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
Affiliations
Robert K. Adamik
Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UK
Naiara Hernández-Ibáñez
Departamento de Química Física e Instituto Universitario de Electroquímica, Universidad de Alicante, Apartado 99, 03080 Alicante, Spain
Jesus Iniesta
Departamento de Química Física e Instituto Universitario de Electroquímica, Universidad de Alicante, Apartado 99, 03080 Alicante, Spain
Jennifer K. Edwards
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK
Alexander G. R. Howe
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK
Robert D. Armstrong
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK
Stuart H. Taylor
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK
Alberto Roldan
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK
Yuanyang Rong
Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UK
Richard Malpass-Evans
East Chem, School of Chemistry, University of Edinburgh, Joseph Black Building, David Brewster Road, Edinburgh, Scotland EH9 3FJ, UK
Mariolino Carta
Department of Chemistry, Swansea University, College of Science, Grove Building, Singleton Park, Swansea SA2 8PP, UK
Neil B. McKeown
East Chem, School of Chemistry, University of Edinburgh, Joseph Black Building, David Brewster Road, Edinburgh, Scotland EH9 3FJ, UK
Daping He
Hubei Engineering Research Center of RF-Microwave Technology and Application, School of Science, Wuhan University of Technology, Wuhan 430070, China
Frank Marken
Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UK
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 PtCl62− 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.
