Issue 39, 2023

Improvement of the Li metal-electrolyte interfacial stability by cistrans polar conformer formation in a carbonate electrolyte

Abstract

With the modulation of the Li-salt, linear carbonate solvents undergo spontaneous transformation of the molecular structure as a consequence of an electrolyte engineering process to improve the cathodic stability of the carbonate electrolyte. The cistrans dimethyl carbonate (ctDMC) electrolyte has a higher lowest unoccupied molecular orbital (LUMO) energy level than the typical ciscis DMC (ccDMC), which suggests that controlling the salt concentration can enhance the reduction stability of carbonate electrolytes due to a LUMO shift. The shifted LUMO level promotes the nucleation-growth of the Li deposits by reducing the development of an SEI layer on the Li metal and increasing the charge transfer kinetics. While severe electrolyte consumption is demonstrated with conventional carbonates from porously grown lithium and the limited cathodic stability of the bulk electrolyte, dense Li deposits are formed with the conformer electrolyte, which reduces the electrolyte decomposition on the deposited Li surface. As a consequence, the conformer-based electrolyte is used to demonstrate lithium metal battery cycleability associated with a high areal capacity positive electrode.

Graphical abstract: Improvement of the Li metal-electrolyte interfacial stability by cis–trans polar conformer formation in a carbonate electrolyte

Supplementary files

Article information

Article type
Paper
Submitted
05 Aug 2023
Accepted
09 Sep 2023
First published
11 Sep 2023

J. Mater. Chem. A, 2023,11, 21244-21250

Improvement of the Li metal-electrolyte interfacial stability by cistrans polar conformer formation in a carbonate electrolyte

M. A. Lee, H. J. Leem, J. B. Lee, C. Hwang, J. Yu and H. Kim, J. Mater. Chem. A, 2023, 11, 21244 DOI: 10.1039/D3TA04673G

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