Insights into soil NO emissions and the contribution to surface ozone formation in China

ATMOSPHERIC CHEMISTRY AND PHYSICS(2023)

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摘要
Elevated ground-level ozone concentrations have emerged as a major environmental issue in China. Nitrogen oxide (NO x ) is a key precursor to ozone formation. Although control strategies aimed at reducing NO x emissions from conventional combustion sources are widely recognized, soil NO x emissions (mainly as NO) due to microbial processes have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. This study estimated soil NO emissions in China using the Berkeley-Dalhousie Soil NO x Parameterization (BDSNP) algorithm. A typical modeling approach was used to quantify the contribution of soil NO emissions to surface ozone concentration. The brute-force method (BFM) and the Ozone Source Apportionment Technology (OSAT) implemented in the Comprehensive Air Quality Model with Extensions (CAMx) were used. The total soil NO emissions in China for 2018 were estimated to be 1157.9 Gg N, with an uncertainty range of 715.7-1902.6 Gg N. Spatially, soil NO emissions are mainly concentrated in Central China, North China, Northeast China, the northern Yangtze River Delta (YRD), and the eastern Sichuan Basin, with distinct diurnal and monthly variations that are mainly affected by the temperature and timing of fertilizer application. Both the BFM and OSAT results indicate a substantial contribution of soil NO emissions to the maximum daily 8 h (MDA8) ozone concentrations by 8.0-12.5 mu g m - 3 on average for June 2018, with the OSAT results being consistently higher than the BFM results. The results also showed that soil NO emissions led to a relative increase in ozone exceedance days by 10.5 %-43.5 % for selected regions. Reducing the soil NO emissions resulted in a general decrease in monthly MDA8 ozone concentrations, and the magnitude of ozone reduction became more pronounced as reductions increased. However, even with complete reductions in soil NO emissions, approximately 450.3 million people are still exposed to unhealthy ozone levels, necessitating multiple control policies at the same time. This study highlights the importance of soil NO emissions for ground-level ozone concentrations and the potential for reducing NO emissions as a future control strategy for ozone mitigation in China.
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