Electron Delocalization Enables Sulfone-based Single-solvent Electrolyte for Lithium Metal Batteries

Rahman, Muhammad Mominur; Hu, Enyuan

doi:10.1002/ange.202311051

Title: Electron Delocalization Enables Sulfone-based Single-solvent Electrolyte for Lithium Metal Batteries

Journal Article · 13 September 2023 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202311051 · OSTI ID:2008213

Rahman, Muhammad Mominur ^[1];

^[1]

Brookhaven National Laboratory (BNL), Upton, NY (United States)

Abstract Li‐metal batteries (LMB), although providing high energy density, face the grand challenge of identifying good electrolyte solvents for cycling. Common solvents are either only stable against lithium metal anode or only stable against LiNi _x Mn _y Co _{1‐ x ‐ y} O ₂ (NMC) cathode. There is significant effort trying to increase the cathode stability for ether electrolytes, which are in general stable against lithium metal anode. In comparison, there is much less effort trying to increase the anode stability of electrolytes that are stable against NMC cathode. One example is the sulfone‐based electrolyte. It has good cathode stability but is hindered from practical application because of (1) high viscosity and poor wetting capability and (2) poor anode stability. Here, we solve these issues by modifying the sulfone molecules using resonance and electron withdrawing effect. The viscosity is significantly reduced by delocalizing the electrons through introducing additional oxygen on the molecular backbone and applying appropriate fluorination. The resulting molecule 2,2,2‐trifluoroethyl mesylate (TFEM) has decreased Lewis basicity and less reactivity toward Li ⁺ . The electrolyte based on TFEM as single solvent enables cycling of LMB under harsh conditions of low N/P ratio (21 mg/cm ² NMC811 and 50 μm Li) with 90 % capacity retention after 160 cycles at C/3 discharge rate.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 2008213

Alternate ID(s):: OSTI ID: 2005011

Report Number(s):: BNL-224881-2023-JAAM

Journal Information:: Angewandte Chemie, Vol. 135, Issue 44; ISSN 0044-8249

Publisher:: German Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Electron Delocalization Enables Sulfone-based Single-solvent Electrolyte for Lithium Metal Batteries

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