Spatiotemporal Distribution, Sources, and Impact on Atmospheric Oxidation of Reactive Nitrogen Oxides in the North China Plain Agricultural Regions in Summer

Abstract

The lack of vertical observation of reactive nitrogen oxides in agricultural areas has posed a significant challenge in fully understanding their sources and impacts on atmospheric oxidation. Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations were conducted in the agricultural regions of the North China Plain (NCP) during the summer of 2019 to measure the vertical distributions of aerosols, nitrogen dioxide (NO2), and nitrous acid (HONO). This study aimed at revealing the spatiotemporal distribution, sources, and environmental effects of reactive nitrogen oxides in the NCP agricultural areas. Our findings indicated that the vertical profiles of aerosols and NO2 exhibited a near-Gaussian distribution, with distinct peak times occurring between 8:00–10:00 and 16:00–18:00. HONO reached its maximum concentration near the surface around 8:00 in the morning and decreased exponentially with altitude. After sunrise, the concentration of HONO rapidly decreased due to photolysis. Additionally, the potential source contribution function (PSCF) was used to evaluate the potential sources of air pollutants. The results indicated that the main potential pollution sources of aerosols were located in the southern part of the Hebei, Shanxi, Shandong, and Jiangsu provinces, while the potential pollution sources of NO2 were concentrated in the Beijing–Tianjin–Hebei region. At altitudes exceeding 500 m, the heterogeneous reactions of NO2 on aerosol surfaces were identified as one of the important contributors to the formation of HONO. Furthermore, we discussed the production rate of hydroxyl radicals (OH) from HONO photolysis. It was found that the production rate of OH from HONO photolysis decreased with altitude, with peaks occurring in the morning and late afternoon. This pattern was consistent with the variations in HONO concentration, indicating that HONO was the main contributor to OH production in the agricultural regions of the NCP. This study provides a new perspective on the sources of active nitrogen in agricultural regions and their contribution to atmospheric oxidation capacity from a vertical perspective.