journal article·2021-01Open access

Stabilizing Anionic Redox Chemistry in a Mn‐Based Layered Oxide Cathode Constructed by Li‐Deficient Pristine State

Xin Cao, Haifeng Li, Yu Qiao, Min Jia, Xiang Li, Jordi Cabana, Haoshen Zhou

Advanced Materials· Volume 33· Issue 2

Abstract

Abstract Li‐rich cathode materials are of significant interest for coupling anionic redox with cationic redox chemistry to achieve high‐energy‐density batteries. However, lattice oxygen loss and derived structure distortion would induce serious capacity loss and voltage decay, further hindering its practical application. Herein, a novel Li‐rich cathode material, O3‐type Li0.6[Li0.2Mn0.8]O2, is developed with the pristine state displaying both a Li excess in the transition metal layer and a deficiency in the alkali metal layer. Benefiting from stable structure evolution and Li migration processes, not only can high reversible capacity (≈329 mAh g−1) be harvested but also irreversible/reversible anionic/cationic redox reactions are comprehensively assigned via the combination of in/ex situ spectroscopies. Furthermore, irreversible lattice oxygen loss and structure distortion are effectively restrained, resulting in long‐term cycle stability (capacity drop of 0.045% per cycle, 500 cycles). Altogether, tuning the Li state in the alkali metal layer presents a promising way for modification of high‐capacity Li‐rich cathode candidates.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced battery technologies research

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

Affiliations

Energy Technology Research Institute National Institute of Advanced Industrial Science and Technology (AIST) 1‐1‐1, Umezono Tsukuba 305‐8568 Japan

Graduate School of System and Information Engineering University of Tsukuba 1‐1‐1, Tennoudai Tsukuba 305‐8573 Japan

Department of Chemistry University of Illinois at Chicago Chicago IL 60607 USA

Argonne National Laboratory 9700 S. Cass Avenue Lemont IL 60439 USA

Center of Energy Storage Materials and Technology College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials National Laboratory of Solid State Microstructures, and Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 P. R. China

Funding

National Basic Research Program of China · National Natural Science Foundation of China · U.S. Department of Energy · Argonne National Laboratory

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