Beyond LiF: Tailoring Li2O-Dominated Solid Electrolyte Interphase for Stable Lithium Metal Batteries

法拉第效率 电解质 锂(药物) 材料科学 电化学 化学工程 阴极 相间 溶剂化 电池(电) 金属锂 金属 纳米技术 电极 化学 离子 物理化学 有机化学 工程类 物理 内分泌学 生物 功率(物理) 冶金 医学 量子力学 遗传学
作者
Huipeng Zeng,Kai Yu,Jiawei Li,Mingman Yuan,Junjie Wang,Qingrong Wang,Anjie Lai,Yidong Jiang,Yan Xu,Guangzhao Zhang,Hongli Xu,Jun Wang,Wei Huang,Chaoyang Wang,Yonghong Deng,Shang‐Sen Chi
出处
期刊:ACS Nano [American Chemical Society]
卷期号:18 (3): 1969-1981 被引量:97
标识
DOI:10.1021/acsnano.3c07038
摘要

The components and structures of the solid-electrolyte interphase (SEI) are critical for stable cycling of lithium metal batteries (LMBs). LiF has been widely studied as the dominant component of SEI, but Li2O, which has a much lower diffusion barrier for Li+, has rarely been investigated as the dominant component of SEI. The effect of Li2O-dominated SEI on electrochemical performance still remains elusive. Herein, an ultrastrong coordinated cosolvation diluent, 2,3-difluoroethoxybenzene (DFEB), is designed to modulate solvation structure and tailor Li2O-dominated SEI for stable LMBs. In the DFEB-based LHCE (DFEB-LHCE), DFEB intensively participates in the first solvation shell and synergizes with FSI– to tailor an Li2O-dominated inorganic-rich SEI which is different from the LiF-dominated SEI formed in conventional LHCE. Benefiting from this special SEI architecture, a high Coulombic efficiency (CE) of 99.58% in Li||Cu half cells, stable voltage profiles, and dense and uniform lithium deposition, as well as effective inhibition of Li dendrite formation in the symmetrical cell, are achieved. More importantly, the DFEB-LHCE can be matched with various cathodes such as LFP, NCM811, and S cathodes, and the Li||LFP full cell using DFEB-LHCE possesses 85% capacity retention after 650 stable cycles with 99.9% CE. Especially the 1.5 Ah practical lithium metal pouch cell achieves an excellent capacity retention of 89% after 250 cycles with a superb average CE of 99.93%. This work unravels the superiority of the Li2O-dominated SEI and the feasibility of tailoring SEI components through modulation of solvation structures.
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