journal article·2022-07Open access

Elastic Lattice Enabling Reversible Tetrahedral Li Storage Sites in a High‐Capacity Manganese Oxide Cathode

Weiyuan Huang, Luyi Yang, Zhefeng Chen, Tongchao Liu, Guoxi Ren, Peizhao Shan, Bin‐Wei Zhang, Shiming Chen, Shunning Li, Jianyuan Li, Cong Lin, Wenguang Zhao, Jimin Qiu, Jianjun Fang, Mingjian Zhang, Cheng Dong, Fan Li, Yong Yang, Cheng‐Jun Sun, Yang Ren, Qingzhen Huang, Guangjin Hou, Shi‐Xue Dou, Jun Lu, Khalil Amine, Feng Pan

Advanced Materials· Volume 34· Issue 30

Abstract

Abstract The key to breaking through the capacity limitation imposed by intercalation chemistry lies in the ability to harness more active sites that can reversibly accommodate more ions (e.g., Li+) and electrons within a finite space. However, excessive Li‐ion insertion into the Li layer of layered cathodes results in fast performance decay due to the huge lattice change and irreversible phase transformation. In this study, an ultrahigh reversible capacity is demonstrated by a layered oxide cathode purely based on manganese. Through a wealth of characterizations, it is clarified that the presence of low‐content Li2MnO3 domains not only reduces the amount of irreversible O loss; but also regulates Mn migration in LiMnO2 domains, enabling elastic lattice with high reversibility for tetrahedral sites Li‐ion storage in Li layers. This work utilizes bulk cation disorder to create stable Li‐ion‐storage tetrahedral sites and an elastic lattice for layered materials, with a reversible capacity of 600 mA h g−1, demonstrated in th range 0.6–4.9 V versus Li/Li+ at 10 mA g−1. Admittedly, discharging to 0.6 V might be too low for practical use, but this exploration is still of great importance as it conceptually demonstrates the limit of Li‐ions insertion into layered oxide materials.
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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

School of Advanced Materials Peking University Shenzhen Graduate School Shenzhen 518055 P. R. China

Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA

State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai 200050 P. R. China

State Key Laboratory for Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China

Institute for Superconducting and Electronic Materials University of Wollongong Wollongong New South Wales 2522 Australia

State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian Liaoning Province 116023 P. R. China

University of Chinese Academy of Sciences Beijing 100049 P. R. China

X‐Ray Science Division Argonne National Laboratory Lemont IL 60439 USA

NIST Center for Neutron Research National Institute of Standards and Technology 100 Bureau Drive Gaithersburg MD 20899 USA

Material Science and Engineering Stanford University Stanford CA 94305 USA

Funding

Guangdong Science and Technology Department · Ministry of Science and Technology of the People's Republic of China · National Natural Science Foundation of China · Australian Research Council

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