Hydration of the methanesulfonate-ammonia/amine complex and its atmospheric implications.
Hydration of the methanesulfonate-ammonia/amine complex and its atmospheric implications.
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甲磺酸盐-氨/胺络合物的水合及其对大气的影响
DOI：
10.1039/c7ra12064h
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发表时间：
2018-01-12
期刊：
影响因子：
3.9
通讯作者：
Huang, Wei
中科院分区：
文献类型：
--
作者：
Miao, Shou-Kui;Jiang, Shuai;Peng, Xiu-Qiu;Liu, Yi-Rong;Feng, Ya-Juan;Wang, Yan-Bing;Zhao, Feng;Huang, Teng;Huang, Wei
甲烷磺酸盐（MSA−）在大气中的浓度很高，预计会增强气溶胶成核和纳米颗粒的生长，但对甲烷磺酸盐簇的细节知之甚少。在这项研究中，MSA-被选择沿着与氨（NH3）或三种常见的胺和水（H2O），讨论气溶胶形成的三元均匀成核和离子诱导成核的作用。我们采用密度泛函理论方法在PW 91 PW 91/6-311++G（3df，3 pd）水平上研究了团簇的结构特征和热力学性质.非共价相互作用的分析预测，胺可以形成更稳定的簇与MSA−比NH3，在协议的结构和热力学的结果;然而，在胺的稳定性的增强是不够大，以克服在典型的大气条件下NH3和胺的浓度的差异。此外，在298.15 K下，（MSA−）（NH3/amines）（H2O）n（n = 0-3）团簇形成的有利自由能表明，MSA−可以促进气溶胶成核过程，结合NH3/amines和H2O，直到n = 3。复合物的形成有很强的温度和湿度依赖性;较高的湿度和温度促进较大水合物的形成。最后，对于（MSA-）（NH3/胺）（H2O）n团簇，蒸发速率被确定，以进一步研究大气的影响。甲烷磺酸盐（MSA−）在大气中的浓度很高，预计会增强气溶胶成核和纳米颗粒的生长，但对甲烷磺酸盐簇的细节知之甚少。
Methanesulfonate (MSA−), found in substantial concentrations in the atmosphere, is expected to enhance aerosol nucleation and the growth of nanoparticles, but the details of methanesulfonate clusters are poorly understood. In this study, MSA− was chosen along with ammonia (NH3) or three common amines and water (H2O) to discuss the roles of ternary homogeneous nucleation and ion-induced nucleation in aerosol formation. We studied the structural characteristics and thermodynamics of the clusters using density functional theory at the PW91PW91/6-311++G(3df,3pd) level. The analysis of noncovalent interactions predicts that the amines can form more stable clusters with MSA− than NH3, in agreement with the results from structures and thermodynamics; however, the enhancement in stability for amines is not large enough to overcome the difference in the concentrations of NH3 and amines under typical atmospheric conditions. In addition, the favorable free energies of formation for the (MSA−)(NH3/amines)(H2O)n (n = 0–3) clusters at 298.15 K show that MSA− could contribute to the aerosol nucleation process with binding NH3/amines and H2O up to n = 3. There are strong temperature and humidity dependences for the formation of complexes; higher humidity and temperature promote the formation of larger hydrates. Finally, for the (MSA−)(NH3/amines)(H2O)n clusters, the evaporation rates were determined to further investigate the atmospheric implications. Methanesulfonate (MSA−), found in substantial concentrations in the atmosphere, is expected to enhance aerosol nucleation and the growth of nanoparticles, but the details of methanesulfonate clusters are poorly understood.
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DOI：
10.1073/pnas.1211878109
发表时间：
2012-11-13
影响因子：
11.1
作者：
Dawson, Matthew L.;Varner, Mychel E.;Finlayson-Pitts, Barbara J.
通讯作者：
Finlayson-Pitts, Barbara J.
影响因子：
3.3
作者：
Chen, Haihan;Varner, Mychel E.;Finlayson-Pitts, Barbara J.
通讯作者：
Finlayson-Pitts, Barbara J.
苯炔铜配合物的气相合成及其反应活性
影响因子：
4.9
作者：
Chai, Yunfeng;Shen, Shanshan;Pan, Yuanjiang
通讯作者：
Pan, Yuanjiang
影响因子：
2.8
作者：
Herb, Jason;Nadykto, Alexey B.;Yu, Fangqun
通讯作者：
Yu, Fangqun
影响因子：
4.4
作者：
Berresheim, H;Elste, T;O'Dowd, CD
通讯作者：
O'Dowd, CD