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

Author:

Wang Ruoyang1,Wu Yuqing1,Niu Yifan2,Yang Qing1,Li Haoyu1,Song Yang1,Zhong Benhe1,Yang Liwen3,Chen Ting4,Wu Zhenguo1,Guo Xiaodong14

Affiliation:

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

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

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

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

Abstract

Comprehensive SummaryChemical 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 investigation 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 homogenization 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 energy density of 179.74% and up to 648.35 Wh·kg–1.

Funder

State Key Laboratory of Polymer Materials Engineering

National Natural Science Foundation of China

Science and Technology Department of Sichuan Province

Publisher

Wiley

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