Spatial and temporal variability of ozone sensitivity over China observed from the Ozone Monitoring Instrument

Surface ozone (O3) air pollution in populated regions has been attributed to emissions of nitrogen oxides (NO + NO2 = NOx) and reactive volatile organic compounds (VOCs). These constituents react with hydrogen oxide radicals (OH + HO2 = HOx) in the presence of sunlight and heat to produce O3. The question of whether to reduce NOx emissions, VOC emissions, or both is complicated by spatially and temporally heterogeneous ozone-NOx-VOC sensitivity. This study characterizes spatial and temporal variations in O3 sensitivity by analyzing the ratio of formaldehyde (HCHO, a marker of VOCs) to nitrogen dioxide (NO2), a metric known as the formaldehyde nitrogen ratio (FNR). Level 3 gridded retrievals from the Ozone Monitoring Instrument (OMI) aboard the NASA Aura satellite were used to calculate FNR, with our analysis focusing on China. Based on previous studies, we take FNR < 1.0 as indicating VOC-limited regimes, FNR > 2.0 as indicating NOx-limited regime, and FNR between 1.0 and 2.0 as indicating transitional regime (where either NOx reductions or VOC reductions would be expected to reduce O3). We find that the transitional regime is widespread over the North China Plain (NCP), the Yangtze River Delta, and the Pearl River Delta during the ozone season (defined as having near-surface air temperatures >20°C at the early afternoon OMI overpass time). Outside of these regions, the NOx-limited regime is dominant. Because HCHO and NO2 have distinct seasonal patterns, FNR also has a pronounced seasonality, consistent with the seasonal cycle of surface O3. Examining trends from 2005 to 2013 indicates rapid growth in NO2, especially over less-developed areas where O3 photochemistry is NOx limited. Over this time period, HCHO decreased in southern China, where VOC emissions are dominated by biogenic sources, but increased slightly over the NCP, where VOC emissions are dominated by anthropogenic sources. A linear regression approach suggests that most of China (70% of grid cells) will be characterized by a transitional regime during the O3 season by 2030. However, in megacities such as Guangzhou, Shanghai, and Beijing, NO2 has decreased such that the chemical regime has shifted from VOC limited in 2005 to transitional in 2013.