Manganese and Cobalt-Free Ultrahigh-Ni-Rich Single-Crystal Cathode for High-Performance Lithium Batteries

Adil Saleem; He Zhu; Muhammad K Majeed; Rashid Iqbal; Bushra Jabar; Arshad Hussain; M Zeeshan Ashfaq; Muhammad Ahmad; Sajid Rauf; Jean Pierre Mwizerwa; Jun Shen; Qi Liu

doi:10.1021/acsami.2c19687

Manganese and Cobalt-Free Ultrahigh-Ni-Rich Single-Crystal Cathode for High-Performance Lithium Batteries

ACS Appl Mater Interfaces. 2023 May 3;15(17):20843-20853. doi: 10.1021/acsami.2c19687. Epub 2023 Apr 17.

Authors

Adil Saleem^{1

2}, He Zhu³, Muhammad K Majeed⁴, Rashid Iqbal⁵, Bushra Jabar^{1

2}, Arshad Hussain⁵, M Zeeshan Ashfaq⁶, Muhammad Ahmad⁵, Sajid Rauf⁵, Jean Pierre Mwizerwa^{1

2}, Jun Shen^{1

7}, Qi Liu⁸

Affiliations

¹ College of Mechatronics and Control Engineering, Shenzhen University, Shenzhen 518060, China.
² Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province, College of Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China.
³ Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
⁴ Materials Chemistry Laboratory, Department of Materials Science & Engineering, The University of Texas at Arlington, Arlington 76019-0019, Texas, United States.
⁵ Institute for Advanced Study, College of Electronic and Information Engineering, Shenzhen University, Shenzhen 518060, Guangdong, China.
⁶ School of Materials Science and Engineering, Shandong University, Jinan 250061, China.
⁷ Guangdong Key Laboratory of Electromagnetic Control and Intelligent Robots, Shenzhen 518060, China.
⁸ Department of Physics, City University of Hong Kong, Kowloon Tong, Kowloon, Hong Kong SAR, China.

PMID: 37138461
DOI: 10.1021/acsami.2c19687

Abstract

Current commercial nickel (Ni)-rich Mn, Co, and Al-containing cathodes are employed in high-energy-density lithium (Li) batteries all around the globe. The presence of Mn/Co in them brings out several problems, such as high toxicity, high cost, severe transition-metal dissolution, and quick surface degradation. Herein, a Mn/Co-free ultrahigh-Ni-rich single-crystal LiNi_0.94Fe_0.05Cu_0.01O₂ (SCNFCu) cathode with acceptable electrochemical performance is benchmarked against a Mn/Co-containing cathode. Despite having a slightly lower discharge capacity, the SCNFCu cathode retaining 77% of its capacity across 600 deep cycles in full-cell outperforms comparable to a high-Ni single-crystal LiNi_0.9Mn_0.05Co_0.05O₂ (SCNMC; 66%) cathode. It is shown that the stabilizing ions Fe/Cu in the SCNFCu cathode reduce structural disintegration, undesirable side reactions with the electrolyte, transition-metal dissolution, and active Li loss. This discovery provides a new extent for cathode material development for next-generation high-energy, Mn/Co-free Li batteries due to the compositional tuning flexibility and quick scalability of SCNFCu, which is comparable to the SCNMC cathode.

Keywords: Mn/Co-free cathode; Ni-rich cathode; cathode−electrolyte interphase; lithium batteries; single-crystal.