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Source-receptor relationships between East Asian sulfur dioxide emissions and Northern Hemisphere sulfate concentrations

机译:东亚二氧化硫排放量与北半球硫酸盐浓度之间的源-受体关系

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摘要

We analyze the effect of varying East Asian (EA) sulfur emissions on sulfateconcentrations in the Northern Hemisphere, using a global coupledoxidant-aerosol model (MOZART-2). We conduct a base and five sensitivitysimulations, in which sulfur emissions from each continent are tagged, toestablish the source-receptor (S-R) relationship between EA sulfur emissionsand sulfate concentrations over source and downwind regions. We find thatfrom west to east across the North Pacific, EA sulfate contributesapproximately 80%–20% of sulfate at the surface, but at least 50%at 500 hPa. Surface sulfate concentrations are dominated by localanthropogenic sources. Of the sulfate produced from sources other than localanthropogenic emissions (defined here as "background" sulfate), EA sourcesaccount for approximately 30%–50% (over the Western US) and10%–20% (over the Eastern US). The surface concentrations of sulfatefrom EA sources over the Western US are highest in MAM (up to 0.15 μg/m),and lowest in DJF (less than 0.06 μg/m). Reducing EASO emissions will significantly decrease the spatial extent of the EAsulfate influence (represented by the areas where at least 0.1 μg mof sulfate originates from EA) over the North Pacificboth at the surface and at 500 hPa in all seasons, but the extent ofinfluence is insensitive to emission increases, particularly in DJF and JJA.We find that EA sulfate concentrations over most downwind regions respondnearly linearly to changes in EA SO emissions, but sulfateconcentrations over the EA source region increase more slowly than SOemissions, particularly at the surface and in winter, due to limitedavailability of oxidants (in particular of HO, which oxidizesSO to sulfate in the aqueous phase). We find that similar estimates ofthe S-R relationship for trans-Pacific transport of EA sulfate would beobtained using either sensitivity (i.e., varying emissions from a region toexamine the effects on downwind concentrations) or tagging techniques. Ourfindings suggest that future changes in EA sulfur emissions may cause littlechange in the sulfate-induced health impact over downwind continents.However, SO emission reductions may significantly reduce the sulfateconcentrations and the resulting negative radiative forcing over the NorthPacific and the United States, thus providing a warming tendency.
机译:我们使用全球耦合氧化剂-气溶胶模型(MOZART-2)分析了东亚(EA)硫排放量的变化对北半球硫酸盐浓度的影响。我们进行了一个基础和五个敏感性模拟,其中标记了每个大陆的硫排放量,以建立EA硫排放量与顺风区和顺风区的硫酸盐浓度之间的源-受体(S-R)关系。我们发现,从北到西,从东到西,EA硫酸盐约占表层硫酸盐的80%–20%,但在500 hPa至少占50%。表面硫酸盐的浓度主要由本地人为来源引起。从非人为排放源(此处定义为“背景”硫酸盐)以外的其他来源产生的硫酸盐中,EA来源约占美国西部的30%至50%和美国东部的10%至20%。在美国西部,来自EA来源的硫酸盐的表面浓度在MAM中最高(高达0.15μg/ m),在DJF中最低(小于0.06μg/ m)。减少EASO排放量将在整个太平洋北太平洋和整个季节的500 hPa范围内显着降低EA硫酸盐影响的空间范围(由至少EA产生0.1μgMof硫酸盐的区域表示),但影响程度不敏感我们发现大多数顺风地区的EA硫酸盐浓度对EA SO排放量的变化几乎呈线性响应,但EA源区域的硫酸盐浓度的增长速度比SO排放的增加速度要慢,特别是在地面和冬季,由于氧化剂(特别是HO,其在水相中将SO氧化为硫酸盐)的利用率有限。我们发现,使用敏感性(即通过改变某个地区的排放量以检查对顺风的影响)或标记技术,可以获得类似的估计,即硫酸盐跨太平洋运输的S-R关系。我们的研究结果表明,未来EA硫排放的变化可能不会引起硫酸盐对顺风大陆健康影响的变化,但是SO排放量的减少可能会显着降低北太平洋和美国的硫酸盐浓度以及由此产生的负辐射强迫,从而提供了变暖趋势。

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