Thermochemical Cyclization Constructs Bridged Dual-Coating of Ni-Rich Layered Oxide Cathodes for High-Energy Li-Ion Batteries

Jing Wang; Qiang Yuan; Zhixin Ren; Chunhao Sun; Junfan Zhang; Ran Wang; Mengmeng Qian; Qi Shi; Ruiwen Shao; Daobin Mu; Yuefeng Su; Jing Xie; Feng Wu; Guoqiang Tan

doi:10.1021/acs.nanolett.2c01002

Thermochemical Cyclization Constructs Bridged Dual-Coating of Ni-Rich Layered Oxide Cathodes for High-Energy Li-Ion Batteries

Nano Lett. 2022 Jul 13;22(13):5221-5229. doi: 10.1021/acs.nanolett.2c01002. Epub 2022 Jun 21.

Authors

Jing Wang^{1

2}, Qiang Yuan^{1

2}, Zhixin Ren³, Chunhao Sun⁴, Junfan Zhang^{1

2}, Ran Wang^{1

2}, Mengmeng Qian^{1

2}, Qi Shi^{1

2}, Ruiwen Shao⁴, Daobin Mu¹, Yuefeng Su^{1

2}, Jing Xie³, Feng Wu^{1

2}, Guoqiang Tan^{1

2}

Affiliations

¹ Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, China.
² Beijing Institute of Technology Chongqing Innovation Center, Chongqing, 401120, China.
³ Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, China.
⁴ Beijing Advanced Innovation Center for Intelligent Robots and Systems and Institute of Engineering Medicine, Beijing Institute of Technology, Beijing 100081, China.

PMID: 35727314
DOI: 10.1021/acs.nanolett.2c01002

Abstract

Enhancing microstructural and electrochemical stabilities of Ni-rich layered oxides is critical for improving the safety and cycle-life of high-energy Li-ion batteries. Here we propose a thermochemical cyclization strategy where heating polyacrylonitrile with LiNi_0.8Co_0.1Mn_0.1O₂ can simultaneously construct a cyclized polyacrylonitrile outer layer and a rock-salt bridge-like inner layer, forming a compact dual-coating of LiNi_0.8Co_0.1Mn_0.1O₂. Systematic studies demonstrate that the mild cyclization reaction between polyacrylonitrile and LiNi_0.8Co_0.1Mn_0.1O₂ induces a desirable "layered to rock-salt" structural transformation to create a nano-intermedium that acts as the bridge for binding cyclized polyacrylonitrile to layered LiNi_0.8Co_0.1Mn_0.1O₂. Because of the improvement of the structural and electrochemical stability and electrical properties, this cathode design remarkably enhances the cycling performance and rate capability of LiNi_0.8Co_0.1Mn_0.1O₂, showing a high reversible capacity of 183 mAh g^-1 and a high capacity retention of 83% after 300 cycles at 1 C rate. Notably, this facile and scalable surface engineering makes Ni-rich cathodes potentially viable for commercialization in high-energy Li-ion batteries.

Keywords: Dual-coating; Li-ion battery; Nickel-rich layered oxide; Polyacrylonitrile; Thermochemical cyclization.