ITP OpenIR  > SCI期刊论文
Zhang, YY; Su, M2,4,5; Yu, XF; Zhou, YF; Wang, JG; Cao, RG; Xu, W3; Wang, CM; Baer, DR; Borodin, O8; Xu, K8; Wang, YT; Wang, XL; Xu, ZJ; Wang, FY; Zhu, ZH
Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS
AbstractIon 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.
Subject AreaChemistry
MOST Discipline CatalogueChemistry, Analytical
Indexed BySCIE
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Cited Times:9[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Affiliation1.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
Recommended Citation
GB/T 7714
Zhang, YY,Su, M,Yu, XF,et al. Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS[J]. ANALYTICAL CHEMISTRY,2018,90(5):3341-3348.
APA Zhang, YY.,Su, M.,Yu, XF.,Zhou, YF.,Wang, JG.,...&Zhu, ZH.(2018).Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS.ANALYTICAL CHEMISTRY,90(5),3341-3348.
MLA Zhang, YY,et al."Investigation of Ion-Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS".ANALYTICAL CHEMISTRY 90.5(2018):3341-3348.
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