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N_2O5在含氯气溶胶表面的非均相化学过程(简称N_2O_5+Cl非均相过程)能够同时影响O3和气溶胶的二次生成。准确表征该过程的2个重要参数(分别为γN2O5和φClNO2)的参数化方案，对于精准分析我国O3和PM2.5的二次生成具有重要意义。通过优化GEOS-Chem大气化学模式的非均相化学模块，定量评估本地化参数化方案和模式默认的参数化方案对我国O3和PM2.5耦合生成的影响。结果显示，在采用本地化参数化方案后，GEOS-Chem模式对于全国范围内N_2O5、ClNO2、O3和PM2.5观测浓度的模拟精度整体有所提升。模拟结果显示，相比基于中国实际空气质量情况的本地化参数化方案，GEOS-Chem默认的参数化会严重低估我国年均γN2O5和φClNO2，导致ClNO2的生成被低估，而N_2O5水解程度被高估。最终导致模式对于我国年均MDA8 O3低估48%，而年均PM2.5浓度高估27%。
Abstract：The heterogeneous chemical process of N_2O5 on the surface of chlorine-containing aerosols(referred to as the N_2O_5+ Cl heterogeneous process) can simultaneously affect the secondary formation of O3 and aerosols.The parameterization schemes for the two important parameters(γN2O5 and φClNO2) of this process are crucial for accurately analyzing the secondary formation of O3 and PM2.5 in China.In this study,the heterogeneous chemical module of the GEOS-Chem atmospheric chemical model was optimized to quantitatively evaluate the impact of the localized parameterization scheme and the default parameterization scheme of the model on the coupled generation of O3 and PM2.5 in China.The results showed that after the localized parameterization scheme was adopted,the simulation accuracy of the GEOS-Chem model for the observed concentrations of N_2O5,ClNO2,O3,and PM2.5 across the country has generally improved.The simulation results indicated that compared to the localized parameterization scheme based on the actual air quality situation in China,the default parameterization of the GEOS-Chem model underestimated the annual average γN_2O5 and φClNO2in China,resulting in an underestimation of ClNO2 formation and an overestimation of the N_2O5 hydrolysis degree.Ultimately,this leads to an underestimation of 48% of the annual average MDA8 O3 by the model and an overestimation of 27% of the annual average PM2.5 concentration in China.
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基本信息:
DOI：10.14034/j.cnki.schj.2026.02.012
中图分类号:X515
引用信息:
[1]杨夏捷,黄映楠.不同N_2O_5+Cl非均相过程参数化方案对我国空气质量影响模拟差异的定量评估与分析[J].四川环境,2026,45(02):101-110.DOI:10.14034/j.cnki.schj.2026.02.012.
2026-04-26
2026-04-26