Li Yasong, Wang Tijian, Wang Qin'geng, Li Mengmeng, Qu Yawei, Wu Hao, Fan Jiachen, Shao Min, Xie Min
School of the Environment, Nanjing University, Nanjing 210023, China.
School of Atmospheric Sciences, Nanjing University, Nanjing 210023, China.
Sci Total Environ. 2024 Oct 10;946:174327. doi: 10.1016/j.scitotenv.2024.174327. Epub 2024 Jun 30.
We employed an enhanced WRF-Chem to investigate the discrete mechanisms of aerosol-radiation-feedback (ARF), extinction-photochemistry (AEP), and heterogeneous-reactions (AHR) across different seasons in eastern China, aiming to assess the synergistic effects arising from the simultaneous operation of multiple processes on O and PM. Our findings demonstrated that ARF fostered the accumulation of pollutants and moisture, initiating two distinct feedback mechanisms concerning O. The elevation in the NO/NO ratio amplified O consumption. Increased near-surface moisture diminished upper-level cloud formation, thereby enhancing photolysis rates and O photochemical production. The pronounced impact of heightened NO/NO on O led to a decrease of 0.1-2.7 ppb. When decoupled from ARF, AEP led to a more significant reduction in photolysis rates, resulting in declines in both O and PM, except for an anomalous increase observed in summer, with O increasing by 1.6 ppb and PM by 2.5 μg m. The heterogeneous absorption of hydroxides in spring, autumn, and winter predominantly governed the AHR-induced variation of O, leading to a decrease in O by 0.7-1 ppb. Conversely, O variations in summer were primarily dictated by O-sensitive chemistry, with heterogeneous absorption of NO catalyzing a decrease of 2.4 ppb in O. Furthermore, AHR accentuated PM by facilitating the formation of fine sulfates and ammonium while impeding nitrate formation. In summer, the collective impact of ARF, AEP, and AHR (ALL) led to a substantial reduction of 6.2 ppb in O, alleviating the secondary oxidation of PM and leading to a decrease of 0.3 μg m in PM. Conversely, albeit aerosol substantially depleted O by 0.4-4 ppb through their interactions except for summer, aerosol feedback on PM was more pronounced, resulting in a significant increase of 1.7-6.1 μg m in PM. Our study underscored the seasonal disparities in the ramifications of multifaceted aerosol-ozone interplay on air quality.
我们采用了增强版的WRF-Chem模型,来研究中国东部不同季节中气溶胶-辐射反馈(ARF)、消光-光化学(AEP)和非均相反应(AHR)的离散机制,旨在评估多个过程同时作用于臭氧(O)和颗粒物(PM)所产生的协同效应。我们的研究结果表明,ARF促进了污染物和水汽的积累,引发了两种与臭氧有关的不同反馈机制。一氧化氮/二氧化氮(NO/NO₂)比值的升高加剧了臭氧的消耗。近地表水汽增加减少了高层云的形成,从而提高了光解速率和臭氧的光化学生成。NO/NO₂升高对臭氧的显著影响导致臭氧浓度降低了0.1 - 2.7 ppb。当与ARF解耦时,AEP导致光解速率更显著降低,致使臭氧和PM均减少,但夏季出现异常增加,臭氧增加了1.6 ppb,PM增加了2.5 μg/m³。春、秋、冬三季中氢氧化物的非均相吸收主要控制了AHR引起的臭氧变化,导致臭氧浓度降低了0.7 - 1 ppb。相反,夏季的臭氧变化主要由对臭氧敏感的化学过程决定,一氧化氮的非均相吸收催化臭氧浓度降低了2.4 ppb。此外,AHR通过促进细硫酸盐和铵盐的形成同时抑制硝酸盐形成,从而加剧了PM的生成。在夏季,ARF、AEP和AHR(ALL)的共同作用导致臭氧大幅减少了6.2 ppb,减轻了PM的二次氧化,导致PM减少了0.3 μg/m³。相反,尽管除夏季外气溶胶通过相互作用使臭氧大幅减少了0.4 - 4 ppb,但气溶胶对PM的反馈更为显著,导致PM显著增加了1.7 - 6.1 μg/m³。我们的研究强调了多方面气溶胶-臭氧相互作用对空气质量影响的季节差异。