Multicomponent nucleation of malonic acid involved in the sulfuric acid-dimethylamine system and its atmospheric implications
Multicomponent nucleation of malonic acid involved in the sulfuric acid-dimethylamine system and its atmospheric implications
复制标题
硫酸-二甲胺体系中丙二酸多组分成核及其大气影响
DOI：
10.1016/j.atmosenv.2021.118558
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发表时间：
2021
影响因子：
5
通讯作者：
Huang Wei
中科院分区：
文献类型：
--
作者：
Wang Zhong-Quan;Liu Yi-Rong;Wang Chun-Yu;Jiang Shuai;Feng Ya-Juan;Huang Teng;Huang Wei
丙二酸（MOA）是气溶胶中的主要二羧酸之一。一些现场观察和实验表明，丙二酸可能参与新颗粒形成（NPF）事件。然而，关于MOA参与的大气团簇形成机制的报道却很少。本研究采用高精度量子化学计算和动力学模拟来研究MOA参与硫酸（SA）-二甲胺（DMA）多组分体系的机制。最稳定的分子结构表明，MOA可以通过氢键和质子转移相互作用与SA-DMA体系形成相对稳定的簇。与CERN-CLOUD实验结果相比，高浓度DMA下SA-MOA-DMA体系的形成速率介于SA-DMA-W和SA–NH3–W体系之间。这意味着三元SA-MOA-DMA体系的成核作用在大气气溶胶成核中不可忽视。还发现温度对于 SA-MOA-DMA 系统的形成速率至关重要。形成速率与温度的强烈反比关系表明，如果温度降低，三元 SA-MOA-DMA 系统在 NPF 事件中变得越来越重要。
Malonic acid (MOA) is one of the main dicarboxylic acids in aerosols. Some field observations and experiments have revealed that malonic acid may be involved in new particle formation (NPF) events. However, there are few reports on the mechanism of atmospheric cluster formation involving MOA. In this study, high-precision quantum chemical calculations and dynamics simulations were used to investigate the mechanism by which MOA participates in a sulfuric acid (SA) - dimethylamine (DMA) multicomponent system. The most stable molecular structures show that MOA can form relatively stable clusters with the SA-DMA system by hydrogen bonding and proton-transfer interactions. Compared with the results of the CERN-CLOUD experiments, the formation rate of the SA-MOA-DMA system is between those of SA-DMA-W and SA–NH3–W systems at high concentration of DMA. This means that nucleation of the ternary SA-MOA-DMA system cannot be ignored in atmospheric aerosol nucleation. It was also found that temperature was crucial to the formation rate of the SA-MOA-DMA system. The strong inverse relationship of the formation rate and temperature indicates that if the temperature decreases the ternary SA-MOA-DMA system becomes increasingly important in NPF events.