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A critical review of sulfate aerosol formation mechanisms during winter polluted periods

Journal of Environmental Sciences 2023年第1期123卷 387-399页

作者： Can Ye Keding Lu Huan Song Yujing Mu Jianmin Chen Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science and EngineeringInstitute of Atmospheric SciencesFudan UniversityShanghai 200438China

sulfate aerosol contributes to particulate matter pollution and plays a key role in aerosol radiative forcing,impacting human health and climate change.Atmospheric models tend to substantially underestimate sulfate concentrations during haze episodes,indicating that there are still missing mechanisms not considered by the models.Despite recent good progress in understanding the missing sulfate sources,knowledge on different sulfate formation pathways during polluted periods still involves large uncertainties and the dominant mechanism is under heated debate,calling for more field,laboratory,and modeling work.Here,we review the traditional sulfate formation mechanisms in cloud water and also discuss the potential factors affecting multiphase S(Ⅳ)oxidation.Then recent progress in multiphase S(Ⅳ)oxidation mechanisms is summarized.sulfate formation rates by different prevailing oxidation pathways under typical winter-haze conditions are also calculated and compared.Based on the literature reviewed,we put forward control of the atmospheric oxidation capacity as a means to abate sulfate aerosol pollution.Finally,we conclude with a concise set of research priorities for improving our understanding of sulfate formation mechanisms during polluted periods.

关键词： sulfate aerosol Formation mechanisms Multiphase oxidation Transition metal ions Reactive oxygen species

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Characteristics of Anthropogenic sulfate and Carbonaceous aerosols over East Asia: Regional Modeling and Observation

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Advances in Atmospheric Sciences 2008年第6期25卷 946-959页

作者： Yan HUANG William L. CHAMEIDES Qian TAN Robert E. DICKINSON School of Earth and Atmospheric Sciences Georgia Institute of Technology Atlanta GA 30332 Nicholas School of the Environment and Earth Sciences Duke University Durham NC 27708 Goddard Earth Sciences and Technology Center University of Maryland Baltimore MD 21228

The authors present spatial and temporal characteristics of anthropogenic sulfate and carbonaceous aerosols over East Asia using a 3-D coupled regional climate-chemistry-aerosol model, and compare the simulation with the limited aerosol observations over the region. The aerosol module consists of SO2, SO4^2-, hydrophobic and hydrophilic black carbon （BC） and organic carbon compounds （OC）, including emission, advections, dry and wet deposition, and chemical production and conversion. The simulated patterns of SO2 are closely tied to its emission rate, with sharp gradients between the highly polluted regions and more rural areas. Chemical conversion （especially in the aqueous phase） and dry deposition remove 60% and 30% of the total SO2 emission, respectively. The SO4^2- shows less horizontal gradient and seasonality than SO2, with wet deposition （60%） and export （27%） being two major sinks. Carbonaceous aerosols are spatially smoother than sulfur species. The aging process transforms more than 80% of hydrophobic BC and OC to hydrophilic components, which are removed by wet deposition （60%） and export （30%）. The simulated spatial and seasonal SO4^2-, BC and OC aerosol concentrations and total aerosol optical depth are generally consistent with the observations in rural areas over East Asia, with lower bias in simulated OC aerosols, likely due to the underestimation of anthropogenic OC emissions and missing treatment of secondary organic carbon. The results suggest that our model is a useful tool for characterizing the anthropogenic aerosol cycle and for assessing its potential climatic and environmental effects in future studies.

关键词： regional climate modeling anthropogenic emission sulfate aerosol black carbon and organic carbon East Asia

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THE DIRECT EFFECTS OF aerosolS AND DECADAL VARIATION OF GLOBAL SEA SURFACE TEMPERATURE ON THE EAST ASIAN SUMMER PRECIPITATION IN CAM3.0

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Journal of Tropical Meteorology 2017年第2期23卷 217-228页

作者：刘超胡海波张媛杨修群 CMA-NJU Joint Laboratory for Climate Prediction Studies Instituted for Climate and Global Change ResearchSchool of Atmospheric SciencesNanjing UniversityNanjing 210093 China Key Laboratory of Meteorological Disaster of Ministry of Education Nanjing University of Information Science and TechnologyNanjing 210044 China School of Oceanic Sciences Nanjing University of Information Science and TechnologyNanjing 210044 China

Using the CAM3.0 model, we investigated the respective effects of aerosol concentration increasing and decadal variation of global sea surface temperature(SST) around year 1976/77 on the East Asian precipitation in boreal summer. By doubling the concentration of the sulfate aerosol and black carbon aerosol separately and synchronously in East Asia(100-150 °E, 20-50 °N), the climate effects of these aerosols are specifically investigated. The results show that both the decadal SST changing and aerosol concentration increasing could lead to rainfall decreasing in the center of East Asia, but increasing in the regions along southeast coast areas of China. However, the different patterns of rainfall over ocean and lower wind field over Asian continent between aerosol experiments and SST experiments in CAM3.0 indicate the presence of different mechanisms. In the increased aerosol concentration experiments, scattering effect is the main climate effect for both sulfate and black carbon aerosols in the Eastern Asian summer. Especially in the increased sulfate aerosol concentration experiment, the climate scattering effect of aerosol leads to the most significant temperature decreasing, sinking convection anomalies and decreased rainfall in the troposphere over the central part of East Asia. However, in an increased black carbon aerosol concentration experiment, weakened sinking convection anomalies exist at the southerly position. This weakened sinking and its compensating rising convection anomalies in the south lead to the heavy rainfall over southeast coast areas of China. When concentrations of both sulfate and black carbon aerosols increase synchronously, the anomalous rainfall distribution is somewhat like that in the increased black carbon concentration aerosol experiment but with less intensity.

关键词： black carbon aerosol sulfate aerosol global decadal change of SST East Asian summer monsoon precipitation southern flood and northern drought

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