Multi-electron transfer enabled by topotactic reaction in magnetite

Wei Zhang, Yan Li, Lijun Wu, Yandong Duan, Kim Kisslinger, Chunlin Chen, David C. Bock, Feng Pan, Yimei Zhu, Amy C. Marschilok, Esther S. Takeuchi, Kenneth J. Takeuchi and Feng Wang ()
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Wei Zhang: Brookhaven National Laboratory
Yan Li: American Physical Society
Lijun Wu: Brookhaven National Laboratory
Yandong Duan: Brookhaven National Laboratory
Kim Kisslinger: Center for Functional Nanomaterials, Brookhaven National Laboratory
Chunlin Chen: Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
David C. Bock: Energy Sciences Directorate, Brookhaven National Laboratory
Feng Pan: Peking University, Shenzhen Graduate School
Yimei Zhu: Brookhaven National Laboratory
Amy C. Marschilok: Energy Sciences Directorate, Brookhaven National Laboratory
Esther S. Takeuchi: Energy Sciences Directorate, Brookhaven National Laboratory
Kenneth J. Takeuchi: Stony Brook University
Feng Wang: Brookhaven National Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract A bottleneck for the large-scale application of today’s batteries is low lithium storage capacity, largely due to the use of intercalation-type electrodes that allow one or less electron transfer per redox center. An appealing alternative is multi-electron transfer electrodes, offering excess capacity, which, however, involves conversion reaction; according to conventional wisdom, the host would collapse during the process, causing cycling instability. Here, we report real-time observation of topotactic reaction throughout the multi-electron transfer process in magnetite, unveiled by in situ single-crystal crystallography with corroboration of first principles calculations. Contradicting the traditional belief of causing structural breakdown, conversion in magnetite resembles an intercalation process—proceeding via topotactic reaction with the cubic close packed oxygen-anion framework retained. The findings from this study, with unique insights into enabling multi-electron transfer via topotactic reaction, and its implications to the cyclability and rate capability, shed light on designing viable multi-electron transfer electrodes for high energy batteries.

Date: 2019
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DOI: 10.1038/s41467-019-09528-9

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