DataVXAdvanced MaterialsPaper
journal article·2021-12Open access

Uncommon Behavior of Li Doping Suppresses Oxygen Redox in P2‐Type Manganese‐Rich Sodium Cathodes

Biwei Xiao, Xiang Liu, Xi Chen, Gi‐Hyeok Lee, Miao Song, Xin Yang, Fred Omenya, David M. Reed, Vincent Sprenkle, Yang Ren, Cheng‐Jun Sun, Wanli Yang, Khalil Amine, Xin Li, Guiliang Xu, Xiaolin Li

Advanced Materials· Volume 33· Issue 52
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Source abstract

Abstract

Abstract Utilizing both cationic and anionic oxygen redox reactions is regarded as an important approach to exploit high‐capacity layered cathode materials with earth abundant elements. It has been popular strategies to effectively elevate the oxygen redox activities by Li‐doping to introduce unhybridized O 2p orbitals in NaxMnO2‐based chemistries or enabling high covalency transition metals in P2‐Na0.66MnxTM1−xO2 (TM = Fe, Cu, Ni) materials. Here, the effect of Li doping on regulating the oxygen redox activities P2‐structured Na0.66Ni0.25Mn0.75O2 materials is investigated. Systematic X‐ray characterizations and ab initio simulations have shown that the doped Li has uncommon behavior in modulating the density of states of the neighboring Ni, Mn, and O, leading to the suppression of the existing oxygen and Mn redox reactivities and the promotion of the Ni redox. The findings provide a complementary scenario to current oxygen redox mechanisms and shed lights on developing new routes for high‐performance cathodes.
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Research context

Energy storage

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

Energy & Environment Directorate Pacific Northwest National Laboratory Richland WA 99352 USA

Chemical Sciences and Engineering Division Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA

John A. Paulson School of Engineering and Applied Sciences Harvard University Cambridge MA 02138 USA

Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA

Department of Materials Science and Engineering Dongguk University Seoul 04620 Republic of Korea

Physical and Computational Sciences Directorate Pacific Northwest National Laboratory Richland WA 99352 USA

X‐ray science division Argonne National Laboratory Lemont IL 60439 USA

Materials Science and Engineering Stanford University Stanford CA 94305 USA

Funding

U.S. Department of Energy · Pacific Northwest National Laboratory · Office of Science · Argonne National Laboratory · Harvard University

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