A molecular understanding of the interaction of typical aromatic acids with common aerosol nucleation precursors and their atmospheric implications.
A molecular understanding of the interaction of typical aromatic acids with common aerosol nucleation precursors and their atmospheric implications.
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对典型芳香酸与常见气溶胶成核前体的相互作用及其大气影响的分子理解
DOI：
10.1039/c9ra07398a
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发表时间：
2019-11-04
期刊：
影响因子：
3.9
通讯作者：
Zhang, Qingzhu
中科院分区：
文献类型：
--
作者：
Wang, Hetong;Zhao, Xianwei;Zuo, Chenpeng;Ma, Xiaohui;Xu, Fei;Sun, Yanhui;Zhang, Qingzhu
芳香酸是由大量人为排放和二次转化产生的，被认为在新颗粒的形成中发挥着至关重要的作用。在本研究中，我们在PW 91/6-311++G（3df，3 pd）水平上进行了理论计算，研究了典型的芳香酸苯甲酸（BA）、苯乙酸（PAA）、邻苯二甲酸（PA）、间苯二甲酸（mPA）和对苯二甲酸（PTA）与常见的大气成核前体硫酸（SA）、水（H2O）、氨（NH3）、甲胺（MA）、二甲胺（DMA）和三甲胺（TMA）。通过几何分析、吉布斯自由能分析、OH/NH伸缩振动频率计算和分子中原子（AIM）分析确定了配合物中的相互作用。异二聚体通过4种氢键形成6 ~ 8元环，其氢键强度大小顺序为SO-H O > O-H O/N > N-H O。BA/PAA/mPA/PTA-SA复合物的吉布斯自由能最低。PA是更有可能与NH3或胺，而不是SA由于分子内氢键相互作用。此外，芳族酸具有与SA和NH3相互作用的类似能力，作为一元羧酸/二元羧酸。研究了芳香酸与常见成核前驱体在大气中形成异二聚体的可能性。
Aromatic acids, which are generated from numerous anthropogenic emissions and secondary transformations, have been considered to play a crucial role in new particle formation. In this study, we performed theoretical calculations at the PW91PW91/6-311++G(3df,3pd) level to investigate the interaction between typical aromatic acids namely benzoic acid (BA), phenylacetic acid (PAA), phthalic acid (PA), isophthalic acid (mPA), and terephthalic acid (PTA) and common atmospheric nucleation precursors namely sulfuric acid (SA), water (H2O), ammonia (NH3), methylamine (MA), dimethylamine (DMA), and trimethylamine (TMA). The geometric analysis, Gibbs free energy analysis, OH/NH-stretching vibrational frequency calculation, and atoms in molecules (AIM) analysis were conducted to determine the interactions in the complexes. The heterodimers formed a six to eight membered ring through four types of hydrogen bond, and the bond strength could be ranked in descending order: SO–H⋯O > O–H⋯O/N > N–H⋯O. The BA/PAA/mPA/PTA–SA complexes had the lowest Gibbs free energy values. PA was more likely to interact with NH3 or amines rather than SA due to an intra-molecular hydrogen bond. Additionally, the aromatic acids have similar ability to interact with SA and NH3 as monocarboxylic/dicarboxylic acid. The formation potential of the heterodimers from aromatic acids with common nucleation precursors in ambient atmosphere was investigated.
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