Engineering Solid Electrolyte Interphase Composition by Assessing Decomposition Pathways of Fluorinated Organic Solvents in Lithium Metal Batteries

Zhang, Yumin; Krishnamurthy, Dilip; Viswanathan, Venkatasubramanian

doi:10.1149/1945-7111/ab836b

Engineering Solid Electrolyte Interphase Composition by Assessing Decomposition Pathways of Fluorinated Organic Solvents in Lithium Metal Batteries

Journal Article · Wed Apr 08 00:00:00 EDT 2020 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ab836b· OSTI ID:1608726

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Studies have shown fluorinated electrolyte solvents can form desirable solid electrolyte interphase (SEI) in lithium metal batteries. In this study, we develop a detailed mechanistic understanding of two high performing electrolytes, Fluoroethylene Carbonate (FEC) and Difluoroethylene Carbonate (DFEC) to demonstrate minimal structural variations can lead to different decomposition products, and thereby the nature of the SEI. Using density functional theory (DFT) calculations, we find different initial bond-breaking mechanisms between FEC and DFEC. We develop free energy diagrams for the decomposition pathways including both electrochemical and chemical steps. Using the computational Li electrode, we identify the largest limiting potential of 1.77 V for FEC decomposition, associated with the formation of lithium fluoride, lithium oxide and FEC oligomers, and 1.53 V for DFEC, which correspond to the formation of polymerized vinylene carbonate and lithium fluoride. We suggest the formation of oligomers in the case of FEC instead of long polymers may lead to better SEI compactness. We also demonstrate the SEI components of FEC and DFEC are not stable on typical cathode voltage (3.87 V). This study presents a unified electrocatalytic perspective on SEI formation and decomposition.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: EE0007810

OSTI ID:: 1608726

Alternate ID(s):: OSTI ID: 1799385

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 7 Vol. 167; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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