Fluorinated Rocksalt Cathode with Ultra‐high Active Li Content for Lithium‐ion Batteries

Pei, Yi; Chen, Qing; Ha, Yang; Su, Dong; Zhou, Hua; Li, Shuang; Yao, Zhenpeng; Ma, Lu; Sanders, Kevin J.; Sheng, Chuanchao; Goward, Gillian R.; Gu, Lin; Yu, Aiping; Yang, Wanli; Chen, Zhongwei

doi:10.1002/ange.202212471

Title: Fluorinated Rocksalt Cathode with Ultra‐high Active Li Content for Lithium‐ion Batteries

Journal Article · Thu Oct 20 00:00:00 EDT 2022 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202212471· OSTI ID:1894150

Pei, Yi ^[1]; Chen, Qing ^[1]; Ha, Yang ^[2];

^[3]; Zhou, Hua ^[4]; Li, Shuang ^[5]; Yao, Zhenpeng ^[6]; Ma, Lu ^[7]; Sanders, Kevin J. ^[8]; Sheng, Chuanchao ^[9]; Goward, Gillian R. ^[8]; Gu, Lin ^[3]; Yu, Aiping ^[1]; Yang, Wanli ^[2]; Chen, Zhongwei ^[1]

Department of Chemical Engineering Waterloo Institute for Nanotechnology University of Waterloo Waterloo Ontario N2 L 3G1 Canada
Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA
Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China
Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
Department of Chemistry and Department of Computer Science University of Toronto Toronto Ontario M5S 3H6 Canada
National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA
Department of Chemistry McMaster University Hamilton ON L8S 4 L8 Canada
Center of Energy Storage Materials &, Technology College of Engineering and Applied Sciences National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China

Abstract The key to increasing the energy density of lithium‐ion batteries is to incorporate high contents of extractable Li into the cathode. Unfortunately, this triggers formidable challenges including structural instability and irreversible chemistry under operation. Here, we report a new kind of ultra‐high Li compound: Li _{4+ x} MoO ₅ F _x (1≤ x ≤3) for cathode with an unprecedented level of electrochemically active Li (>3 Li ⁺ per formula), delivering a reversible capacity up to 438 mAh g ⁻¹ . Unlike other reported Li‐rich cathodes, Li _{4+ x} MoO ₅ F _x presents distinguished structure stability to immunize against irreversible behaviors. Through spectroscopic and electrochemical techniques, we find an anionic redox‐dominated charge compensation with negligible oxygen release and voltage decay. Our theoretical analysis reveals a “reductive effect” of high‐level fluorination stabilizes the anionic redox by reducing the oxygen ions in pure‐Li conditions, enabling a facile, reversible, and high Li‐portion cycling.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357; DEAC02-05CH11231; SC0012704

OSTI ID:: 1894150

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 134 Journal Issue: 47; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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