气溶胶稳定硫同位素研究进展  

Research progress on stable sulfur isotopes in aerosols

作　　者：马皓 王森[1,2,3] 牛振川[4,5,6,7] 冯雪 黄智浦[1,4] MA Hao;WANG Sen;NIU Zhenchuan;FENG Xue;HUANG Zhipu(College of Urban and Environmental Sciences,Northwest University,Xi’an 710127,China;Shannxi Key Laboratory of Earth Surface System and Environmental Carrying Capacity,Northwest University,Xi’an 710127,China;Shannxi Xi’an Urban Forest Ecosystem Research Station,Xi’an 710127,China;State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,Chinese Academy of Sciences,Xi’an 710061,China;CAS Center for Excellence in Quaternary Science and Global Change,Xi’an 710061,China;Shannxi Key Laboratory of Accelerator Mass Spectrometry Technology and Application,Xi’an Accelerator Mass Spectrometry Center,Xi’an 710061,China;Shaanxi Guanzhong Plain Ecological Environment Change and Comprehensive Treatment National Observation and Research Station,Xi’an 710061,China;Xi’an Institute for Innovative Earth Environment Research,Xi’an 710061,China)

机构地区：[1]西北大学城市与环境学院,西安710127 [2]西北大学陕西省地表过程与环境承载力重点实验室,西安710127 [3]陕西西安城市生态系统定位观测研究站,西安710127 [4]中国科学院地球环境研究所黄土与第四纪地质国家重点实验室,西安710061 [5]中国科学院第四纪科学与全球变化卓越创新中心,西安710061 [6]陕西省加速器质谱技术及应用重点实验室,西安加速器质谱中心,西安710061 [7]陕西关中平原区域生态环境变化与综合治理国家野外科学观测研究站,西安710061 [8]西安地球环境创新研究院,西安710061

出　　处：《地球环境学报》2021年第4期359-377,共19页Journal of Earth Environment

基　　金：国家自然科学基金项目(41773141,42173082);中国科学院战略性先导科技专项(A类)(XDA23010302);中国科学院青年创新促进会(2016360)~~。

摘　　要：稳定硫同位素可以用来示踪硫酸盐气溶胶的来源、迁移和转化的过程。本文首先介绍了目前气溶胶稳定硫同位素相关的分析测试方法,即EA-IRMS、MC-ICPMS和NanoSIMS。归纳了国内外气溶胶δ^(34)S的时空组成特征,两极和沿海区域气溶胶δ^(34)S值普遍高于内陆区域;冬季燃煤和夏季生物排放作用使得气溶胶δ^(34)S值冬高夏低。同时,综述了硫酸盐气溶胶稳定硫同位素分馏特征,其质量分馏与SO_(2)氧化途径有关,非质量分馏与SO_(2)光化学反应、燃烧过程和矿物粉尘表面的非均相氧化有关。最后,探讨了稳定硫同位素在示踪气溶胶硫酸盐来源方面的应用,分析了人为成因硫和自然成因硫对气溶胶硫酸盐的贡献;并展望了稳定硫同位素在未来大气气溶胶溯源中的应用,以期为控制硫酸盐气溶胶的污染源提供科学依据。Background,aim,and scope The compositions of stable sulfur isotopes in aerosols can be used to trace the origin,migration,and transformation of sulfate aerosols.The changes in pollution source and SO_(2)oxidation pathway will lead to the changes ofδ^(34)S of sulfate aerosols,which affects the results of sulfur isotope tracing.In addition,some studies have shown that rather than the photochemical oxidation of SO_(2)in the stratosphere,the combustion process and mineral surface oxidation contribute to the sulfur isotopic anomalies.It is necessary to summarize the oxidation mode and fractionation effect of SO_(2)when analyzing the change of sulfur isotope of aerosol sulfate.Materials and methods The review describes the measurement methods,spatial distribution,and temporal variation of stable sulfur isotope(δ^(34)S)in aerosols.In addition,the fractionation characteristics and tracing researches of the stable sulfur isotope in aerosols are analyzed.Future researches on aerosol sulfur isotope are proposed.Results(1)EA-IRMS enables the measurement of multiple sulfur isotopes with high precision,while the MC-ICPMS is suitable for low-sulfur samples.NanoSIMS has a good application prospect in the analysis of stable sulfur isotope of single-particle aerosol.(2)Theδ^(34)S exhibits the following pattern:ocean area>coastal area>inland area,with its seasonal variation being higher in winter and lower in summer.(3)The oxidation of SO_(2)includes homogeneous oxidation,decreasing theδ^(34)S value,and the heterogeneous oxidation process,increasing theδ^(34)S value.(4)Aerosol sulfur includes anthropogenic sources mainly from vehicle exhaust and fossil fuels,and natural sources from biology,sea salt,and volcano.Theδ^(34)S of sulfate differs among sources.Discussion(1)The spatial distribution of aerosol sulfur isotope is affected by pollution sources and long-distance migration,while the seasonal variation of aerosolδ^(34)S is mainly due to the temporal fluctuation of SO_(2)enriched heavy sulfur isotope emitted from coal comb

关 键 词：气溶胶 硫同位素 δ^(34)S 分馏效应 示踪研究 

分 类 号：X513[环境科学与工程—环境工程]