Issue 10, 2023

A “tug-of-war” effect tunes Li-ion transport and enhances the rate capability of lithium metal batteries

Abstract

“Solvent-in-salt” electrolytes (high-concentration electrolytes (HCEs)) and diluted high-concentration electrolytes (DHCEs) show great promise for reviving secondary lithium metal batteries (LMBs). However, the inherently sluggish Li+ transport of such electrolytes limits the high-rate capability of LMBs for practical conditions. Here, we discovered a “tug-of-war” effect in a multilayer solvation sheath that promoted the rate capability of LMBs; the pulling force of solvent–nonsolvent interactions competed with the compressive force of Li+-nonsolvent interactions. By elaborately manipulating the pulling and compressive effects, the interaction between Li+ and the solvent was weakened, leading to a loosened solvation sheath. Thereby, the developed electrolytes enabled a high Li+ transference number (0.65) and a Li (50 μm)‖NCM712 (4 mA h cm−2) full cell exhibited long-term cycling stability (160 cycles; 80% capacity retention) at a high rate of 0.33C (1.32 mA cm−2). Notably, Li (50 μm)‖LiFePO4 (LFP; 17.4 mg cm−2) cells with a designed electrolyte reached a capacity retention of 80% after 1450 cycles at a rate of 0.66C. An 6 Ah Li‖LFP pouch cell (over 250 W h kg−1) showed excellent cycling stability (130 cycles, 96% capacity retention) under practical conditions. This design concept for an electrolyte provides a promising path to build high-energy-density and high-rate LMBs.

Graphical abstract: A “tug-of-war” effect tunes Li-ion transport and enhances the rate capability of lithium metal batteries

Supplementary files

Article information

Article type
Edge Article
Submitted
02 Dec 2022
Accepted
02 Jan 2023
First published
07 Feb 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2023,14, 2745-2754

A “tug-of-war” effect tunes Li-ion transport and enhances the rate capability of lithium metal batteries

H. Zhang, Z. Zeng, M. Liu, F. Ma, M. Qin, X. Wang, Y. Wu, S. Lei, S. Cheng and J. Xie, Chem. Sci., 2023, 14, 2745 DOI: 10.1039/D2SC06620C

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