State Key Joint Laboratory of Environmental Simulation and Pollution Control, Department of Environmental Science, Peking University, Beijing 100871, China.
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Environ Sci Technol. 2022 Jun 21;56(12):7771-7778. doi: 10.1021/acs.est.2c02533. Epub 2022 May 24.
There is a large gap between the simulated and observed sulfate concentrations during winter haze events in North China. Although multiphase sulfate formation mechanisms have been proposed, they have not been evaluated using chemical transport models. In this study, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) was used to apportion sulfate formation. It was found that Mn-catalyzed oxidation on aerosol surfaces was the dominant sulfate formation pathway, accounting for 92.3 ± 3.5% of the sulfate formation during haze events. Gas-phase oxidation contributed 3.1 ± 0.5% to the sulfate formation due to the low OH levels. The HO oxidation in aerosol water accounted for 4.2 ± 3.6% of the sulfate formation, caused by the rapid consumption of HO. The contributions of O, NO oxidation, and transition metal ion-catalyzed reactions in aerosol water could be negligible owing to the low aerosol water content, low pH, and high ionic strength. The contributions from in-cloud reactions were negligible due to the barrier provided by stable stratification during winter haze events.
在中国北方冬季霾事件期间,模拟和观测到的硫酸盐浓度之间存在很大差距。尽管已经提出了多相硫酸盐形成机制,但它们尚未通过化学输送模型进行评估。在这项研究中,使用天气研究和预测模型与化学(WRF-Chem)来分配硫酸盐的形成。结果发现,气溶胶表面的 Mn 催化氧化是硫酸盐形成的主要途径,占霾事件期间硫酸盐形成的 92.3±3.5%。由于 OH 水平较低,气相氧化对硫酸盐形成的贡献为 3.1±0.5%。由于 HO 的快速消耗,气溶胶水的 HO 氧化占硫酸盐形成的 4.2±3.6%。由于气溶胶含水量低、pH 值低和离子强度高,O、NO 氧化和过渡金属离子催化反应在气溶胶水中的贡献可以忽略不计。由于冬季霾事件期间稳定的分层提供了障碍,云内反应的贡献可以忽略不计。