Platinum nanoparticle inclusion into a carbonized polymer of intrinsic microporosity: Electrochemical characteristics of a catalyst for electroless hydrogen peroxide production

Robert K. Adamik, Naiara Hernández-Ibáñez, Jesus Iniesta, Jennifer K. Edwards, Alexander G.R. Howe, Robert D. Armstrong, Stuart H. Taylor, Alberto Roldan, Yuanyang Rong, Richard Malpass-Evans, Mariolino Carta, Neil B. McKeown, Daping He, Frank Marken

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Abstract

The one-step vacuum carbonization synthesis of a platinum nano-catalyst embedded in a microporous heterocarbon (Pt@cPIM) is demonstrated. A nitrogen-rich polymer of an intrinsic microporosity (PIM) precursor is impregnated with PtCl₆ 2- to give (after vacuum carbonization at 700 °C) a nitrogen-containing heterocarbon with embedded Pt nanoparticles of typically 1⁻4 nm diameter (with some particles up to 20 nm diameter). The Brunauer-Emmett-Teller (BET) surface area of this hybrid material is 518 m² g -1 (with a cumulative pore volume of 1.1 cm³ g -1) consistent with the surface area of the corresponding platinum-free heterocarbon. In electrochemical experiments, the heterocarbon-embedded nano-platinum is observed as reactive towards hydrogen oxidation, but essentially non-reactive towards bigger molecules during methanol oxidation or during oxygen reduction. Therefore, oxygen reduction under electrochemical conditions is suggested to occur mainly via a 2-electron pathway on the outer carbon shell to give H₂O₂. Kinetic selectivity is confirmed in exploratory catalysis experiments in the presence of H₂ gas (which is oxidized on Pt) and O₂ gas (which is reduced on the heterocarbon surface) to result in the direct formation of H₂O₂.

Original languageEnglish
Article number542
Pages (from-to)1-14
Number of pages14
JournalNanomaterials
Volume8
Issue number7
DOIs
Publication statusPublished - 18 Jul 2018

Funding

Funding: N.H.-I. and J.I. thank MINICINN, Spain (projects CTQ2013-48280-C3-3-R and CTQ2016-76231-C2-2-R) for financial support and the University of Alicante for support for a Ph.D. exchange visit. F.M. and N.B.M. thank the Leverhulme Foundation for financial support (RPG-2014-308: “New Materials for Ionic Diodes and Ionic Photodiodes”). Acknowledgments: J.K.E., A.G.R.H. and F.M. thank the Catalysis DTC in Cardiff. D.H. thanks the Royal Society for a Newton International Fellowship.

Keywords

  • Bifunctional catalysis
  • Heterocarbon
  • Microporosity
  • Peroxide
  • Voltammetry

ASJC Scopus subject areas

  • General Materials Science
  • General Chemical Engineering

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