Interaction between Common Organic Acids and Trace Nucleation Species in the Earth's Atmosphere

被引:62
作者
Xu, Yisheng [1 ,2 ]
Nadykto, Alexey B. [1 ]
Yu, Fangqun [1 ]
Herb, J. [1 ]
Wang, Wei [2 ]
机构
[1] SUNY Albany, Atmospher Sci Res Ctr, Albany, NY 12203 USA
[2] Chinese Res Inst Environm Sci, Atmospher Chem & Aerosol Res Div, Beijing 100012, Peoples R China
基金
美国国家科学基金会; 中国国家自然科学基金;
关键词
PARTICLE FORMATION EVENTS; CONDENSATION NUCLEI CCN; AEROSOL FORMATION; PYRUVIC-ACID; MOLECULAR-STRUCTURE; DICARBOXYLIC-ACIDS; CHARGING STATE; BENZOIC-ACID; AB-INITIO; COMPLEXES;
D O I
10.1021/jp9068575
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Atmospheric aerosols formed via nucleation in the Earth's atmosphere play an important role in the aerosol radiative forcing associated directly with global climate changes and public health. Although it is well-known that atmospheric aerosol particles contain organic species, the chemical nature of and physicochemical processes behind atmospheric nucleation involving organic species remain unclear. In the present work, the interaction of common organic acids with molecular weights of 122, 116, 134, 88, 136, and 150 (benzoic, maleic, malic, pyruvic, phenylacetic, and tartaric acids) with nucleation precursors and charged trace species has been investigated. We found a moderate strong effect of the organic species on the stability of neutral and charged ionic species. In most cases, the free energies of the mixed H2SO4-organic acid dimer formation are within 1 - 1.5 kcal mol(-1) of the (H2SO4)(NH3) formation energy. The interaction of the organic acids with trace ionic species is quite strong, and the corresponding free energies far exceed those of the (H3O+)(H2SO4) and (H3O+)(H2SO4)(2) formation. These considerations lead us to conclude that the aforementioned organic acids may possess a substantial capability of stabilizing both neutral and positively charged prenucleation clusters, and thus, they should be Studied further with regard to their involvement in the gas-to-particle conversion in the Earth's atmosphere.
引用
收藏
页码:387 / 396
页数:10
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