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A general Lewis acidic etching route for preparing MXenes with enhanced electrochemical performance in non-aqueous electrolyte

Nature Materials volume 19, pages 894–899 (2020)Cite this article

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Abstract

Two-dimensional carbides and nitrides of transition metals, known as MXenes, are a fast-growing family of materials that have attracted attention as energy storage materials. MXenes are mainly prepared from Al-containing MAX phases (where A = Al) by Al dissolution in F-containing solution; most other MAX phases have not been explored. Here a redox-controlled A-site etching of MAX phases in Lewis acidic melts is proposed and validated by the synthesis of various MXenes from unconventional MAX-phase precursors with A elements Si, Zn and Ga. A negative electrode of Ti3C2 MXene material obtained through this molten salt synthesis method delivers a Li+ storage capacity of up to 738 C g−1 (205 mAh g−1) with high charge–discharge rate and a pseudocapacitive-like electrochemical signature in 1 M LiPF6 carbonate-based electrolyte. MXenes prepared via this molten salt synthesis route may prove suitable for use as high-rate negative-electrode materials for electrochemical energy storage applications.

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Fig. 1: Schematic of Ti3C2Tx MXene preparation.
Fig. 2: Morphological and structural characterizations of MS-Ti3C2Tx MXene.
Fig. 3: Generalization of the Lewis acid etching route to a large family of MAX phases.
Fig. 4: Electrochemical characterizations of MS-Ti3C2Tx MXene electrode in 1 M LiPF6 (in 1:1 ethylene carbonate/dimethyl carbonate) electrolyte.

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Source data for Figs. 2a,d and 4 are provided with the paper. The remaining data that support the findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

This study was supported financially by the National Natural Science Foundation of China (grant nos. 21671195, 91426304, 51902320 and 51902319) and by the China Postdoctoral Science Foundation (grant no. 2018M642498). H.S. was supported by a grant from the China Scolarship Council. P.S., P.L.T. and H.S. thank the Agence Nationale de la Recherche (Labex STORE-EX) for financial support. Q.H. thanks the International Partnership Program of Chinese Academy of Sciences (grant no. 174433KYSB20190019), the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang, and the Ningbo top-talent team program for financial support. Z.L. is supported by the Fundamental Research Funds for the Central Universities (grant no. YJ201886). We acknowledge the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (faculty grant SFO‐Mat‐LiU no. 2009 00971). The Knut and Alice Wallenberg Foundation is acknowledged for support of the electron microscopy laboratory in Linköping, a Fellowship grant (P.E) and a scholar grant (L.H., 2016-0358).

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  1. These authors contributed equally: Youbing Li, Hui Shao.

Authors and Affiliations

  1. Engineering Laboratory of Advanced Energy Materials, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, China

    Youbing Li, Mian Li, Ke Chen, Xian-Hu Zha, Shiyu Du, Zhifang Chai & Qing Huang

  2. University of Chinese Academy of Sciences, Beijing, China

    Youbing Li

  3. CIRIMAT, Université de Toulouse, CNRS, Toulouse, France

    Hui Shao, Liyuan Liu, Benjamin Duployer, Patrick Rozier, Pierre-Louis Taberna & Patrice Simon

  4. Réseau sur le Stockage Electrochimique de l’Energie (RS2E), CNRS, Amiens, France

    Hui Shao, Liyuan Liu, Benjamin Duployer, Patrick Rozier, Encarnacion Raymundo-Piñero, Pierre-Louis Taberna & Patrice Simon

  5. College of Materials Science and Engineering, Sichuan University, Chengdu, China

    Zifeng Lin

  6. Thin Film Physics Division, Department of Physics, Chemistry, and Biology (IFM), Linköping University, Linköping, Sweden

    Jun Lu, Per O. Å. Persson, Per Eklund & Lars Hultman

  7. CNRS, CEMHTI UPR3079, Université Orléans, Orléans, France

    Encarnacion Raymundo-Piñero

  8. Institut Universitaire de France, Paris, France

    Patrice Simon

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Contributions

Q.H., Z.L., P.-L.T. and P.S. designed the research. Y.L. conducted material preparations and most of the characterization. H.S. and L.L. conducted the electrochemical tests and Z.L., P.-L.T. and P.S. analysed the data. H.S., B.D. and P.R. carried out the in situ XRD. J.L., P.O.Å.P, P.E. and L.H. carried out the STEM measurements. E.R.-P. performed the temperature-programmed desorption/mass spectrometry. Z.L., P.S. and Q.H. prepared the manuscript. All authors contributed to the discussion of the data and writing the paper.

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Correspondence to Zifeng Lin, Patrice Simon or Qing Huang.

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Supplementary Figs. 1–24, text, materials, Tables 1–8 and full reference list.

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Li, Y., Shao, H., Lin, Z. et al. A general Lewis acidic etching route for preparing MXenes with enhanced electrochemical performance in non-aqueous electrolyte. Nat. Mater. 19, 894–899 (2020). https://doi.org/10.1038/s41563-020-0657-0

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