Photocatalytic carbon dioxide reduction with rhodium-based catalysts in solution and heterogenized within metal-organic frameworks

Matthew B. Chambers, Xia Wang, Noémie Elgrishi, Christopher H. Hendon, Aron Walsh, Jonathan Bonnefoy, Jérôme Canivet, Elsje Alessandra Quadrelli, David Farrusseng, Caroline Mellot-draznieks, Marc Fontecave

Research output: Contribution to journalArticlepeer-review

125 Citations (SciVal)

Abstract

The first photosensitization of a rhodium-based catalytic system for CO2 reduction is reported, with formate as the sole carbon-containing product. Formate has wide industrial applications and is seen as valuable within fuel cell technologies as well as an interesting H2-storage compound. Heterogenization of molecular rhodium catalysts is accomplished via the synthesis, post-synthetic linker exchange, and characterization of a new metal–organic framework (MOF) Cp*Rh@UiO-67. While the catalytic activities of the homogeneous and heterogeneous systems are found to be comparable, the MOF-based system is more stable and selective. Furthermore it can be recycled without loss of activity. For formate production, an optimal catalyst loading of ∼10 % molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H2. There is no precedent for a MOF catalyzing the latter reaction so far.
Original languageEnglish
Pages (from-to)603-608
JournalChemSusChem
Volume8
Issue number4
DOIs
Publication statusPublished - 22 Jan 2015

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