Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS

doi:10.1021/acs.analchem.7b04921

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	Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS
	Borodin, O 8; Zhang, YY ; Su, M 2,4,5; Yu, XF ; Zhou, YF; Wang, JG ; Cao, RG ; Xu, W 3; Wang, CM ; Baer, DR
刊名	ANALYTICAL CHEMISTRY
	2018
卷号	90 期号:5 页码:3341-3348
关键词	CARBONATE-BASED ELECTROLYTES DENSITY-FUNCTIONAL THEORY MASS-SPECTROMETRY BATTERY ELECTROLYTES PROPYLENE CARBONATE LI-ION PREFERENTIAL SOLVATION INTERPHASIAL CHEMISTRY MOLECULAR-DYNAMICS ETHYLENE CARBONATE
ISSN号	0003-2700
DOI	10.1021/acs.analchem.7b04921
英文摘要	Ion solvent interactions in nonaqueous electrolytes are of fundamental interest and practical importance, yet debates regarding ion preferential solvation and coordination numbers persist. In this work, in situ liquid SIMS was used to examine ion-solvent interactions in three representative electrolytes, i.e., lithium hexafluorophosphate (LiPF6) at 1.0 M in ethylene carbonate (EC)-dimethyl carbonate (DMC) and lithium bis(fluorosulfonyl)imide (LiFSI) at both low (1.0 M) and high (4.0 M) concentrations in 1,2-dimethoxyethane (DME). In the positive ion mode, solid molecular evidence strongly supports the preferential solvation of Li+ by EC. Besides, from the negative spectra, we also found that PF6- forms association with EC, which has been neglected by previous studies due to the relatively weak interaction. In both LiFSI in DME electrolytes, however, no evidence shows that FSI- is associated with DME. Furthermore, strong salt ion cluster signals were observed in the 1.0 M LiPF6 in EC DMC electrolyte, suggesting that a significant amount of Li+ ions stay in the vicinity of anions. In sharp comparison, weak ion cluster signals were detected in dilute LiFSI in DME electrolyte, suggesting most ions are well separated, in agreement with our molecular dynamics simulation results. These findings indicate that with virtues of little bias on detecting positive and negative ions and the capability of directly analyzing concentrated electrolytes, in situ liquid SIMS is a powerful tool that can provide key evidence for improved understanding on the ion solvent interactions in nonaqueous electrolytes. Therefore, we anticipate wide applications of in situ liquid SIMS on investigations of various ion solvent interactions in the near future.
学科主题	Chemistry
语种	英语
内容类型	期刊论文
源URL	[http://ir.itp.ac.cn/handle/311006/22940]
专题	理论物理研究所_理论物理所1978-2010年知识产出
作者单位	1.Chinese Acad Sci, Beijing Natl Lab Mol Sci, Natl Ctr Mass Spectrometry Beijing, CAS Key Lab Analyt Chem Living Biosyst,Inst Chem, Beijing 100190, Peoples R China 2.Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA 3.Pacific Northwest Natl Lab, Computat Math Grp, Phys & Computat Sci Directorate, Richland, WA 99354 USA 4.Pacific Northwest Natl Lab, Energy Proc & Mat Div, Energy & Environm Directorate, Richland, WA 99354 USA 5.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 6.Chinese Acad Sci, Inst Theoret Phys, CAS Key Lab Theoret Phys, 55 East Zhongguancun Rd,POB 2735, Beijing 100190, Peoples R China 7.Shandong Univ, Sch Phys, State Key Lab Crystal Mat, Jinan 250100, Shandong, Peoples R China 8.Shandong Univ, Key Lab Particle Phys & Particle Irradiat MOE, Jinan 250100, Shandong, Peoples R China 9.US Army Res Lab, Electrochem Branch, Power & Energy Div, Sensor & Electron Devices Directorate, Adelphi, MD 20783 USA
推荐引用方式 GB/T 7714	Borodin, O,Zhang, YY,Su, M,et al. Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS[J]. ANALYTICAL CHEMISTRY,2018,90(5):3341-3348.
APA	Borodin, O.,Zhang, YY.,Su, M.,Yu, XF.,Zhou, YF.,...&Zhu, ZH.(2018).Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS.ANALYTICAL CHEMISTRY,90(5),3341-3348.
MLA	Borodin, O,et al."Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS".ANALYTICAL CHEMISTRY 90.5(2018):3341-3348.