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Spontaneous Formation of a ZnO Monolayer by the Redox Reaction of Zn on Graphene Oxide

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    Surfaces, Interfaces, and Applications

    Spontaneous Formation of a ZnO Monolayer by the Redox Reaction of Zn on Graphene Oxide
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    • Seungwoo Son
      Seungwoo Son
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Seungwoo Son
      Orcidhttp://orcid.org/0000-0001-6003-4382
    • , 
    • Yeonchoo Cho
      Yeonchoo Cho
      Samsung Advanced Institute of Technology (SAIT), Suwon 16678, Republic of Korea
      More by Yeonchoo Cho
    • , 
    • Hyo-Ki Hong
      Hyo-Ki Hong
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      More by Hyo-Ki Hong
      Orcidhttp://orcid.org/0000-0002-9722-9615
    • , 
    • Jongyeong Lee
      Jongyeong Lee
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Jongyeong Lee
    • , 
    • Jung Hwa Kim
      Jung Hwa Kim
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Jung Hwa Kim
      Orcidhttp://orcid.org/0000-0002-2615-963X
    • , 
    • Kangsik Kim
      Kangsik Kim
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
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    • , 
    • Yeongdong Lee
      Yeongdong Lee
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Yeongdong Lee
      Orcidhttp://orcid.org/0000-0001-9749-5270
    • , 
    • Aram Yoon
      Aram Yoon
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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      Orcidhttp://orcid.org/0000-0001-9520-306X
    • , 
    • Hyeon-Jin Shin*
      Hyeon-Jin Shin
      Samsung Advanced Institute of Technology (SAIT), Suwon 16678, Republic of Korea
      *Email: [email protected]
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      Orcidhttp://orcid.org/0000-0002-6992-6341
    • , and 
    • Zonghoon Lee*
      Zonghoon Lee
      Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      *Email: [email protected]
      More by Zonghoon Lee
      Orcidhttp://orcid.org/0000-0003-3246-4072
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 48, 54222–54229
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    https://doi.org/10.1021/acsami.0c18291
    Published November 18, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Graphene-based two-dimensional heterostructures are of substantial interest both for fundamental studies and their various potential applications. Particularly interesting are atomically thin semiconducting oxides on graphene, which uniquely combine a wide band gap and optical transparency. Here, we report the atomic-scale investigation of a novel self-formation of a ZnO monolayer from the Zn metal on a graphene oxide substrate. The spontaneous oxidation of the ultrathin Zn metal occurs by a reaction with oxygen supplied from the graphene oxide substrate, and graphene oxide is deoxygenated by a transfer of oxygen from O-containing functional groups to the zinc metal. The ZnO monolayer formed by this spontaneous redox reaction shows a graphene-like structure and a band gap of about 4 eV. This study demonstrates a unique and straightforward synthetic route to atomically thin two-dimensional heterostructures made from a two-dimensional metal oxide and graphene, formed by the spontaneous redox reaction of a very thin metal layer directly deposited on graphene oxide.

    Copyright © 2020 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.0c18291.

    • Bright field and AFM images of pristine graphene oxide monolayer; comparison of Zn deposited on graphene and graphene oxide their respective XPS spectrum; crystal structure model of ZnO on graphene for image simulation; crystalline defects in the polycrystalline ZnO monolayer on graphene oxide; metallic Zn to ZnO transition mechanism using DFT calculation; thickness of ZnO on graphene oxide; cross-sectional analysis of ZnO on graphene oxide; ARTEM images of partially reduced grapehen oxide after etching ZnO; and TOF-SIMS results (PDF)

    • Movie showing time-elapsed images of adsorbed ZnO adatoms on graphene oxide (MP4)

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    This article is cited by 12 publications.

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 48, 54222–54229
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c18291
    Published November 18, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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