RESUMEN
Toughest-ever clean air actions in China have been implemented nationwide to improve air quality. However, it was unexpected that from 2014 to 2018, the observed wintertime PM2.5 (particulate matter with an aerodynamic diameter of less than 2.5 µm) concentrations showed an insignificant decrease in Henan Province (HNP), a region in the west of the North China Plain. Emission controls seem to have failed to improve winter air quality in HNP, which has caused great confusion in formulating the next air improvement strategy. We employed a deweathering technique to decouple the impact of meteorological conditions. The results showed that the deweathered PM2.5 trend was -3.3%/yr in winter from 2014 to 2018, which had a larger decrease than the observed concentrations (-0.9%/yr), demonstrating that emission reduction was effective at improving air quality. However, compared with the other two megacity clusters, Beijing-Tianjin-Hebei (BTH) (-8.4%/yr) and Yangtze River Delta (YRD) (-7.4%/yr), the deweathered decreasing trend of PM2.5 for HNP remained slow. The underlying mechanism driving the changes in PM2.5 and its chemical components was further explored, using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). Model simulations indicated that nitrate dominated the increase of PM2.5 components in HNP and the proportions of nitrate to total PM2.5 increased from 22.4% in January 2015 to 39.7% in January 2019. There are two primary reasons for this phenomenon. One is the limited control of nitrogen oxide emissions, which facilitates the conversion of nitric acid to particulate nitrate by ammonia. The other is unfavourable meteorological conditions, particularly increasing humidity, further enhancing nitrate formation through multiphase reactions. This study highly emphasizes the importance of reducing nitrogen oxide emissions owing to their impact on the formation of particulate nitrate in China, especially in the HNP region.