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DOI	10.1073/pnas.2020357118
	Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries
	Cao X.; Gao P.; Ren X.; Zou L.; Engelhard M.H.; Matthews B.E.; Hu J.; Niu C.; Liu D.; Arey B.W.; Wang C.; Xiao J.; Liu J.; Xu W.; Zhang J.-G.
发表日期	2021
ISSN	00278424
卷号	118 期号:9
英文摘要	Electrolyte is very critical to the performance of the high-voltage lithium (Li) metal battery (LMB), which is one of the most attractive candidates for the next-generation high-density energy-storage systems. Electrolyte formulation and structure determine the physical properties of the electrolytes and their interfacial chemistries on the electrode surfaces. Localized high-concentration electrolytes (LHCEs) outperform state-of-the-art carbonate electrolytes in many aspects in LMBs due to their unique solvation structures. Types of fluorinated cosolvents used in LHCEs are investigated here in searching for the most suitable diluent for high-concentration electrolytes (HCEs). Nonsolvating solvents (including fluorinated ethers, fluorinated borate, and fluorinated orthoformate) added in HCEs enable the formation of LHCEs with high-concentration solvation structures. However, low-solvating fluorinated carbonate will coordinate with Li+ ions and form a second solvation shell or a pseudo-LHCE which diminishes the benefits of LHCE. In addition, it is evident that the diluent has significant influence on the electrode/electrolyte interphases (EEIs) beyond retaining the high-concentration solvation structures. Diluent molecules surrounding the high-concentration clusters could accelerate or decelerate the anion decomposition through coparticipation of diluent decomposition in the EEI formation. The varied interphase features lead to significantly different battery performance. This study points out the importance of diluents and their synergetic effects with the conductive salt and the solvating solvent in designing LHCEs. These systematic comparisons and fundamental insights into LHCEs using different types of fluorinated solvents can guide further development of advanced electrolytes for high-voltage LMBs. © This open access article is distributed under Creative Commons Attribution-NonCommercialNoDerivatives License 4.0 (CC BY-NC-ND).
英文关键词	Diluent; Interphase; LHCE; Lithium metal batteries; Solvation structure
语种	英语
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/180497
作者单位	Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, United States; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, United States; Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354, United States; Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
推荐引用方式 GB/T 7714	Cao X.,Gao P.,Ren X.,et al. Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries[J],2021,118(9).
APA	Cao X..,Gao P..,Ren X..,Zou L..,Engelhard M.H..,...&Zhang J.-G..(2021).Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries.Proceedings of the National Academy of Sciences of the United States of America,118(9).
MLA	Cao X.,et al."Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries".Proceedings of the National Academy of Sciences of the United States of America 118.9(2021).