High interfacial-energy heterostructure facilitates large-sized lithium nucleation and rapid Li+ desolvation process

Zhipeng Wen; Yuanhong Kang; Qilong Wu; Xiu Shen; Pengbin Lai; Yang Yang; Cheng Chao Li; Jinbao Zhao

doi:10.1016/j.scib.2022.11.026

High interfacial-energy heterostructure facilitates large-sized lithium nucleation and rapid Li⁺ desolvation process

Sci Bull (Beijing). 2022 Dec 31;67(24):2531-2540. doi: 10.1016/j.scib.2022.11.026. Epub 2022 Nov 25.

Authors

Zhipeng Wen¹, Yuanhong Kang², Qilong Wu², Xiu Shen², Pengbin Lai², Yang Yang³, Cheng Chao Li⁴, Jinbao Zhao⁵

Affiliations

¹ School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China; State Key Lab of Physical Chemistry of Solid Surfaces, Collaborative Innovation Centre of Chemistry for Energy Materials, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
² State Key Lab of Physical Chemistry of Solid Surfaces, Collaborative Innovation Centre of Chemistry for Energy Materials, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
³ State Key Lab of Physical Chemistry of Solid Surfaces, Collaborative Innovation Centre of Chemistry for Energy Materials, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China. Electronic address: yangyang419@xmu.edu.cn.
⁴ School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China. Electronic address: licc@gdut.edu.cn.
⁵ State Key Lab of Physical Chemistry of Solid Surfaces, Collaborative Innovation Centre of Chemistry for Energy Materials, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China. Electronic address: jbzhao@xmu.edu.cn.

PMID: 36604031
DOI: 10.1016/j.scib.2022.11.026

Abstract

High interfacial energy Li⁰-electrolyte interface contributes to larger Li⁰ nucleation embryos and a more stable interface, so the interfacial energy is essential for highly reversible Li⁰ deposition/stripping. Herein, a high interfacial-energy artificial solid electrolyte interphase (SEI) with rich LiF embedded in lithiated poly-2-acrylamido-2-methylpropane sulfonic acid (PAMPS-Li) network is designed to realize favorable Li⁰ nucleation and rapid desolvation of Li⁺ simultaneously. The Li-F bonds in LiF (001) exhibit stronger ion-dipole interactions with Li atoms, offering higher interfacial energies. When the growth surface energy and total interfacial energy of Li⁰ are balanced, the high interfacial energy SEI with abundant LiF can promote the formation of larger Li⁰ nucleation embryos. In addition, the PAMPS-Li with immobilized anions presents weaker interaction with Li⁰ and possesses higher polymer-Li interfacial energy, and its amide and sulfonic acid groups exhibit higher binding energies with Li⁺. Therefore, PAMPS-Li can easily promote the Li⁺ to escape from the solvent sheath and weaken the desolvation energy barrier. The highly reversible Li⁰ deposition behavior with restricted side reactions is achieved based on the synergistic modification of high interfacial energy SEI with heterostructure. Most importantly, lifespan of multi-layered Li⁰ pouch cell (330 Wh kg^-1) with a low N/P ratio (1.67) is over 100 cycles, verifying its potential practical application.

Keywords: Crystalline LiF-rich; High interfacial energy; Large metallic Li(0) nucleate size; Pouch cell; Rapid Li(+) desolvation.