In-situ formed Co nano-clusters as separator modifier and catalyst to regulate the film-like growth of Li and promote the cycling stability of lithium metal batteries

Zhenjia Wang; Yongji Xia; Yana Li; Tianle Mao; Zheyu Hong; Jiajia Han; Dong-Liang Peng; Guanghui Yue

doi:10.1016/j.jcis.2024.01.020

In-situ formed Co nano-clusters as separator modifier and catalyst to regulate the film-like growth of Li and promote the cycling stability of lithium metal batteries

J Colloid Interface Sci. 2024 Apr 15:660:226-234. doi: 10.1016/j.jcis.2024.01.020. Epub 2024 Jan 11.

Authors

Zhenjia Wang¹, Yongji Xia¹, Yana Li¹, Tianle Mao¹, Zheyu Hong¹, Jiajia Han², Dong-Liang Peng¹, Guanghui Yue³

Affiliations

¹ State Key Lab of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen 361005, China.
² State Key Lab of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen 361005, China. Electronic address: jiajiahan@xmu.edu.cn.
³ State Key Lab of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen 361005, China. Electronic address: yuegh@xmu.edu.cn.

PMID: 38244491
DOI: 10.1016/j.jcis.2024.01.020

Abstract

Lithium metal batteries (LMBs) are considered a highly prospective next-generation energy storage technology. However, their large-scale commercial application is hampered by the uncontrollable growth of Li dendrites, which accompany the boundless inflation of the battery's volume. In this study, we address this challenge by fabricating a porous structure of the MOF-derived CoP nanocube film (CoP-NC@PP) as a adorned layer for the separator. During the initial cycle, this film facilitates the in situ formation of Li₃P with ultrahigh ionic conductivity and a lithiophilic Co, which helps rule the nucleation and deposition behavior of lithium and stabilizes the solid-electrolyte interphase. The symmetric cell incorporating the CoP-NC@PP modified layer exhibits exceptional cycling stability, surpassing 1500 h of continuous operation. The kinetic process of Li interaction with CoP and the structural factors contributing to the high cycling stability and high naminal voltage were investigated by molecular dynamics simulation and density functional theory calculations. Furthermore, full cells employing Li||CoP-NC@PP||LFP (LFP = LiFePO₄) configurations demonstrate excellent cycling stability and high capacity, even at a high rate of 5 C (≈5.2 mA cm^-2), with the cathode mass loading reaching as high as 10.3 mg cm^-2.