A "tug-of-war" effect tunes Li-ion transport and enhances the rate capability of lithium metal batteries. Issue 10 (22nd February 2023)

• Record Type: Journal Article
• Authors: Zhang, Han; Zeng, Ziqi; Liu, Mengchuang; Ma, Fenfen; Qin, Mingsheng; Wang, Xinlan; Wu, Yuanke; Lei, Sheng; Cheng, Shijie; Xie, Jia
• Is Part Of: Chemical science. Volume 14:Issue 10(2023)
• Page Start: 2745
• Page End: 2754
• Publication Date: 2023-02-22
• Subjects: Chemistry -- Periodicals; 540.5
• DOI: 10.1039/d2sc06620c
• Languages: English
• ISSNs: 2041-6520

Abstract

Abstract : We discovered a "tug-of-war" effect in a multilayer solvation sheath: direct solvent–nonsolvent and indirect Li + –nonsolvent interactions were leveraged to tune binding energy between Li + and solvent, thereby leading to a loosened solvation sheath. 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.