Amines in the Earth's Atmosphere: A Density Functional Theory Study of the Thermochemistry of Pre-Nucleation Clusters
Amines in the Earth's Atmosphere: A Density Functional Theory Study of the Thermochemistry of Pre-Nucleation Clusters
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DOI：
10.3390/e13020554
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发表时间：
2011-02-01
期刊：
影响因子：
2.7
通讯作者：
Xu, Yisheng
中科院分区：
文献类型：
--
作者：
Nadykto, Alexey B.;Yu, Fangqun;Xu, Yisheng
地球大气中存在的有机物对新粒子爆发的影响对于理解大气成核现象的分子性质至关重要。胺最近被提出作为可能的二元预成核团簇的稳定剂。为了促进对大气成核现象的理解，已进行了硫酸-水二元团簇与甲基-、二甲基-和三甲基胺的氢键复合物的量子化学研究，所述氢键复合物代表常见的大气有机物种、植物产物和实验室杂质。硫酸-胺-水复合物的热化学稳定性被认为是高于硫酸-氨-水复合物，定性与以前的研究。然而，由于胺的稳定性的增强似乎不足以克服氨和胺的典型大气浓度的差异。需要进一步的研究，以解决现有的不确定性，并达成一个最终的结论，胺的重要性，大气成核。
The impact of organic species which are present in the Earth's atmosphere on the burst of new particles is critically important for the understanding of the molecular nature of atmospheric nucleation phenomena. Amines have recently been proposed as possible stabilizers of binary pre-nucleation clusters. In order to advance the understanding of atmospheric nucleation phenomena, a quantum-chemical study of hydrogen-bonded complexes of binary sulfuric acid-water clusters with methyl-, dimethyl-and trimethylamines representing common atmospheric organic species, vegetation products and laboratory impurities has been carried out. The thermochemical stability of the sulfuric acid-amines-water complexes was found to be higher than that of the sulfuric acid-ammonia-water complexes, in qualitative agreement with the previous studies. However, the enhancement in stability due to amines appears to not be large enough to overcome the difference in typical atmospheric concentrations of ammonia and amines. Further research is needed in order to address the existing uncertainties and to reach a final conclusion about the importance of amines for the atmospheric nucleation.