Efficient production of hydrogen from formic acid using a Covalent Triazine Framework supported molecular catalyst. Issue 5 (11th February 2015)

• Record Type: Journal Article
• Authors: Bavykina, A. V.; Goesten, M. G.; Kapteijn, F.; Makkee, M.; Gascon, J.
• Is Part Of: ChemSusChem. Volume 8:Issue 5(2015:Mar.)
• Page Start: 809
• Page End: 812
• Publication Date: 2015-02-11
• Subjects: Green chemistry -- Periodicals; Sustainable engineering -- Periodicals; Chemistry -- Periodicals; Chemical engineering -- Periodicals; 660
• DOI: 10.1002/cssc.201403173
• Languages: English
• ISSNs: 1864-5631

Abstract

<abstract abstract-type="main" xml:lang="en"> <title>Abstract</title> <p>A heterogeneous molecular catalyst based on Ir^IIICp* (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 <italic>β</italic>‐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.</p> </abstract>