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Modulation of the Electronic Properties of MXene (Ti3C2Tx) via Surface-Covalent Functionalization with Diazonium

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    Modulation of the Electronic Properties of MXene (Ti3C2Tx) via Surface-Covalent Functionalization with Diazonium
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    • Hongyue Jing
      Hongyue Jing
      SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University, Suwon 440-746, Korea
      More by Hongyue Jing
    • Hyeonwoo Yeo
      Hyeonwoo Yeo
      School of Electrical Engineering, Korea Advanced Institute of Science and Technology (KAIST),291 Daehak-ro, Yuseong-gu, Daejeon 34141, Korea
      More by Hyeonwoo Yeo
    • Benzheng Lyu
      Benzheng Lyu
      SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University, Suwon 440-746, Korea
      More by Benzheng Lyu
    • Junga Ryou
      Junga Ryou
      School of Electrical Engineering, Korea Advanced Institute of Science and Technology (KAIST),291 Daehak-ro, Yuseong-gu, Daejeon 34141, Korea
      More by Junga Ryou
    • Seunghyuk Choi
      Seunghyuk Choi
      SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University, Suwon 440-746, Korea
      More by Seunghyuk Choi
    • Jin-Hong Park
      Jin-Hong Park
      SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University, Suwon 440-746, Korea
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      Orcidhttp://orcid.org/0000-0001-8401-6920
    • Byoung Hun Lee
      Byoung Hun Lee
      Department of Electrical Engineering, Pohang University of Science and Technology, Pohang 37673, Korea
      More by Byoung Hun Lee
      Orcidhttp://orcid.org/0000-0002-4540-7731
    • Yong-Hoon Kim
      Yong-Hoon Kim
      School of Electrical Engineering, Korea Advanced Institute of Science and Technology (KAIST),291 Daehak-ro, Yuseong-gu, Daejeon 34141, Korea
      More by Yong-Hoon Kim
      Orcidhttp://orcid.org/0000-0001-5209-4908
    • Sungjoo Lee*
      Sungjoo Lee
      SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University, Suwon 440-746, Korea
      Department of Nano Engineering, Sungkyunkwan University, Suwon 440-746, Korea
      *Email: [email protected]
      More by Sungjoo Lee
      Orcidhttp://orcid.org/0000-0003-1284-3593
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    ACS Nano

    Cite this: ACS Nano 2021, 15, 1, 1388–1396
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    https://doi.org/10.1021/acsnano.0c08664
    Published January 5, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    The physical and chemical properties of MXenes are strongly dependent on surface terminations; thus, the tailoring of surface functional groups in two-dimensional transition-metal carbides (MXenes) may extend the applicability of these compelling materials to a wider set of fields. In this work, we demonstrate the chemical modification of Ti3C2Tx MXene via diazonium covalent chemistry and the subsequent effects on the electrical properties of MXene. The 4-nitrophenyl group was grafted onto the surface of MXene through a solid–liquid reaction, which was confirmed by various characterization methods, including X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, electron energy loss spectroscopy, atomic force microscopy, and transmission electron microscopy. The degree of modification of MXene is expediently tunable by adjusting the concentration of the diazonium salt solution. The work function of functionalized MXene is modifiable by regulating the quantity of grafted diazonium surface groups, with an adjustable range of around 0.6 eV. Further, in this study, the electrical properties of modified MXene are investigated through the fabrication of field-effect-transistor devices that utilize modified MXene as a channel material. It was demonstrated that with increasing concentration of 4-nitrophenyl groups grafted onto the surface the on/off current ratio of the modified MXene was improved to as much as 3.56, with a corresponding decrease in conductivity and mobility. The proposed approach of controlled modification of surface groups in Ti3C2Tx may imbue Ti3C2Tx with favorable electronic behaviors and demonstrate prospects for use in electronic field applications.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.0c08664.

    • AFM images, thickness, and relevant roughness of pristine Ti3C2Tx and 0.01 mM f- Ti3C2Tx; Ti 2p XPS spectra of pristine Ti3C2Tx and 0.01 and 10 mM f-Ti3C2Tx; EDS investigations of pristine and f-Ti3C2Tx; XRD patterns of pristine Ti3C2Tx and 1 mM f-Ti3C2Tx; SEM images of pristine Ti3C2Tx and 1 mM f- Ti3C2Tx; TEM images of pristine Ti3C2Tx and 1 mM f- Ti3C2Tx; schematic diagram of the Kelvin probe force microscope; plot of ln(R) as a function of 1/T of 0.01 and 10 mM f-Ti3C2Tx; Hall measurement of pristine Ti3C2Tx; Hall mobility of 0.01 and 10 mM f-Ti3C2Tx; top and side views of ball-and-stick models for Ti3C2O2 and Ti3C2(OH)2 without an 4-NB molecule and with one, two, and three (NB3) 4-NB molecules absorbed on the surface (PDF)

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    Cited By

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    This article is cited by 141 publications.

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