journal article·2020-04Open access

Constructing Na‐Ion Cathodes via Alkali‐Site Substitution

Chenglong Zhao, Zhenpeng Yao, Dong Zhou, Liwei Jiang, Jianlin Wang, Vadim Murzin, Yaxiang Lu, Xuedong Bai, Alán Aspuru‐Guzik, Liquan Chen, Yong‐Sheng Hu

Advanced Functional Materials· Volume 30· Issue 17

Abstract

Abstract Na‐ion batteries have experienced rapid development over the past decade and received significant attention from the academic and industrial communities. Although a large amount of effort has been made on material innovations, accessible design strategies on peculiar structural chemistry remain elusive. An approach to in situ construction of new Na‐based cathode materials by substitution in alkali sites is proposed to realize long‐term cycling stability and high‐energy density in low‐cost Na‐ion cathodes. A new compound, [K0.444(1)Na1.414(1)][Mn3/4Fe5/4](CN)6, is obtained through a rational control of K+ content from electrochemical reaction. Results demonstrate that the remaining K+ (≈0.444 mol per unit) in the host matrix can stabilize the intrinsic K‐based structure during reversible Na+ extraction/insertion process without the structural evolution to the Na‐based structure after cycles. Thereby, the as‐prepared cathode shows the remarkably enhanced structural stability with the capacity retention of >78% after 1800 cycles, and a higher average operation voltage of ≈3.65 V versus Na+/Na, directly contrasting the non‐alkali‐site‐substitution cathode materials. This provides new insights into alkali‐site‐substitution constructing advanced Na‐ion cathode 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

Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and Devices Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China

Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China

Department of Chemistry and Chemical Biology Harvard University Cambridge MA 02138 USA

Helmholtz Zentrum Berlin für Materialien und Energie Hahn‐Meitner‐Platz 1 14109 Berlin Germany

State Key Laboratory for Surface Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China

Bergische Universität Wuppertal Gaußstraße 20 42119 Wuppertal Germany

Department of Chemistry and Department of Computer Science University of Toronto Toronto ON M5S 3H6 Canada

Yangtze River Delta Physics Research Center Co. Ltd. Liyang 213300 China

Funding

National Natural Science Foundation of China · Beijing Municipal Science and Technology Commission · U.S. Department of Energy · Office of Science · Basic Energy Sciences

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