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内陆传输的海洋喷雾气溶胶在东亚夏季风期间氯离子消耗的单个颗粒研究

Individual particle investigation on the chloride depletion of inland transported sea spray aerosols during East Asian summer monsoon.

机构信息

Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air Pollution, Institute of Mass Spectrometry and Atmospheric Environment, Jinan University, Guangzhou 510632, PR China.

State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China; University of Chinese Academy of Sciences, Beijing 100039, PR China.

出版信息

Sci Total Environ. 2021 Apr 15;765:144290. doi: 10.1016/j.scitotenv.2020.144290. Epub 2020 Dec 24.

Abstract

Inland transported sea spray aerosol (SSA) particles along with multiphase reactions are essential to drive the regional circulation of nitrogen, sulfur and halogen species in the atmosphere. Specially, the physicochemical properties of SSA will be significantly affected by the displacement reaction of chloride. However, the role of organic species and the mixing state on the chloride depletion of SSA during long-range inland transport remains unclear. Hence, a single particle aerosol mass spectrometer (SPAMS) was employed to investigate the particle size and chemical composition of individual SSA particles over inland southern China during the East Asian summer monsoon. Based on the variation of chemical composition, SSA particles were clustered into SSA-Aged, SSA-Bio and SSA-Ca. SSA-Aged was regarded as the aged Na-rich SSA particles. In comparison to the SSA-Aged, SSA-Bio involved some extra organic species associated with biological origin (i.e., organic nitrogen and phosphate). Each type occupies for approximately 50% of total detected SSA particles. Besides, SSA-Ca may relate to organic shell of Na-rich SSA particles, which is negligible (~3%). Tight correlation between Na and diverse organic acids was exhibited for the SSA-Aged (r = 0.52, p < 0.01) and SSA-Bio (r = 0.61, p < 0.01), reflecting the impact of organic acids to the chloride displacement during inland transport SSA particles. The chloride depletion occupied by organic acids is estimated to be up to 34%. It is noted that distinctly different degree of chloride depletion was observed between SSA-Aged and SSA-Bio. It is more likely to be attributed to the associated organic coatings for the SSA-Bio particles, which inhibits the displacement reactions between acids and chloride. As revealed from the mixing state of SSA-Bio, defined hourly mean peak area ratio of Cl / Na increases with the increasing phosphate and organic nitrogen. This finding provides additional basis for the improvement of modeling simulations in chlorine circulation and a comprehensive understanding of the effects of organics on chloride depletion of SSA particles.

摘要

内陆传输的海雾气溶胶(SSA)颗粒与多相反应对于驱动大气中氮、硫和卤素物种的区域循环至关重要。特别是,SSA 的物理化学性质将受到氯离子置换反应的显著影响。然而,在长距离内陆传输过程中,有机物质的作用以及混合状态对 SSA 中氯离子损耗的影响仍不清楚。因此,本研究采用单颗粒气溶胶质谱仪(SPAMS),在东亚夏季风期间,对中国南部内陆地区 SSA 颗粒的粒径和化学成分进行了研究。根据化学成分的变化,将 SSA 颗粒分为 SSA-Aged、SSA-Bio 和 SSA-Ca。SSA-Aged 被认为是富含 Na 的老化 SSA 颗粒。与 SSA-Aged 相比,SSA-Bio 包含一些与生物来源有关的额外有机物质(即有机氮和磷酸盐)。每种类型的颗粒约占总检测到的 SSA 颗粒的 50%。此外,SSA-Ca 可能与富含 Na 的 SSA 颗粒的有机壳有关,但其含量可以忽略不计(~3%)。SSA-Aged(r = 0.52,p < 0.01)和 SSA-Bio(r = 0.61,p < 0.01)中 Na 与各种有机酸之间表现出紧密的相关性,反映了内陆传输过程中 SSA 颗粒中有机酸对氯离子置换的影响。有机酸对氯离子的损耗估计高达 34%。需要注意的是,在 SSA-Aged 和 SSA-Bio 之间观察到明显不同程度的氯离子损耗。这更可能归因于 SSA-Bio 颗粒的有机涂层,其抑制了酸与氯离子之间的置换反应。从 SSA-Bio 的混合状态来看,定义为每小时平均峰值面积比 Cl / Na 随磷酸盐和有机氮的增加而增加。这一发现为改进氯循环模型模拟以及全面理解有机物质对 SSA 颗粒中氯离子损耗的影响提供了额外的依据。

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