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DOI	10.1016/j.atmosenv.2021.118373
	Valine involved sulfuric acid-dimethylamine ternary homogeneous nucleation and its atmospheric implications
	Liu Y.; Liu Y.-R.; Feng Y.-J.; Huang T.; Jiang S.; Wang Z.-H.; Cao H.; Huang W.
发表日期	2021
ISSN	1352-2310
卷号	254
英文摘要	New Particle Formation (NPF) is considered as the dominant source of aerosol particles, influencing the environment and human health tightly. In recent years, valine (VAL) has been identified in field detection in urban areas, which reveals that VAL may play an important role in participating in atmospheric nucleation. However, there have been no categorical reports explaining how VAL participates in the multi-component nucleation with precursor Sulfuric Acid (SA) and the atmospheric organic amine Dimethylamine (DMA) so far. In this paper, quantum chemical calculation and cluster kinetic simulation have been studied to research the nucleation mechanism of (SA)x(DMA)y(VAL)z (0≤x, y, z ≤ 3) system. Structural and thermodynamic analysis at ωB97XD/6-31++G(d, p) theory level and basis set shows that VAL could form various stable structures through hydrogen bonds with SA and DMA, and proton transfer in ternary structure enhances the stability of system. However, in the clusters of SA-DMA-VAL system with large numbers of molecules, there has been steric hindrance between molecules of cluster due to the high proportion of inactive groups in VAL, which insulates the further formation of hydrogen bonds. With regard to the distribution of Gibbs free energy on VAL-DMA grid, the energy decreases rapidly along the diagonal with VAL and DMA in different numbers of SA molecules, predicting possible nucleation path along the diagonal. Besides, there is a synergistic effect of VAL in system SA-DMA-VAL, and VAL tends to replace the role of DMA in the ternary system. Evaporation rate analysis indicates that the ternary system containing SA is more stable. The simulating formation rate of SA-DMA-VAL system compared with the CLOUD experiment at CERN shows that the nucleation potential of SA-DMA-VAL is superior to that of SA-NH3-H2O, but inferior to that of SA-DMA-H2O, inferring that VAL may show more potential in growth processes than the initial nucleation processes in the light of the specific value of formation rate. © 2021
关键词	Amino acid Atmospheric relevance Evaporation rate Nucleation mechanism Topological analysis
语种	英语
scopus关键词	Ammonia; Atmospheric chemistry; Evaporation; Free energy; Gibbs free energy; Hydrogen bonds; Molecules; Nucleation; Quantum chemistry; Sulfuric acid; Ternary systems; Thermoanalysis; Amino-acids; Atmospheric implications; Atmospheric relevance; Dimethylamines; Energy; Evaporation rate; Formation rates; Homogeneous nucleation; Nucleation mechanism; Topological analysis; Amino acids; dimethylamine; hydrogen; sulfuric acid; valine; aerosol; experimental study; Gibbs free energy; nucleation; simulation; sulfur isotope; sulfuric acid; atmosphere; chemical structure; controlled study; energy; evaporation; hydrogen bond; molecular stability; proton transport; stereospecificity; structure analysis; synergistic effect; temperature dependence; thermodynamics
来源期刊	ATMOSPHERIC ENVIRONMENT
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/248450
作者单位	School of Information Science and Technology, University of Science and Technology of China, Hefei, Anhui 230026, China; Laboratory of Atmospheric Physico-Chemistry, Anhui Institute of Optics & Fine Mechanics, Chinese Academy of Sciences, Hefei, Anhui 230031, China; Center for Excellent in Urban Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, Fujian 361021, China
推荐引用方式 GB/T 7714	Liu Y.,Liu Y.-R.,Feng Y.-J.,et al. Valine involved sulfuric acid-dimethylamine ternary homogeneous nucleation and its atmospheric implications[J],2021,254.
APA	Liu Y..,Liu Y.-R..,Feng Y.-J..,Huang T..,Jiang S..,...&Huang W..(2021).Valine involved sulfuric acid-dimethylamine ternary homogeneous nucleation and its atmospheric implications.ATMOSPHERIC ENVIRONMENT,254.
MLA	Liu Y.,et al."Valine involved sulfuric acid-dimethylamine ternary homogeneous nucleation and its atmospheric implications".ATMOSPHERIC ENVIRONMENT 254(2021).