journal article·2023-11-10

Unveiling the Evolution of LiCoO2 beyond 4.6 V

Zixin Wu, Guifan Zeng, Jianhua Yin, Chao-Lung Chiang, Qinghua Zhang, Baodan Zhang, Jianken Chen, Yawen Yan, Yonglin Tang, Haitang Zhang, Shiyuan Zhou, Qingsong Wang, Xiaoxiao Kuai, Yan-Gu Lin, Lin Gu, Yu Qiao, Shi-Gang Sun

ACS Energy Letters· Volume 8· Issue 11
Publisher page

Abstract

The working mechanism of LiCoO 2 beyond 4.6 V presents complicated issues: (1) the ambiguous multistructural evolutions, (2) the vague O-related anionic redox reactions (ARR) triggered by the overlap Co–O bands, and (3) the serious electrode–electrolyte interface stability challenges. The intricate relationship among them turns into a classic “chicken and egg” conundrum, leading to a confusing evolution process of LiCoO 2 . Herein, from an ingenious perspective combining stacking faults and nonhomogeneous delithiation, we originally demonstrate a series of intergrowth phase evolutions from O3 to O1, passing through the so-called H1-3 phase. Moreover, in sharp contrast to the O–O dimer formed in a traditional Li-rich layered cathode, a moderate and stable arrangement of oxidized lattice oxygen is unveiled as a manifestation of ARR in LiCoO 2 . Additionally, we clarify the nature that dehydrogenation and hydrolysis of electrolyte trigger the chain decompositions and intensify the surface degradation.
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Research context

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

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

Affiliations

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People’s Republic of China

National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan, Republic of China

Institute of Physics, Chinese Academy of Sciences, Beijing 100190, People’s Republic of China

Bavarian Center for Battery Technology (BayBatt), Department of Chemistry, University of Bayreuth, Universitätsstrasse 30, Bayreuth 95447, Germany

Fujian Science & Technology Innovation Laboratory for Energy Materials of China (Tan Kah Kee Innovation Laboratory), Xiamen 361005, People’s Republic of China

School of Materials Science and Engineering, Tsinghua University, Beijing 100084, People’s Republic of China

Funding

Ministry of Science and Technology of the People's Republic of China · Natural Science Foundation of Beijing Municipality · Fundamental Research Funds for the Central Universities · National Natural Science Foundation of China · Xiamen University · Tan Kah Kee Innovation Laboratory

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