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Wide-temperature-range operation of lithium-metal batteries using partially and weakly solvating liquid electrolytes†
Saehun Kim,Jeong-A Lee,Tae Kyung Lee,Kyungeun Baek,Juyoung Kim,Boguen Kim,Jeong Hwan Byun,Hyun-Wook Lee,Seok Ju Kang,Ji-Ae Choi,So-Young Lee,Moon-Hyung Choi,Jong-Hyun Lee,Nam-Soon Choi
Energy & Environmental Science Pub Date : 09/13/2023 00:00:00 , DOI:10.1039/D3EE02106H
Abstract

The optimal design of liquid electrolytes is vital for the build-up of long-lifespan lithium-metal batteries (LMBs) that function over a wide-temperature-range. Tuning the electrolyte solvation-structure using partially-fluorinated ether solvents and constructing stable electrode–electrolyte interfaces using electrolyte additives enhance the electrochemical reversibility of lithium-metal anodes and facilitate the realization of high-capacity cathodes for LMBs. This study reports a partially and weakly solvating electrolyte (PWSE) which enables the stable cycling of LMBs at high-voltages within a wide-temperature range through modulation of an electrolyte local-environment using a low-salt concentration of 1.3 M. 1,2-Bis(1,1,2,2-tetrafluoroethoxy)ethane contains two oxygen atoms that coordinate weakly with Li+-ions; it transforms the 1,2-dimethoxyethane-dominated electrolyte solvation-structure to a more anion-incorporated structure. Moreover, a combination of lithium fluoromalonato(difluoro)borate and silver nitrate strengthens the electrode–electrolyte interfaces and improves the oxidation durability of ether-based electrolytes. The PWSE enables the construction of 4.4 V Li|LiCoO2 full cells with a long-lifespan and high-areal-capacity of 3.12 mA h cm−2.

Graphical abstract: Wide-temperature-range operation of lithium-metal batteries using partially and weakly solvating liquid electrolytes
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