Integrating a Ferroelectric Interface with a Well-Tuned Electronic Structure in Lithium-Rich Layered Oxide Cathodes for Enhanced Lithium Storage

Chunxiao Zhang; Tianshuo Wang; Youquan Zhang; Yuelei Zhu; Hai Zhu; Bo Wei; Jianghua Wu; Chaoping Liang; Libao Chen; Peng Wang; Weifeng Wei

doi:10.1021/acs.inorgchem.2c02315

Integrating a Ferroelectric Interface with a Well-Tuned Electronic Structure in Lithium-Rich Layered Oxide Cathodes for Enhanced Lithium Storage

Inorg Chem. 2023 Jan 16;62(2):685-693. doi: 10.1021/acs.inorgchem.2c02315. Epub 2022 Dec 30.

Authors

Chunxiao Zhang¹, Tianshuo Wang¹, Youquan Zhang¹, Yuelei Zhu², Hai Zhu¹, Bo Wei³, Jianghua Wu², Chaoping Liang¹, Libao Chen¹, Peng Wang^{2

4}, Weifeng Wei¹

Affiliations

¹ State Key Laboratory of Powder Metallurgy, Powder Metallurgy Research Institute, Central South University, Changsha, Hunan 410083, P. R. China.
² National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences and Collaborative, Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, P. R. China.
³ School of Materials Science and Engineering, Beihang University, Beijing 100191, P. R. China.
⁴ Department of Physics, University of Warwick, Coventry CV4 7AL, U.K.

PMID: 36583612
DOI: 10.1021/acs.inorgchem.2c02315

Abstract

Li-rich layered oxides (LLOs) are considered promising candidates for new high-energy-density cathode materials for next-generation power batteries. However, their large-scale applications are largely hindered by irreversible Li/O loss, structural degradation, and interfacial side reactions during cycling. Herein, we demonstrate an integration strategy that tunes the electronic structure by La/Al codoping and constructs a ferroelectric interface on the LLOs surface through Bi_0.5Na_0.5TiO₃ (BNT) coating. Experimental characterization reveals that the synergistic effect of the ferroelectric interface and the well-tuned electronic structure can not only promote the diffusion of Li⁺ and hinder the migration of O^n- but also suppress the lattice volume changes and reduce interfacial side reactions at high voltages up to 4.9 V vs Li⁺/Li. As a result, the modified material shows enhanced initial capacities and retention rates of 224.4 mAh g^-1 and 78.57% after 500 cycles at 2.0-4.65 V and 231.7 mAh g^-1 and 85.76% after 200 cycles at 2.0-4.9 V at 1C, respectively.