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Improved atmospheric mercury simulation using updated gas-particle partition and organic aerosol concentrations

Journal of Environmental Sciences 2022年第9期34卷 106-118页

作者： Kaiyun Liu Qingru Wu Shuxiao Wang Xing Chang Yi Tang Long Wang Tonghao Liu Lei Zhang Yu Zhao Qin’geng Wang Jinsheng Chen State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084China Institute of Atmospheric Environment Guangdong provincial academy of environmental scienceGuangzhou 510045China China National Environmental Monitoring Centre Beijing 100012China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing210023China Center for Excellence in Regional Atmos.Environ. Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

The gaseous or particulate forms of divalent mercury(HgⅡ) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux(FLX). In the new nested-grid geos-chem model, we try to modify the HgⅡ gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg(GOM), particulate-bound Hg(PBM), and PM 2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature( T) and organic aerosol(OA) concentrations under different relative humidity(RH). Results showed that with increasing RH, the dominant process of HgⅡ gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgⅡ gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds(I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases(NMBs) of monthly gaseous element mercury(GEM), GOM, PBM, WFLX were reduced from-33%–29%, 95%–300%, 64%–261%, 117%–122% to-13%–0%,-20%–80%,-31%–50%,-17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.

关键词： nested geos-chem model HgⅡgas-particle partitioning Organic aerosol Atmospheric mercury Mercury deposition flux

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