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Synthesis of Holey Graphene Nanoparticle Compounds
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    Functional Nanostructured Materials (including low-D carbon)

    Synthesis of Holey Graphene Nanoparticle Compounds
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    • David L. White
      David L. White
      Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States
    • Levi Lystrom
      Levi Lystrom
      Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United States
      More by Levi Lystrom
    • Xiaoyun He
      Xiaoyun He
      Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States
      More by Xiaoyun He
    • Seth C. Burkert
      Seth C. Burkert
      Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States
    • Dmitri S. Kilin
      Dmitri S. Kilin
      Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United States
    • Svetlana Kilina
      Svetlana Kilina
      Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United States
    • Alexander Star*
      Alexander Star
      Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States
      Department of Bioengineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, United States
      *Email: [email protected]
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 32, 36513–36522
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    https://doi.org/10.1021/acsami.0c09394
    Published July 16, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    Bulk-scale syntheses of sp2 nanocarbon have typically been generated by extensive chemical oxidation to yield graphite oxide from graphite, followed by a reductive step. Materials generated via harsh random processes lose desirable physical characteristics. Loss of sp2 conjugation inhibits long-range electronic transport and the potential for electronic band manipulation. Here, we present a nanopatterned holey graphene material electronically hybridized with metal-containing nanoparticles. Oxidative plasma etching of highly ordered pyrolytic graphite via previously developed covalent organic framework (COF)-5-templated patterning yields bulk-scale materials for electrocatalytic applications and fundamental investigations into band structure engineering of nanocomposites. We establish a broad ability (Ag, Au, Cu, and Ni) to grow metal-containing nanoparticles in patterned holes in a metal precursor-dependent manner without a reducing agent. Graphene nanoparticle compounds (GNCs) show metal-contingent changes in the valence band structure. Density functional theory investigations reveal preferences for uncharged metal states, metal contributions to the valence band, and embedding of nanoparticles over surface incorporation. Ni–GNCs show activity for oxygen evolution reaction in alkaline media (1 M KOH). Electrocatalytic activity exceeds 10,000 mA/mg of Ni, shows stability for 2 h of continuous operation, and is kinetically consistent via a Tafel slope with Ni(OH)2-based catalysis.

    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.0c09394.

    • Experimental methods; images of electron microscopy of the as-patterned HOPG; RIE screening conditions; RIE without COF control experiments, Ag–GNCs, Cu–GNCs, Ni–GNCs, low salt and longer-time Cu–GNCs; Raman spectra of screening conditions; XPS metal-based metal loadings; valence XPS comparison of HG, GNCs, and metal references; UV–vis calibration curve of HG, postwash GNCs, and different Cu metal conditions for Cu–GNC; FTIR spectra of HG and the resulting GNCs; DLS/zeta potential measurements for RIE control, HG, and all GNCs; DFT calculations of metal clusters and DOS; electrochemical impedance spectra; and cyclic voltammogram (PDF)

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    This article is cited by 6 publications.

    1. Walker M. Vickery, Juhi Singh, Jason D. Orlando, Ting-Chih Lin, Julia Wang, Stefanie A. Sydlik. Polyurethane-grafted graphene oxide from repurposed foam mattress waste. RSC Advances 2025, 15 (4) , 2737-2748. https://doi.org/10.1039/D4RA06691J
    2. Abdiel de Jesús Espinosa-Champo, Gerardo G Naumis. Flat bands without twists: periodic holey graphene. Journal of Physics: Condensed Matter 2024, 36 (27) , 275703. https://doi.org/10.1088/1361-648X/ad39be
    3. Walker M. Vickery, Hunter B. Wood, Jason D. Orlando, Juhi Singh, Chenyun Deng, Li Li, Jing-Yi Zhou, Frederick Lanni, Aidan W. Porter, Stefanie A. Sydlik. Environmental and health impacts of functional graphenic materials and their ultrasonically altered products. NanoImpact 2023, 31 , 100471. https://doi.org/10.1016/j.impact.2023.100471
    4. V.D. Nithya. A review on holey graphene electrode for supercapacitor. Journal of Energy Storage 2021, 44 , 103380. https://doi.org/10.1016/j.est.2021.103380
    5. Muhammad Zahoor, Nausheen Nazir, Muhammad Iftikhar, Sumaira Naz, Ivar Zekker, Juris Burlakovs, Faheem Uddin, Abdul Waheed Kamran, Anna Kallistova, Nikolai Pimenov, Farhat Ali Khan. A Review on Silver Nanoparticles: Classification, Various Methods of Synthesis, and Their Potential Roles in Biomedical Applications and Water Treatment. Water 2021, 13 (16) , 2216. https://doi.org/10.3390/w13162216
    6. Qiang Zhao, Chiheng Chu, Xin Xiao, Baoliang Chen. Selectively coupled small Pd nanoparticles on sp2-hybridized domain of graphene-based aerogel with enhanced catalytic activity and stability. Science of The Total Environment 2021, 771 , 145396. https://doi.org/10.1016/j.scitotenv.2021.145396

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 32, 36513–36522
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c09394
    Published July 16, 2020
    Copyright © 2020 American Chemical Society

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