Efficient production of hydrogen from formic acid using a Covalent Triazine Framework supported molecular catalyst

A. V. Bavykina, M. G. Goesten*, F. Kapteijn, M. Makkee, J. Gascon

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

61 Scopus citations

Abstract

A heterogeneous molecular catalyst based on IrIIICp∗ (Cp∗=pentamethylcyclopentadienyl) attached to a covalent triazine framework (CTF) is reported. It catalyses the production of hydrogen from formic acid with initial turnover frequencies (TOFs) up to 27 000 h-1 and turnover numbers (TONs) of more than one million in continuous operation. The CTF support, with a Brunauer-Emmett-Teller (BET) surface area of 1800 m2 g-1, was constructed from an optimal 2:1 ratio of biphenyl and pyridine carbonitrile building blocks. Biphenyl building blocks induce mesoporosity and, therefore, facilitate diffusion of reactants and products whereas free pyridinic sites activate formic acid towards β-hydride elimination at the metal, rendering unprecedented rates in hydrogen production. The catalyst is air stable, produces CO-free hydrogen, and is fully recyclable. Hydrogen production rates of more than 60 mol L-1 h-1 were obtained at high catalyst loadings of 16 wt % Ir, making it attractive towards process intensification.

Original languageEnglish (US)
Pages (from-to)809-812
Number of pages4
JournalChemSusChem
Volume8
Issue number5
DOIs
StatePublished - Mar 1 2015
Externally publishedYes

Keywords

  • covalent triazine frameworks
  • formic acid
  • heterogeneous catalysis
  • hydrogen production
  • iridium

ASJC Scopus subject areas

  • Environmental Chemistry
  • Chemical Engineering(all)
  • Materials Science(all)
  • Energy(all)

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