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Reversible Al Metal Anodes Enabled by Amorphization for Aqueous Aluminum Batteries

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2022, 144, 25, 11444-11455
    Article

    Reversible Al Metal Anodes Enabled by Amorphization for Aqueous Aluminum Batteries
    Click to copy article linkArticle link copied!

    • Chunshuang Yan*
      Chunshuang Yan
      MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150001, China
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      *Email: [email protected]
      More by Chunshuang Yan
      Orcidhttps://orcid.org/0000-0003-3840-7052
    • Chade Lv
      Chade Lv
      MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150001, China
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Chade Lv
      Orcidhttps://orcid.org/0000-0002-0964-1037
    • Bei-Er Jia
      Bei-Er Jia
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Bei-Er Jia
    • Lixiang Zhong
      Lixiang Zhong
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Lixiang Zhong
    • Xun Cao
      Xun Cao
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Xun Cao
      Orcidhttps://orcid.org/0000-0002-6034-381X
    • Xuelin Guo
      Xuelin Guo
      Materials Science and Engineering Program and Walker Department of Mechanical Engineering, Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States
      More by Xuelin Guo
    • Hengjie Liu
      Hengjie Liu
      National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230029, China
      More by Hengjie Liu
      Orcidhttps://orcid.org/0000-0001-6499-3935
    • Wenjie Xu
      Wenjie Xu
      National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230029, China
      More by Wenjie Xu
    • Daobin Liu
      Daobin Liu
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Daobin Liu
    • Lan Yang
      Lan Yang
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Lan Yang
    • Jiawei Liu
      Jiawei Liu
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Jiawei Liu
    • Huey Hoon Hng
      Huey Hoon Hng
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Huey Hoon Hng
      Orcidhttps://orcid.org/0000-0002-8950-025X
    • Wei Chen
      Wei Chen
      Department of Physics, National University of Singapore, Singapore 117542, Singapore
      More by Wei Chen
      Orcidhttps://orcid.org/0000-0002-1131-3585
    • Li Song
      Li Song
      Institute of Materials Research and Engineering, A*STAR, 2 Fusionopolis Way, Innovis, #08-03, Singapore 138634, Singapore
      More by Li Song
      Orcidhttps://orcid.org/0000-0003-0585-8519
    • Shuzhou Li
      Shuzhou Li
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Shuzhou Li
      Orcidhttps://orcid.org/0000-0002-2159-2602
    • Zheng Liu
      Zheng Liu
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      More by Zheng Liu
      Orcidhttps://orcid.org/0000-0002-8825-7198
    • Qingyu Yan*
      Qingyu Yan
      School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
      Institute of Materials Research and Engineering, A*STAR, 2 Fusionopolis Way, Innovis, #08-03, Singapore 138634, Singapore
      *Email: [email protected]
      More by Qingyu Yan
      Orcidhttps://orcid.org/0000-0003-0317-3225
    • Guihua Yu*
      Guihua Yu
      Materials Science and Engineering Program and Walker Department of Mechanical Engineering, Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States
      *Email: [email protected]
      More by Guihua Yu
      Orcidhttps://orcid.org/0000-0002-3253-0749
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 25, 11444–11455
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.2c04820
    Published June 18, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

    Abstract

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    Aqueous aluminum metal batteries (AMBs) are regarded as one of the most sustainable energy storage systems among post-lithium-ion candidates, which is attributable to their highest theoretical volumetric capacity, inherent safe operation, and low cost. Yet, the development of aqueous AMBs is plagued by the incapable aluminum plating in an aqueous solution and severe parasitic reactions, which results in the limited discharge voltage, thus making the development of aqueous AMBs unsuccessful so far. Here, we demonstrate that amorphization is an effective strategy to tackle these critical issues of a metallic Al anode by shifting the reduction potential for Al deposition. The amorphous aluminum (a-Al) interfacial layer is triggered by an in situ lithium-ion alloying/dealloying process on a metallic Al substrate with low strength. Unveiled by experimental and theoretical investigations, the amorphous structure greatly lowers the Al nucleation energy barrier, which forces the Al deposition competitive to the electron-stealing hydrogen evolution reaction (HER). Simultaneously, the inhibited HER mitigates the passivation, promoting interfacial ion transfer kinetics and enabling steady aluminum plating/stripping for 800 h in the symmetric cell. The resultant multiple full cells using Al@a-Al anodes deliver approximately a 0.6 V increase in the discharge voltage plateau compared to that of bare Al-based cells, which far outperform all reported aqueous AMBs. In both symmetric cells and full cells, the excellent electrochemical performances are achieved in a noncorrosive, low-cost, and fluorine-free Al2(SO4)3 electrolyte, which is ecofriendly and can be easily adapted for sustainable large-scale applications. This work brings an intriguing picture of the design of metallic anodes for reversible and high-voltage AMBs.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c04820.

    • SEM images, XRD patterns, TEM images, XPS spectra, Raman spectra, contact angle measurements, mechanical properties tests, electrochemical tests, and computational results (PDF)

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    Cited By

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    This article is cited by 23 publications.

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    2. Zhongchen Zhao, Zonghan Zhang, Tian Xu, Wenbin Wang, Baofeng Wang, Xuebin Yu. Solvation Structure Regulation for Highly Reversible Aqueous Al Metal Batteries. Journal of the American Chemical Society 2024, 146 (3) , 2257-2266. https://doi.org/10.1021/jacs.3c13003
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 25, 11444–11455
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.2c04820
    Published June 18, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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