Thermal-healing of lattice defects for high-energy single-crystalline battery cathodes

Shaofeng Li; Guannan Qian; Xiaomei He; Xiaojing Huang; Sang-Jun Lee; Zhisen Jiang; Yang Yang; Wei-Na Wang; Dechao Meng; Chang Yu; Jun-Sik Lee; Yong S Chu; Zi-Feng Ma; Piero Pianetta; Jieshan Qiu; Linsen Li; Kejie Zhao; Yijin Liu

doi:10.1038/s41467-022-28325-5

Thermal-healing of lattice defects for high-energy single-crystalline battery cathodes

Nat Commun. 2022 Feb 4;13(1):704. doi: 10.1038/s41467-022-28325-5.

Authors

Shaofeng Li^#^{1

2}, Guannan Qian^#^{1

3}, Xiaomei He^#⁴, Xiaojing Huang⁵, Sang-Jun Lee¹, Zhisen Jiang¹, Yang Yang⁵, Wei-Na Wang³, Dechao Meng³, Chang Yu², Jun-Sik Lee¹, Yong S Chu⁵, Zi-Feng Ma³, Piero Pianetta¹, Jieshan Qiu⁶, Linsen Li^{7

8}, Kejie Zhao⁹, Yijin Liu¹⁰

Affiliations

¹ Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
² State Key Lab of Fine Chemicals, School of Chemical Engineering, Liaoning Key Lab for Energy Materials and Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.
³ Department of Chemical Engineering, School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China.
⁴ School of Mechanical Engineering, Purdue University, West Lafayette, IN, 47906, USA.
⁵ National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, 11973, USA.
⁶ State Key Lab of Fine Chemicals, School of Chemical Engineering, Liaoning Key Lab for Energy Materials and Chemical Engineering, Dalian University of Technology, Dalian, 116024, China. jqiu@dlut.edu.cn.
⁷ Department of Chemical Engineering, School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China. linsenli@sjtu.edu.cn.
⁸ Shanghai Jiao Tong University Sichuan Research Institute, Chengdu, 610213, China. linsenli@sjtu.edu.cn.
⁹ School of Mechanical Engineering, Purdue University, West Lafayette, IN, 47906, USA. kjzhao@purdue.edu.
¹⁰ Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA. liuyijin@slac.stanford.edu.

^# Contributed equally.

Abstract

Single-crystalline nickel-rich cathodes are a rising candidate with great potential for high-energy lithium-ion batteries due to their superior structural and chemical robustness in comparison with polycrystalline counterparts. Within the single-crystalline cathode materials, the lattice strain and defects have significant impacts on the intercalation chemistry and, therefore, play a key role in determining the macroscopic electrochemical performance. Guided by our predictive theoretical model, we have systematically evaluated the effectiveness of regaining lost capacity by modulating the lattice deformation via an energy-efficient thermal treatment at different chemical states. We demonstrate that the lattice structure recoverability is highly dependent on both the cathode composition and the state of charge, providing clues to relieving the fatigued cathode crystal for sustainable lithium-ion batteries.

Grants and funding

DE-AC02-76SF00515/DOE | Office of Science (SC)