Diagnosing ozone-NOx-VOC sensitivity and revealing causes of ozone increases in China based on 2013-2021 satellite retrievals

Abstract

Particulate matter (PM2.5) concentrations in China have decreased significantly in recent years, but surface ozone (O3) concentrations showed upward trends at more than 71g% of air quality monitoring stations from 2015 to 2021. To reveal the causes of O3 increases, O3 production sensitivity is accurately diagnosed by deriving regional threshold values of the satellite tropospheric formaldehyde-to-NO2 ratio (HCHO/NO2), and O3 responses to precursor changes are evaluated by tracking volatile organic compounds (VOCs) and NOx with satellite HCHO and NO2. Results showed that the HCHO/NO2 ranges of transition from VOC-limited to NOx-limited regimes apparently vary among Chinese regions. VOC-limited regimes are found widely over megacity clusters (North China Plain, Yangtze River Delta and Pearl River Delta) and concentrated in developed cities (such as Chengdu, Chongqing, Xi'an and Wuhan). NOx-limited regimes dominate most of the remaining areas. From 2013 to 2021, satellite NO2 and HCHO columns showed an annual decrease of 3.0g% and 0.3g%, respectively, indicating an effective reduction in NOx emissions but a failure to reduce VOC emissions. This finding further shows that O3 increases in major cities occur because the Clean Air Action Plan only reduces NOx emissions without effective VOC control. Based on the O3-NOx-VOC relationship by satellite NO2 and HCHO in Beijing, Chengdu and Guangzhou, the ozone concentration can be substantially reduced if the reduction ratio of VOCs/NOx is between 2:1 and 4:1.