Structural Regulation Enables High Interfacial Functionality for Ni-Rich Single-Crystalline Cathodes

Pei Liu; Haoran Wei; Tao Huang; Zhencheng Huang; Lingli Chen; Xuanlong He; Yuying Liu; Hongkai Yang; Mijie Liu; Shenghua Ye; Xuming Yang; Zhanhua Wu; Yaming Liu; Qingqing Jia; XiaoBai Ma; Jing Chen; Xiangzhong Ren; Xiaoping Ouyang; Jianhong Liu; Qianling Zhang; Jiangtao Hu

doi:10.1021/acsami.4c10398

Structural Regulation Enables High Interfacial Functionality for Ni-Rich Single-Crystalline Cathodes

ACS Appl Mater Interfaces. 2024 Sep 24. doi: 10.1021/acsami.4c10398. Online ahead of print.

Authors

Pei Liu¹, Haoran Wei¹, Tao Huang², Zhencheng Huang¹, Lingli Chen¹, Xuanlong He¹, Yuying Liu¹, Hongkai Yang³, Mijie Liu⁴, Shenghua Ye¹, Xuming Yang¹, Zhanhua Wu⁵, Yaming Liu⁵, Qingqing Jia⁵, XiaoBai Ma⁵, Jing Chen⁵, Xiangzhong Ren¹, Xiaoping Ouyang⁶, Jianhong Liu^{1

7}, Qianling Zhang¹, Jiangtao Hu¹

Affiliations

¹ Graphene Composite Research Center, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, China.
² College of Energy Engineering, Zhejiang University, Hangzhou, Zhejiang 310027, China.
³ School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, China.
⁴ BASIS Bilingual School Shenzhen, Nanshan District, Shenzhen 518067, China.
⁵ China Institute of Atomic Energy, Beijing 102413, China.
⁶ School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China.
⁷ Shenzhen Eigen-Equation Graphene Technology Co., Ltd, Shenzhen 518000, China.

PMID: 39316669
DOI: 10.1021/acsami.4c10398

Abstract

Ni-rich single-crystalline layered cathodes have garnered significant attention due to their high energy density and thermal stability. However, they experience severe capacity degradation caused by lattice strain and interfacial side reactions during practical applications. In this study, an effective yttrium modification method is employed to stabilize the structure of Ni-rich single-crystalline LiNi_0.83Mn_0.05Co_0.12O₂ (SC-NMC83) to solve these issues. This innovative approach successfully immobilizes oxygen within the material, preventing crack formation while simultaneously broadening the diffusion path of Li⁺. The yttrium-modified sample (SC-NMC83-Y) exhibits a superior capacity retention compared to the SC-NMC83 sample, with values of 90% and 76.1% after 100 cycles, respectively. This work demonstrates the promising potential of a doping strategy for Ni-rich single-crystalline cathodes and paves a pathway for its practical implementation, such as all-solid-state batteries.

Keywords: Ni-rich cathode; engineering CEI; low migration energy barrier; structural stability; yttrium modification.