Interaction of gas phase oxalic acid with ammonia and its atmospheric implications
Interaction of gas phase oxalic acid with ammonia and its atmospheric implications
复制标题
气相草酸与氨的相互作用及其对大气的影响
DOI：
10.1039/c5cp00027k
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发表时间：
2015-01-01
影响因子：
3.3
通讯作者：
Huang, Wei
中科院分区：
文献类型：
--
作者：
Peng, Xiu-Qiu;Liu, Yi-Rong;Huang, Wei
草酸被认为在大气有机气溶胶的形成和增长中起重要作用。然而，作为一种常见的有机酸，气相草酸与多个氨分子形成的较大团簇的认识是不完整的。本工作在PW 91 PW 91/6-311++G（3df，3 pd）水平上研究了草酸团簇的结构和热力学性质.我们发现草酸与氨分子形成相对稳定的团簇，电离事件起着关键作用。热力学和大气相关性分析表明，H2 C2 O 4（NH3）在大气中具有明显的相对浓度，可能参与了新粒子的生成。然而，随着氨分子数量的增加，团簇的浓度逐渐降低。此外，预测草酸与氨分子的簇合物在低温条件下有利地形成，并显示出高的瑞利散射强度。
Oxalic acid is believed to play an important role in the formation and growth of atmospheric organic aerosols. However, as a common organic acid, the understanding of the larger clusters formed by gas phase oxalic acid with multiple ammonia molecules is incomplete. In this work, the structural characteristics and thermodynamics of oxalic acid clusters with up to six ammonia molecules have been investigated at the PW91PW91/6-311++G(3df,3pd) level of theory. We found that oxalic acid forms relatively stable clusters with ammonia molecules, and that ionization events play a key role. The analyses of the thermodynamics and atmospheric relevance indicate that the heterodimer (H2C2O4)(NH3) shows an obvious relative concentration in the atmosphere, and thus likely participates in new particle formation. However, with increasing number of ammonia molecules, the concentration of clusters decreases gradually. Additionally, clusters of oxalic acid with ammonia molecules are predicted to form favorably in low temperature conditions and show high Rayleigh scattering intensities.