Suppressed Lattice Oxygen Release via Ni/Mn Doping from Spent LiNi0.5Mn0.3Co0.2O2 toward High-Energy Layered-Oxide Cathodes

Kai Jia; Junxiong Wang; Jun Ma; Zheng Liang; Zhaofeng Zhuang; Guanjun Ji; Runhua Gao; Zhihong Piao; Chuang Li; Guangmin Zhou; Hui-Ming Cheng

doi:10.1021/acs.nanolett.2c03090

Suppressed Lattice Oxygen Release via Ni/Mn Doping from Spent LiNi_0.5Mn_0.3Co_0.2O₂ toward High-Energy Layered-Oxide Cathodes

Nano Lett. 2022 Oct 26;22(20):8372-8380. doi: 10.1021/acs.nanolett.2c03090. Epub 2022 Sep 23.

Authors

Kai Jia^{1

2}, Junxiong Wang^{1

2}, Jun Ma², Zheng Liang¹, Zhaofeng Zhuang², Guanjun Ji^{1

2}, Runhua Gao², Zhihong Piao², Chuang Li², Guangmin Zhou², Hui-Ming Cheng^{3

4}

Affiliations

¹ Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
² Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.
³ Faculty of Materials Science and Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Science, Shenzhen 518055, China.
⁴ Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China.

PMID: 36149367
DOI: 10.1021/acs.nanolett.2c03090

Abstract

LiCoO₂ has suffered from poor stability under high voltage as a result of insufficient Co-O bonding that causes lattice oxygen release and lattice distortions. Herein, we fabricated a high-voltage LiCoO₂ at 4.6 V by doping with Ni/Mn atoms, which are obtained from spent LiNi_0.5Mn_0.3Co_0.2O₂ cathode materials. The as-prepared high-voltage LiCoO₂ with Ni/Mn substitutional dopants in the Co layer enhances Co-O bonding that suppresses oxygen release and harmful phase transformation during delithiation, thus stabilizing the layered structure and leading to a superior electrochemical performance at 4.6 V. The pouch cell of modified LiCoO₂ exhibits a capacity retention of 85.1% over 100 cycles at 4.5 V (vs graphite). We found that our strategy is applicable for degraded LiCoO₂, and the regenerated LiCoO₂ using this strategy exhibits excellent capacity retention (84.1%, 100 cycles) at 4.6 V. Our strategy paves the way for the direct conversion of spent batteries into high-energy-density batteries.

Keywords: Degraded LiCoO2; Enhanced Co−O bonding; High-voltage LiCoO2; Lattice oxygen release; Spent LiNi0.5Mn0.3Co0.2O2 cathode materials.