.013. [DOI] [Google Scholar]
- 7.Krzyzanowski M, Cohen A. Update of WHO air quality guidelines. Air Quality, Atmosphere & Health. 2008;1:7–13. doi: 10.1007/s11869-008-0008-9. [DOI] [Google Scholar]
- 8.Wang Z, et al. Temporospatial variations and Spearman correlation analysis of ozone concentrations to nitrogen dioxide, sulfur dioxide, particulate matters and carbon monoxide in ambient air, China. Atmos Pollut Res. 2019;10:1203–1210. doi: 10.1016/j.apr.2019.02.003. [DOI] [Google Scholar]
- 9.Cheng L, et al. Regionalization based on spatial and seasonal variation in ground-level ozone concentrations across China. J Environ Sci-China. 2018;67:179–190. doi: 10.1016/j.jes.2017.08.011. [DOI] [PubMed] [Google Scholar]
- 10.Khaniabadi YO, et al. Cardiopulmonary mortality and COPD attributed to ambient ozone. Environ Res. 2017;152:336–341. doi: 10.1016/j.envres.2016.10.008. [DOI] [PubMed] [Google Scholar]
- 11.Huang J, et al. The burden of ozone pollution on years of life lost from chronic obstructive pulmonary disease in a city of Yangtze River Delta, China. Environ Pollut. 2018;242:1266–1273. doi: 10.1016/j.envpol.2018.08.021. [DOI] [PubMed] [Google Scholar]
- 12.Zhao T, Markevych I, Romanos M, Nowak D, Heinrich J. Ambient ozone exposure and mental health: A systematic review of epidemiological studies. Environ Res. 2018;165:459–472. doi: 10.1016/j.envres.2018.04.015. [DOI] [PubMed] [Google Scholar]
- 13.Liu H, et al. Ground-level ozone pollution and its health impacts in China. Atmos Environ. 2018;173:223–230. doi: 10.1016/j.atmosenv.2017.11.014. [DOI] [Google Scholar]
- 14.Tai APK, Martin MV, Heald CL. Threat to future global food security from climate change and ozone air pollution. Nat Clim change. 2014;4:817–821. doi: 10.1038/nclimate2317. [DOI] [Google Scholar]
- 15.Emberson LD, et al. A comparison of North American and Asian exposure–response data for ozone effects on crop yields. Atmos Environ. 2009;43:1945–1953. doi: 10.1016/j.atmosenv.2009.01.005. [DOI] [Google Scholar]
- 16.Fuhrer J, Booker F. Ecological issues related to ozone: agricultural issues. Environ Int. 2003;29:141–154. doi: 10.1016/S0160-4120(02)00157-5. [DOI] [PubMed] [Google Scholar]
- 17.Broberg MC, Uddling J, Mills G, Pleijel H. Fertilizer efficiency in wheat is reduced by ozone pollution. Sci Total Environ. 2017;607:876–880. doi: 10.1016/j.scitotenv.2017.07.069. [DOI] [PubMed] [Google Scholar]
- 18.Li C, Meng J, Guo L, Jiang G. Effects of ozone pollution on yield and quality of winter wheat under flixweed competition. Environ Exp Bot. 2016;129:77–84. doi: 10.1016/j.envexpbot.2015.11.011. [DOI] [Google Scholar]
- 19.Pu X, et al. Enhanced surface ozone during the heat wave of 2013 in Yangtze River Delta region, China. Sci Total Environ. 2017;603-604:807–816. doi: 10.1016/j.scitotenv.2017.03.056. [DOI] [PubMed] [Google Scholar]
- 20.Kerckhoffs J, et al. A national fine spatial scale land-use regression model for ozone. Environ Res. 2015;140:440–448. doi: 10.1016/j.envres.2015.04.014. [DOI] [PubMed] [Google Scholar]
- 21.Doherty RM. Ozone pollution from near and far. Nat Geosci. 2015;8:664–665. doi: 10.1038/ngeo2497. [DOI] [Google Scholar]
- 22.Xue LK, et al. Ground-level ozone in four Chinese cities: Precursors, regional transport and heterogeneous processes. Atmos Chem Phys. 2014;14:13175–13188. doi: 10.5194/acp-14-13175-2014. [DOI] [Google Scholar]
- 23.Wang T, et al. Ozone pollution in China: A review of concentrations, meteorological influences, chemical precursors, and effects. Sci Total Environ. 2017;575:1582–1596. doi: 10.1016/j.scitotenv.2016.10.081. [DOI] [PubMed] [Google Scholar]
- 24.Xue, L. et al. Oxidative capacity and radical chemistry in the polluted atmosphere of Hong Kong and Pearl River Delta region: analysis of a severe photochemical smog episode. Atmos Chem Phys (2016).
- 25.Deng Y, Li J, Li Y, Wu R, Xie S. Characteristics of volatile organic compounds, NO2, and effects on ozone formation at a site with high ozone level in Chengdu. J Environ Sci-China. 2019;75:334–345. doi: 10.1016/j.jes.2018.05.004. [DOI] [PubMed] [Google Scholar]
- 26.Wang W, et al. Assessing Spatial and Temporal Patterns of Observed Ground-level Ozone in China. Sci Rep-UK. 2017;7:3651. doi: 10.1038/s41598-017-03929-w. [DOI] [PMC free article] [PubMed] [Google Scholar]
- 27.Kanda I, Wakamatsu S. Small-scale variations in ozone concentration in low mountains. Atmos Environ. 2018;184:98–109. doi: 10.1016/j.atmosenv.2018.04.026. [DOI] [Google Scholar]
- 28.Ling ZH, Guo H, Cheng HR, Yu YF. Sources of ambient volatile organic compounds and their contributions to photochemical ozone formation at a site in the Pearl River Delta, southern China. Environ Pollut. 2011;159:2310–2319. doi: 10.1016/j.envpol.2011.05.001. [DOI] [PubMed] [Google Scholar]
- 29.Duan J, Tan J, Yang L, Wu S, Hao J. Concentration, sources and ozone formation potential of volatile organic compounds (VOCs) during ozone episode in Beijing. Atmos Res. 2008;88:25–35. doi: 10.1016/j.atmosres.2007.09.004. [DOI] [Google Scholar]
- 30.Wu W, Zhao B, Wang S, Hao J. Ozone and secondary organic aerosol formation potential from anthropogenic volatile organic compounds emissions in China. J Environ Sci-China. 2017;53:224–237. doi: 10.1016/j.jes.2016.03.025. [DOI] [PubMed] [Google Scholar]
- 31.Ning G, et al. Characteristics of air pollution in different zones of Sichuan Basin, China. Sci Total Environ. 2018;612:975–984. doi: 10.1016/j.scitotenv.2017.08.205. [DOI] [PubMed] [Google Scholar]
- 32.Li R, et al. Spatial and temporal variation of particulate matter and gaseous pollutants in China during 2014–2016. Atmos Environ. 2017;161:235–246. doi: 10.1016/j.atmosenv.2017.05.008. [DOI] [Google Scholar]
- 33.Ou, S. et al. Pollution Characteristics and Sensitivity of Surface Ozone in the Typical Heavy Industry City of North China Plain in Summer. Envirionmental Science, 1-13 (2020). [DOI] [PubMed]
- 34.Zhang C, et al. Satellite UV-Vis spectroscopy: implications for air quality trends and their driving forces in China during 2005–2017. Light: Science & Applications. 2019;8:100. doi: 10.1038/s41377-019-0210-6. [DOI] [PMC free article] [PubMed] [Google Scholar]
- 35.de Foy B, Lu Z, Streets DG. Satellite NO2 retrievals suggest China has exceeded its NOx reduction goals from the twelfth Five-Year Plan. SCI REP-UK. 2016;6:35912. doi: 10.1038/srep35912. [DOI] [PMC free article] [PubMed] [Google Scholar]
- 36.Chen C, et al. Vertical distribution of ozone and stratosphere-troposphere exchanges on the northeastern side of Tibetan Plateau. Plateau Meteorology. 2012;31:295–303. [Google Scholar]
- 37.Shiu C, et al. Photochemical production of ozone and control strategy for Southern Taiwan. Atmos Environ. 2007;41:9324–9340. doi: 10.1016/j.atmosenv.2007.09.014. [DOI] [Google Scholar]
- 38.Guo, H., Cheng, H. R., Ling, Z. H., Louie, P. K. K. & Ayoko, G. A. Which emission sources are responsible for the volatile organic compounds in the atmosphere of Pearl River Delta? Vol. 188. (2011). [DOI] [PubMed]
- 39.Cheng H, et al. On the relationship between ozone and its precursors in the Pearl River Delta: Application of an observation-based model (OBM) Environ Sci Pollut R. 2010;17:547–560. doi: 10.1007/s11356-009-0247-9. [DOI] [PubMed] [Google Scholar]
- 40.Klingberg J, et al. Variation in ozone exposure in the landscape of southern Sweden with consideration of topography and coastal climate. Atmos Environ. 2012;47:252–260. doi: 10.1016/j.atmosenv.2011.11.004. [DOI] [Google Scholar]
- 41.Lin M, Horowitz LW, Oltmans SJ, Fiore AM, Fan S. Tropospheric ozone trends at Mauna Loa Observatory tied to decadal climate variability. Nat Geosci. 2014;7:136–143. doi: 10.1038/ngeo2066. [DOI] [Google Scholar]
- 42.Zhang Q, et al. Variations of ground-level O 3 and its precursors in Beijing in summertime between 2005 and 2011. Atmos Chem Phys. 2014;14:6089–6101. doi: 10.5194/acp-14-6089-2014. [DOI] [Google Scholar]
- 43.Xu J, et al. Measurements of ozone and its precursors in Beijing during summertime: impact of urban plumes on ozone pollution in downwind rural areas. Atmos Chem Phys. 2011;11:12241–12252. doi: 10.5194/acp-11-12241-2011. [DOI] [Google Scholar]
- 44.Cleveland WS, Graedel TE, Kleiner B, Warner JL. Sunday and workday variations in photochemical air pollutants in New Jersey and New York. Science. 1974;186:1037–1038. doi: 10.1126/science.186.4168.1037. [DOI] [PubMed] [Google Scholar]
- 45.Altshuler SL, Arcado TD, Lawson DR. Weekday vs. weekend ambient ozone concentrations: Discussion and hypotheses with focus on Northern California. Journal of the Air and Waste Management Association. 1995;45:967–972. doi: 10.1080/10473289.1995.10467428. [DOI] [Google Scholar]
- 46.Koo B, et al. Impact of meteorology and anthropogenic emissions on the local and regional ozone weekend effect in Midwestern US. Atmos Environ. 2012;57:13–21. doi: 10.1016/j.atmosenv.2012.04.043. [DOI] [Google Scholar]
- 47.Seguel, R. J., Morales, S. R. G. E. & Leiva G., M. A. Ozone weekend effect in Santiago, Chile. Environ Pollut162, 72–79 (2012). [DOI] [PubMed]
- 48.Pont V, Fontan J. Comparison between weekend and weekday ozone concentration in large cities in France. Atmos Environ. 2001;35:1527–1535. doi: 10.1016/S1352-2310(00)00308-3. [DOI] [Google Scholar]
- 49.Schipa I, Tanzarella A, Mangia C. Differences between weekend and weekday ozone levels over rural and urban sites in Southern Italy. Environ Monit Assess. 2009;156:509–523. doi: 10.1007/s10661-008-0501-5. [DOI] [PubMed] [Google Scholar]
- 50.Castell-Balaguer N, Téllez L, Mantilla E. Daily, seasonal and monthly variations in ozone levels recorded at the Turia river basin in Valencia (Eastern Spain) Environ Sci Pollut R. 2012;19:3461–3480. doi: 10.1007/s11356-012-0881-5. [DOI] [PubMed] [Google Scholar]
- 51.Sadanaga Y, Shibata S, Hamana M, Takenaka N, Bandow H. Weekday/weekend difference of ozone and its precursors in urban areas of Japan, focusing on nitrogen oxides and hydrocarbons. Atmos Environ. 2008;42:4708–4723. doi: 10.1016/j.atmosenv.2008.01.036. [DOI] [Google Scholar]
- 52.Tan PH, Chou C, Chou CCK. Impact of urbanization on the air pollution “holiday effect” in Taiwan. Atmos Environ. 2013;70:361–375. doi: 10.1016/j.atmosenv.2013.01.008. [DOI] [Google Scholar]
- 53.Xie M, et al. Temporal characterization and regional contribution to O3 and NO x at an urban and a suburban site in Nanjing, China. Sci Total Environ. 2016;551-552:533–545. doi: 10.1016/j.scitotenv.2016.02.047. [DOI] [PubMed] [Google Scholar]
- 54.Bäumer, D. & Vogel, B. An unexpected pattern of distinct weekly periodicities in climatological variables in Germany. Geophysical Research Letters - Geophys Res Lett35 (2008).
- 55.Hou, L. & Yao, Z. Air Pollution Index and Precipitation Weekly Circulation Characteristics and Its Possible Influencing Mechanism Analysis over Beijing and Its Adjacent Regions. Chinese Journal Of Atmospheric Sciences36 (2012).
- 56.Gong, D.Y., Guo, D. & Ho, C.H. Weekend effect in diurnal temperature range in China: Opposite signals between winter and summer. Journal of Geophysical Research: Atmospheres111 (2006).
- 57.Duan, C., Miao, Q., Ma, L. & Wang, Y. Weekend Effect of Temperature Variation in the Yangtze River Delta Region. Resources and Environment in the Yangtze Basin21 (2012).
- 58.Gong, D.Y. et al. Weekly cycle of aerosol-meteorology interaction over China. Journal of Geophysical Research: Atmospheres112 (2007).
- 59.Bell, T.L. et al. Midweek increase in US summer rain and storm heights suggests air pollution invigorates rainstorms. Journal of Geophysical Research: Atmospheres113 (2008).
- 60.Yoo E, Park O. A study on the formation of photochemical air pollution and the allocation of a monitoring network in Busan. Korean J Chem Eng. 2010;27:494–503. doi: 10.1007/s11814-010-0076-z. [DOI] [Google Scholar]
- 61.Wang MY, Yim SHL, Wong DC, Ho KF. Source contributions of surface ozone in China using an adjoint sensitivity analysis. Sci Total Environ. 2019;662:385–392. doi: 10.1016/j.scitotenv.2019.01.116. [DOI] [PMC free article] [PubMed] [Google Scholar]
- 62.Tang G, et al. Spatial-temporal variations in surface ozone in Northern China as observed during 2009–2010 and possible implications for future air quality control strategies. Atmos Chem Phys. 2012;12:2757–2776. doi: 10.5194/acp-12-2757-2012. [DOI] [Google Scholar]
- 63.Feng X. Variation characteristics of ozone concentration in Taiyuan from 2013 to 2017. Environ Chem. 2019;38:1899–1905. [Google Scholar]
- 64.Zhang S, Zhang X, Chai F, Xue Z. Pollution Characteristics of NOx, O3and OX in the Ambient Air of Taiyuan City and Relativity Study. Environmental Protection Science. 2015;41:54–58. [Google Scholar]
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