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Enabling Magnesium Anodes by Tuning the Electrode/Electrolyte Interfacial Structure

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Mater. Interfaces 2021, 13, 44, 52461-52468
    Energy, Environmental, and Catalysis Applications

    Enabling Magnesium Anodes by Tuning the Electrode/Electrolyte Interfacial Structure
    Click to copy article linkArticle link copied!

    • Xiaoyu Wen
      Xiaoyu Wen
      Department of Chemical and Environmental Engineering, University of California, Riverside, California 92521, United States
      More by Xiaoyu Wen
    • Zhou Yu
      Zhou Yu
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Zhou Yu
      Orcidhttps://orcid.org/0000-0003-3316-4979
    • Yifan Zhao
      Yifan Zhao
      Materials Science and Engineering Program, University of California, Riverside, California 92521, United States
      More by Yifan Zhao
    • Jian Zhang
      Jian Zhang
      Materials Science and Engineering Program, University of California, Riverside, California 92521, United States
      More by Jian Zhang
      Orcidhttps://orcid.org/0000-0003-0356-7611
    • Rui Qiao
      Rui Qiao
      Department of Mechanical Engineering, Virginia Tech, Blacksburg, Virginia 24061, United States
      More by Rui Qiao
      Orcidhttps://orcid.org/0000-0001-5219-5530
    • Lei Cheng*
      Lei Cheng
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      *Email: [email protected]
      More by Lei Cheng
      Orcidhttps://orcid.org/0000-0002-3902-1680
    • Chunmei Ban*
      Chunmei Ban
      Paul M. Rady Department of Mechanical Engineering, University of Colorado Boulder, Boulder, Colorado 80309, United States
      *Email: [email protected]
      More by Chunmei Ban
      Orcidhttps://orcid.org/0000-0002-1472-1496
    • Juchen Guo*
      Juchen Guo
      Department of Chemical and Environmental Engineering, University of California, Riverside, California 92521, United States
      Materials Science and Engineering Program, University of California, Riverside, California 92521, United States
      *Email: [email protected]
      More by Juchen Guo
      Orcidhttps://orcid.org/0000-0001-9829-1202
    Other Access OptionsSupporting Information (1)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 44, 52461–52468
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.1c10446
    Published November 1, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    A new deposition mechanism is presented in this study to achieve highly reversible plating and stripping of magnesium (Mg) anodes for Mg-ion batteries. It is known that the reduction of electrolyte anions such as bis(trifluoromethanesulfonyl)imide (TFSI–) causes Mg surface passivation, resulting in poor electrochemical performance for Mg-ion batteries. We reveal that the addition of sodium cations (Na+) in Mg-ion electrolytes can fundamentally alter the interfacial chemistry and structure at the Mg anode surface. The molecular dynamics simulation suggests that Na+ cations contribute to a significant population in the interfacial double layer so that TFSI– anions are excluded from the immediate interface adjacent to the Mg anode. As a result, the TFSI– decomposition is largely suppressed so does the formation of passivation layers at the Mg surface. This mechanism is supported by our electrochemical, microscopic, and spectroscopic analyses. The resultant Mg deposition demonstrates smooth surface morphology and lowered overpotential compared to the pure Mg(TFSI)2 electrolyte.

    Copyright © 2021 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/acsami.1c10446.

    • Table of MD systems studied in this work; representative CV scan curves at 5 mV s–1; Mg deposition potential curves at 1 mA cm–2; SEM images of Mg deposition at 1 mA cm–2; EDX spectra of Mg deposition; Na 1s XPS spectrum of Mg deposition; calculated distribution of electrical potential in the electrolyte; MD simulation of the number density profiles with the Madrid-2019 force fields; calculated coordination number of TFSI– ions and DME molecules around the interfacial Mg2+ and Na+ cations; and radial distribution functions from Mg/Na to the oxygen atoms of TFSI– ions and DME molecules (PDF)

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    Cited By

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    This article is cited by 10 publications.

    1. Takahiro Okuo, Toshihiko Mandai, Hiroyasu Masunaga, Noboru Ohta, Hidetoshi Matsumoto. Magnesiated Nafion-Based Gel Electrolytes: Structural and Electrochemical Characterization. The Journal of Physical Chemistry C 2023, 127 (29) , 14502-14509. https://doi.org/10.1021/acs.jpcc.3c02924
    2. Nan Yao, Xiang Chen, Zhong-Heng Fu, Qiang Zhang. Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries. Chemical Reviews 2022, 122 (12) , 10970-11021. https://doi.org/10.1021/acs.chemrev.1c00904
    3. Xueting Huang, Jiaxin Wen, Jinglei Lei, Guangsheng Huang, Fusheng Pan, Lingjie Li. Facile and Economic Synthesis of Robust Non-Nucleophilic Electrolyte for High-Performance Rechargeable Magnesium Batteries. ACS Applied Materials & Interfaces 2022, 14 (7) , 8906-8915. https://doi.org/10.1021/acsami.1c19971
    4. M. H. Nassar, Medhat Mesallam, M. Farrag, E. Sheha. Probing the effect of the stoichiometric ratio of Mg(CF 3 SO 3 ) 2 /AlCl 3 on optimizing the electrolyte performance. Materials Research Innovations 2023, 27 (2) , 75-82. https://doi.org/10.1080/14328917.2022.2085004
    5. Mohamed Farrag, H. S. Refai, E. Sheha. The role of adding NaF to the electrolyte in constructing a stable anode/electrolyte interphase for magnesium battery applications. Journal of Solid State Electrochemistry 2023, 27 (2) , 379-389. https://doi.org/10.1007/s10008-022-05329-1
    6. Heng Zhang, Lixin Qiao, Michel Armand. Organic Electrolyte Design for Rechargeable Batteries: From Lithium to Magnesium. Angewandte Chemie 2022, 134 (52) https://doi.org/10.1002/ange.202214054
    7. Heng Zhang, Lixin Qiao, Michel Armand. Organic Electrolyte Design for Rechargeable Batteries: From Lithium to Magnesium. Angewandte Chemie International Edition 2022, 61 (52) https://doi.org/10.1002/anie.202214054
    8. R M Khalil, Talaat A Hameed, M Farrag, E Sheha, A A Ali, F Salman, S Solyman. Microstructure, electrical, optical and electrochemical characteristics of silver phosphate glasses cathode for magnesium battery applications. Journal of Physics D: Applied Physics 2022, 55 (49) , 495303. https://doi.org/10.1088/1361-6463/ac9ab0
    9. Chuanliang Wei, Liwen Tan, Yuchan Zhang, Zhengran Wang, Jinkui Feng, Yitai Qian. Towards better Mg metal anodes in rechargeable Mg batteries: Challenges, strategies, and perspectives. Energy Storage Materials 2022, 52 , 299-319. https://doi.org/10.1016/j.ensm.2022.08.014
    10. Jiangfeng Song, Jing Chen, Xiaoming Xiong, Xiaodong Peng, Daolun Chen, Fusheng Pan. Research advances of magnesium and magnesium alloys worldwide in 2021. Journal of Magnesium and Alloys 2022, 10 (4) , 863-898. https://doi.org/10.1016/j.jma.2022.04.001
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 44, 52461–52468
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.1c10446
    Published November 1, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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