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Critical Role of the Interphase at Magnesium Electrodes in Chloride-Free, Simple Salt Electrolytes

  • Conrad Holc
    Conrad Holc
    Nottingham Applied Materials and Interfaces Group, School of Chemistry, University of Nottingham, Nottingham NG7 2TU, U.K.
    The Faraday Institution, Harwell Campus, Didcot OX11 0RA, U.K.
    More by Conrad Holc
  • Konstantinos Dimogiannis
    Konstantinos Dimogiannis
    Nottingham Applied Materials and Interfaces Group, School of Chemistry, University of Nottingham, Nottingham NG7 2TU, U.K.
  • Emily Hopkinson
    Emily Hopkinson
    Nottingham Applied Materials and Interfaces Group, School of Chemistry, University of Nottingham, Nottingham NG7 2TU, U.K.
  • , and 
  • Lee R. Johnson*
    Lee R. Johnson
    Nottingham Applied Materials and Interfaces Group, School of Chemistry, University of Nottingham, Nottingham NG7 2TU, U.K.
    The Faraday Institution, Harwell Campus, Didcot OX11 0RA, U.K.
    *Email: [email protected]
Cite this: ACS Appl. Mater. Interfaces 2021, 13, 25, 29708–29713
Publication Date (Web):June 18, 2021
https://doi.org/10.1021/acsami.1c06130
Copyright © 2021 American Chemical Society

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    Abstract

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    Magnesium (Mg) batteries are a potential beyond lithium-ion technology but currently suffer from poor cycling performance, partly due to the interphase formed when magnesium electrodes react with electrolytes. The use of magnesium bis(trifluoromethanesulfonyl)imide (Mg(TFSI)2) electrolytes would enable high-voltage intercalation cathodes, but many reports identify poor Mg plating/stripping in the electrolyte solution due to a passivating interphase. Here, we have assessed the Mg plating/stripping mechanism at bulk Mg electrodes in a Mg(TFSI)2-based electrolyte by cyclic voltammetry, ex situ Fourier-transform infrared spectroscopy, and electron microscopy and compared this to the cycling of a Grignard-based electrolyte. Our studies indicate a nontypical cycling mechanism at Mg surfaces in Mg(TFSI)2-based electrolytes that occurs through Mg deposits rather than the bulk electrode. Fourier-transform infrared spectroscopy demonstrates an evolution in the interphase chemistry during conditioning (repeated cycling) and that this is a critical step for stable cycling in the Mg(TFSI)2-tetraglyme (4G) electrolyte. The fully conditioned electrode in Mg(TFSI)2-4G is able to cycle with an overpotential of <0.25 V without additional additives such as Cl or BH4.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c06130.

    • Experimental methods; assignment of infrared absorption peaks; cyclic voltammograms on Cu for both systems; SEM images of Mg electrodes after 1 cycle for both systems; SEM image of an uncycled Mg electrode; SEM image of a conditioned Cu electrode in 0.5 M Mg(TFSI)2-4G, coupled with EDX elemental mapping of the Mg deposit; cross-sectional SEM image of a conditioned Mg electrode in 0.5 M Mg(TFSI)2-4G; SEM image of a conditioned Cu electrode in 0.5 M Mg(TFSI)2-4G; and linear sweep voltammogram in 0.5 M Mg(TFSI)2-4G at Mg, Au, and SS working electrodes (PDF)

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    Cited By

    This article is cited by 7 publications.

    1. Yichao Zhuang, Dongzheng Wu, Fei Wang, Yaoqi Xu, Jing Zeng, Jinbao Zhao. Tailoring a Hybrid Functional Layer for Mg Metal Anodes in Conventional Electrolytes with a Low Overpotential. ACS Applied Materials & Interfaces 2022, 14 (42) , 47605-47615. https://doi.org/10.1021/acsami.2c11911
    2. Zifei Sun, Baichuan Wang, Matthew G. Boebinger, Alexandre Magasinski, Samik Jhulki, Yawei Zhang, Wenbin Fu, Matthew T. McDowell, Gleb Yushin. Stability of FeF3-Based Sodium-Ion Batteries in Nonflammable Ionic Liquid Electrolytes at Room and Elevated Temperatures. ACS Applied Materials & Interfaces 2022, 14 (29) , 33447-33456. https://doi.org/10.1021/acsami.2c10851
    3. Shiyang Wang, Kewei Wang, Yuchen Zhang, Yulin Jie, Xinpeng Li, Yuxue Pan, Xiaowen Gao, Qingshun Nian, Ruiguo Cao, Qi Li, Shuhong Jiao, Dongsheng Xu. High‐entropy Electrolyte Enables High Reversibility and Long Lifespan for Magnesium Metal Anodes. Angewandte Chemie 2023, 135 (31) https://doi.org/10.1002/ange.202304411
    4. Shiyang Wang, Kewei Wang, Yuchen Zhang, Yulin Jie, Xinpeng Li, Yuxue Pan, Xiaowen Gao, Qingshun Nian, Ruiguo Cao, Qi Li, Shuhong Jiao, Dongsheng Xu. High‐entropy Electrolyte Enables High Reversibility and Long Lifespan for Magnesium Metal Anodes. Angewandte Chemie International Edition 2023, 62 (31) https://doi.org/10.1002/anie.202304411
    5. Yuan Liu, Wanyu Zhao, Zhenghui Pan, Zhengqing Fan, Meng Zhang, Xiaoli Zhao, Jianping Chen, Xiaowei Yang. Interfacial Engineering of Magnesiophilic Coordination Layer Stabilizes Mg Metal Anode. Angewandte Chemie 2023, 135 (25) https://doi.org/10.1002/ange.202302617
    6. Yuan Liu, Wanyu Zhao, Zhenghui Pan, Zhengqing Fan, Meng Zhang, Xiaoli Zhao, Jianping Chen, Xiaowei Yang. Interfacial Engineering of Magnesiophilic Coordination Layer Stabilizes Mg Metal Anode. Angewandte Chemie International Edition 2023, 62 (25) https://doi.org/10.1002/anie.202302617
    7. Wanyu Zhao, Yuan Liu, Xiaoli Zhao, Zhenghui Pan, Jianping Chen, Songhe Zheng, Lingli Qu, Xiaowei Yang. Chloride‐Free Electrolytes for High‐Voltage Magnesium Metal Batteries: Challenges, Strategies, and Perspectives. Chemistry – A European Journal 2023, 29 (10) https://doi.org/10.1002/chem.202203334

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