二氧化硫和硫酸盐是硫的重要存在形式,是影响环境空气质量的重要大气污染物.硫酸盐气溶胶是影响全球气候变化的重要大气组分,大气中的硫酸盐气溶胶生命周期短,其浓度空间差异大、时间变化显著.在区域尺度乃至全球尺度研究其迁移转化和区域交叉影响,具有十分重要的科学意义.本研究以2010年SO_2全球排放清单为基础,应用国际通用大气化学模式(Mozart-4),模拟全球大气硫的迁移转化及其季节变化和空间分布特征,并分析全球不同区域间的交叉影响.结果表明:1SO_2柱浓度全球年均值为424.73μg S·m~(-2),中东及南亚最高,达3629.27μg S·m~(-2),南美最低,为181.06μg S·m~(-2).2硫酸盐柱浓度全球年均值为1572.86μg S·m~(-2),东亚年均硫酸盐柱浓度最高,达4556.58μg S·m~(-2),南美最低,为1014.33μg S·m~(-2).3冬季SO_2柱浓度高于其他春夏秋3季,夏季硫酸盐柱浓度高于冬季,主要是由于冬季低温使SO_2不易转化为硫酸盐.4硫酸盐表现出明显的全球迁移特征,全球各区域间交叉影响显著.东亚的净输出量最大,达4.01 Tg S·a~(-1).非洲、中亚及俄罗斯硫酸盐柱浓度的外源影响比例分别高达80.54%和73.00%.
Sulfate aerosols significantly influence both global climate and regional air quality. As a short-lived climate forcer,atmospheric sulfate aerosols have significant variances both in space and time. It is essential to investigate transformation,transport and cross-attribution of sulfur at both regional and global scales. Here,we modeled sulfur transformation and its global transport using the popular General Circulation Model( GCM) Mozart-4. Crossattribution among individual regions was also analyzed. It was shown that the estimated global annual mean column concentration of SO_2 was 424. 73μg S·m~(-2). The peak value( 3629. 27 μg S·m~(-2)) was found to occur in Middle East and South Asia,while the minimum value( 181. 06 μg S·m~(-2))occurred in South America. The estimated global annual mean column concentration of sulfate was 1572. 86 μg S·m~(-2). The peak value( 4556. 58μg S·m~(-2)) was observed in East Asia,whereas the minimum value( 1014. 33 μg S·m~(-2)) was found in South America. Modeled SO_2 column concentration in winter was higher than that in spring,summer and autumn,mainly due to its low oxidation rate in winter. Modeled sulfate column concentrations in spring and summer were higher than those in autumn and winter,mainly because of rainfall-induced wet deposition in the former seasons. Longrange transport of sulfate was evident,indicating significant cross-attribution among individual regions. East Asia had the highest sulfur net outflow( 4. 01 Tg S·a~(-1)). In Africa,Middle East and Russia,estimated proportion of sulfate from outside was as high as 80.54% and 73.00%,respectively.