• 关键词：二氧化硫  硫酸盐  大气硫循环  Mozart-4  交叉影响

• 基金项目：国家自然科学基金（No.41371443，41390240）

• 李本纲
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 古陈
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 王晓利
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 李新月
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 李玮
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 雷瑞雪
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 张宇
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 付博
• 北京大学城市与环境学院, 地表过程分析与模拟教育部重点实验室, 北京 100871

• 摘要：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SO₂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：① SO₂柱浓度全球年均值为424.73 μgS·m^-2，中东及南亚最高，达3629.27 μgS·m^-2，南美最低，为181.06 μgS·m^-2.②硫酸盐柱浓度全球年均值为1572.86 μgS·m^-2，东亚年均硫酸盐柱浓度最高，达4556.58 μgS·m^-2，南美最低，为1014.33 μgS·m^-2.③冬季SO₂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SO₂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 TgS·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%.

• Abstract：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. Cross-attribution among individual regions was also analyzed. It was shown that the estimated global annual mean column concentration of SO₂ was 424.73 μgS·m^-2. The peak value (3629.27 μgS·m^-2) was found to occur in Middle East and South Asia, while the minimum value (181.06 μgS·m^-2) occurred in South America. The estimated global annual mean column concentration of sulfate was 1572.86 μgS·m^-2. The peak value (4556.58 μgS·m^-2) was observed in East Asia, whereas the minimum value (1014.33 μgS·m^-2) was found in South America. Modeled SO₂ 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. Long-range transport of sulfate was evident, indicating significant cross-attribution among individual regions. East Asia had the highest sulfur net outflow (4.01 TgS·a^-1). In Africa, Middle East and Russia, estimated proportion of sulfate from outside was as high as 80.54% and 73.00%, respectively.

• Key words：SO₂  sulfate  atmospheric sulfur cycle  Mozart-4  cross-attribution

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