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

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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
Number of pages6
JournalChemSusChem
Volume8
Issue number4
DOIs
Publication statusPublished - 2015 Feb

All Science Journal Classification (ASJC) codes

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

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    Chambers, M. B., Wang, X., Elgrishi, N., Hendon, C. H., Walsh, A., Bonnefoy, J., Canivet, J., Quadrelli, E. A., Farrusseng, D., Mellot-Draznieks, C., & Fontecave, M. (2015). Photocatalytic Carbon Dioxide Reduction with Rhodium-based Catalysts in Solution and Heterogenized within Metal-Organic Frameworks. ChemSusChem, 8(4), 603-608. https://doi.org/10.1002/cssc.201403345