首页|Efficient Chemical Prelithiation with Modificatory Li+Solvation Structure Enabling Spatially Homogeneous SEI toward High Performance SiOx Anode

Efficient Chemical Prelithiation with Modificatory Li+Solvation Structure Enabling Spatially Homogeneous SEI toward High Performance SiOx Anode

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Chemical prelithiation is widely proven to be an effective strategy to address the low initial coulombic efficiency(ICE)of promising SiOx anode.Though the reagent composition has been widely explored,the Li+solvation structure,which practically plays the cornerstone role in the prelithiation ability,rate,uniformility,has rarely been explored.A novel environmentally-friendly reagent with weak solvent cyclopentyl methyl ether(CPME)is proposed that enables both improved ICE and spatial homogeneous solid electrolyte interphase(SEI).And the prelithiation behavior and mechanism were explored focused on the Li+solvation structure.Both theoretical investiga-tion and spectroscopic results suggest that weak solvent feature of CPME reduces the solvent coordination number and decreases the Li+desolvation energy.The optimized Li+solvation structure enables high-efficiency prelithiation that ensures the horizontal homoge-nization and mechanical properties of SEI.Moreover,the accompanied CPME molecules preferentially occupy positions in initial SEI,reducing the likelihood of LiPF6 decomposition and promoting longitudinal homogenization of SEI.Consequently,the efficient and homogenous prelithiation enables impressive ICE of 109.52％and improved cycling performance with 80.77％retained after 300 cycles via just 5 min soaking.Furthermore,the full cells with LiNi0.83Co0.12Mn0.05O2(NCM831205)cathode display an enhancement in the en-ergy density of 179.74％and up to 648.35 Wh·kg-1.

Lithium-ion batterySiOx anodePrelithiationWeak solventHomogeneous SEIEnergy conversionDesolvation energy

Ruoyang Wang、Yuqing Wu、Yifan Niu、Qing Yang、Haoyu Li、Yang Song、Benhe Zhong、Liwen Yang、Ting Chen、Zhenguo Wu、Xiaodong Guo

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School of Chemical Engineering,Sichuan University,Chengdu,Sichuan 610065,China

Chengdu No.7 High School,Chengdu,Sichuan 6100412,China

Institute for Applied Materials(IAM),Karlsruhe Institute of Technology(KIT),Hermann-von-Helmholtz-Platz 1,D-76344 Eggenstein-Leopoldshafen,Germany

Institute for Advanced Study,Chengdu University,Chengdu,Sichuan 610106,China

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2024

10.1002/cjoc.202400226

中国化学(英文版)
中国化学会 上海有机化学研究所

中国化学(英文版)

CSTPCD
影响因子：0.848
ISSN：1001-604X
年,卷(期)：2024.42(17)