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

Zeng，Huipeng1; Yu，Kai1; Li，Jiawei2; Yuan，Mingman1; Wang，Junjie1; Wang，Qingrong1; Lai，Anjie1; Jiang，Yidong1; Yan，Xu1; Zhang，Guangzhao1; Xu，Hongli1; Wang，Jun1; Huang，Wei3; Wang，Chaoyang4; Deng，Yonghong1; Chi，Shang Sen1

2024-01-23

10.1021/acsnano.3c07038

ACS Nano   影响因子和分区

1936-0851

1936-086X

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 LiO, which has a much lower diffusion barrier for Li, has rarely been investigated as the dominant component of SEI. The effect of LiO-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 LiO-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 LiO-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 LiO-dominated SEI and the feasibility of tailoring SEI components through modulation of solvation structures.

cosolventization lithium metal batteries lithium oxide localized high-concentration electrolytes solid electrolyte interphase solvation structures

SCI ; EI

英语

第一 ; 通讯

2-s2.0-85182560113

Scopus

1.Department of Materials Science and Engineering,School of Innovation and Entrepreneurship,Southern University of Science and Technology,Shenzhen,518055,China
2.Key Laboratory of Marine Environmental Corrosion and Bio-Fouling,Institute of Oceanology,Chinese Academy of Sciences,Qingdao,266071,China
3.National Center for Applied Mathematics Shenzhen (NCAMS,Digital Economy Research Center─DeFin),College of Business,Southern University of Science and Technology,Shenzhen,518055,China
4.Research Institute of Materials Science,South China University of Technology,Guangzhou,510640,China

Zeng，Huipeng,Yu，Kai,Li，Jiawei,et al. Beyond LiF: Tailoring Li2O-Dominated Solid Electrolyte Interphase for Stable Lithium Metal Batteries[J]. ACS Nano,2024,18(3):1969-1981.

Zeng，Huipeng.,Yu，Kai.,Li，Jiawei.,Yuan，Mingman.,Wang，Junjie.,...&Chi，Shang Sen.(2024).Beyond LiF: Tailoring Li2O-Dominated Solid Electrolyte Interphase for Stable Lithium Metal Batteries.ACS Nano,18(3),1969-1981.

Zeng，Huipeng,et al."Beyond LiF: Tailoring Li2O-Dominated Solid Electrolyte Interphase for Stable Lithium Metal Batteries".ACS Nano 18.3(2024):1969-1981.