Synthesis of Holey Graphene Nanoparticle CompoundsClick to copy article linkArticle link copied!
- David L. WhiteDavid L. WhiteDepartment of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United StatesMore by David L. White
- Levi LystromLevi LystromDepartment of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United StatesMore by Levi Lystrom
- Xiaoyun HeXiaoyun HeDepartment of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United StatesMore by Xiaoyun He
- Seth C. BurkertSeth C. BurkertDepartment of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United StatesMore by Seth C. Burkert
- Dmitri S. KilinDmitri S. KilinDepartment of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United StatesMore by Dmitri S. Kilin
- Svetlana KilinaSvetlana KilinaDepartment of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United StatesMore by Svetlana Kilina
- Alexander Star*Alexander Star*Email: [email protected]Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United StatesDepartment of Bioengineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, United StatesMore by Alexander Star
Abstract

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.
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