journal article·2022-12-09

Tuning Co/O Redox Chemistry via Fermi Level Regulation for Stable High-Voltage LiCoO2

Mingpu Wen, Weijin Kong, Jicheng Zhang, Qinghua Zhang, Wen Yin, Nian Zhang, Ke Chai, Yang Yu, Huaican Chen, Xiangfeng Liu

ACS Energy Letters· Volume 7· Issue 12
Publisher page

Abstract

LiCoO2 (LCO) is ideal for 3C electronics due to its high tap density. However, the excessive O → Co charge transfer at high delithiation leads to irreversible Co reduction, O release, and structural degradation, deteriorating the high-voltage performance of LCO. Herein, we propose to regulate the intrinsic Fermi level via uneven trace Zr/Mg doping. First, the increase of electron density in the Fermi level mitigates both the O oxidation/coupled Co reduction through alleviating the O → Co charge transfer, restraining the formations of Co2+ and O2. This elevates Co redox activity and reduces O redox activity. In addition, the structural evolution of the cathode at delithiation is simplified. The modulated LCO delivers a high discharge capacity and a high cycling stability with 4.5 and 4.6 V ceilings. This study sheds new light on the modulation of Co/O redox chemistry and the reliable large-scale production of high-voltage LiCoO2.
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Research context

OpenAlex topics: Advancements in Battery Materials · Supercapacitor Materials and Fabrication · Advanced Battery Materials and Technologies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Center of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Science, Beijing 100190, People’s Republic of China

Spallation Neutron Source Science Center, Dongguan 523803, People’s Republic of China

Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, People’s Republic of China

CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100190, People’s Republic of China

Funding

Natural Science Foundation of Beijing Municipality · China Postdoctoral Science Foundation · Central University Basic Research Fund of China · National Natural Science Foundation of China · Strategic Priority Research Program of the Chinese Academy of Sciences · International Partnership Program · Scientific Instrument Developing Project

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