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High-Energy-Density Hydrogen-Ion-Rocking-Chair Hybrid Supercapacitors Based on Ti3C2Tx MXene and Carbon Nanotubes Mediated by Redox Active Molecule

  • Minmin Hu
    Minmin Hu
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    School of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China
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  • , 
  • Cong Cui
    Cong Cui
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    School of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China
    More by Cong Cui
  • , 
  • Chao Shi
    Chao Shi
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    More by Chao Shi
  • , 
  • Zhong-Shuai Wu*
    Zhong-Shuai Wu
    Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
    *E-mail: [email protected]
    More by Zhong-Shuai Wu
    Orcidhttp://orcid.org/0000-0003-1851-4803
  • , 
  • Jinxing Yang
    Jinxing Yang
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    School of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China
    More by Jinxing Yang
  • , 
  • Renfei Cheng
    Renfei Cheng
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    School of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China
    More by Renfei Cheng
  • , 
  • Tianjia Guang
    Tianjia Guang
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    School of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China
    More by Tianjia Guang
  • , 
  • Hailong Wang
    Hailong Wang
    School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
    More by Hailong Wang
  • , 
  • Hongxia Lu
    Hongxia Lu
    School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
    More by Hongxia Lu
  • , and 
  • Xiaohui Wang*
    Xiaohui Wang
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
    *E-mail: [email protected]
    More by Xiaohui Wang
    Orcidhttp://orcid.org/0000-0001-7271-2662
Cite this: ACS Nano 2019, 13, 6, 6899–6905
Publication Date (Web):May 17, 2019
https://doi.org/10.1021/acsnano.9b01762
Copyright © 2019 American Chemical Society
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    Abstract

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    MXenes have emerged as promising high-volumetric-capacitance supercapacitor electrode materials, whereas their voltage windows are not wide. This disadvantage prevents MXenes from being made into aqueous symmetric supercapacitors with high energy density. To attain high energy density, constructing asymmetric supercapacitors is a reliable design choice. Here, we propose a strategy to achieve high energy density of hydrogen ion aqueous-based hybrid supercapacitors by integrating a negative electrode of Ti3C2Tx MXene and a positive electrode of redox-active hydroquinone (HQ)/carbon nanotubes. The two electrodes are separated by a Nafion film that is proton permeable in H2SO4 electrolyte. Upon charging/discharging, hydrogen ions shuttle back and forth between the cathode and anode for charge compensation. The proton-induced high capacitance of MXene and HQ, along with complementary working voltage windows, simultaneously enhance the electrochemical performance of the device. Specifically, the hybrid supercapacitors operate in a 1.6 V voltage window and deliver a high energy density of 62 Wh kg–1, which substantially exceeds those of the state-of-the-art aqueous asymmetric supercapacitors reported so far. Additionally, the device exhibits excellent cycling stability and the all-solid-state planar hybrid supercapacitor displays exceptional flexibility and integration for bipolar cells to boost the capacitance and voltage output. These encouraging results provide the possibility of designing high-energy-density noble-metal-free asymmetric supercapacitors for practical applications.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.9b01762.

    • SEM image, TEM image, CV curves and rate performance of Ti3C2Tx MXene; TEM images and Raman spectra of CNTs; CV curves of CNT-NaOH-MA film in H2SO4 electrolyte with different concentrations of HQ; EIS spectra of the assembled hybrid supercapacitor; photograph of the all-solid-state full cell device (PDF)

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