Hydration of 3-hydroxy-4,4-dimethylglutaric acid with dimethylamine complex and its atmospheric implications†,Physical Chemistry Chemical Physics

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Hydration of 3-hydroxy-4,4-dimethylglutaric acid with dimethylamine complex and its atmospheric implications†
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2018-09-25 00:00:00 , DOI: 10.1039/c8cp04029j
Ya-Juan Han _{1,

2,

3,

4,

5} , Ya-Juan Feng _{4,

5,

6,

7} , Shou-Kui Miao _{1,

2,

3,

4,

5} , Shuai Jiang _{4,

5,

6,

7} , Yi-Rong Liu _{4,

5,

6,

7} , Chun-Yu Wang _{1,

2,

3,

4,

5} , Jiao Chen _{4,

5,

8} , Zhong-Quan Wang _{1,

2,

3,

4,

5} , Teng Huang _{1,

2,

3,

4,

5} , Jie Li _{4,

5,

6,

7} , Wei Huang _{1,

2,

3,

4,

5}

Affiliation

Atmospheric aerosols have a tremendous influence on visibility, climate, and human health. New particle formation (NPF) is a crucial source of atmospheric aerosols. At present, certain field observations and experiments have discovered the presence of 3-hydroxy-4,4-dimethylglutaric acid (HDMGA), which may participate in NPF events. However, the nucleation mechanism of HDMGA has not been clearly understood. In addition, dimethylamine (DMA) is an important precursor of nucleation. The nucleation mechanism involving HDMGA and DMA has not been studied. In this study, the most stable structures of (HDMGA)(H₂O)_n (n = 0–3) and (HDMGA)(DMA)(H₂O)_n (n = 0–3) were obtained by using M06-2X coupled with the 6-311++G(3df,3pd) basis set. The α-carboxyl group is directly attached to the amino group in all the most stable configurations. Proton transfer enhances the strength of a hydrogen bond, as well as promotes the generation of a global minimum structure. Temperature has a considerable influence on the distribution of isomers for (HDMGA)(DMA)(H₂O)₃ as compared to the other investigated clusters. The Gibbs free energy values reveal that most of the clusters can exist in NPF, except for (HDMGA)(H₂O)₁. The process of adding a cluster of (H₂O)_n more likely occurs in the atmosphere than gradually adding a single water molecule.

中文翻译：

用二甲胺络合物水合3-羟基-4,4-二甲基戊二酸及其对大气的影响†

大气气溶胶对能见度，气候和人类健康具有巨大影响。新的颗粒形成（NPF）是大气气溶胶的重要来源。目前，某些现场观察和实验已经发现了3-羟基-4,4-二甲基戊二酸（HDMGA）的存在，它可能参与NPF事件。但是，HDMGA的成核机理尚未清楚。此外，二甲胺（DMA）是重要的成核前体。尚未研究涉及HDMGA和DMA的成核机理。在这项研究中，（HDMGA）（H ₂ O）_n（n = 0-3）和（HDMGA）（DMA）（H ₂ O）_n（n= 0–3）是通过将M06-2X与6-311 ++ G（3df，3pd）基础集结合使用而获得的。α-羧基以所有最稳定的构型直接连接到氨基上。质子转移增强了氢键的强度，并促进了整体最小结构的产生。与其他研究的簇相比，温度对（HDMGA）（DMA）（H ₂ O）₃的异构体分布有很大影响。吉布斯自由能值表明，除了（HDMGA）（H ₂ O）₁以外，大多数簇都可以存在于NPF中。与逐渐添加单个水分子相比，添加（H ₂ O）_n簇的过程更有可能在大气中发生。

更新日期：2018-09-25

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