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 journalArticle

79 Citations (Scopus)

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 1

Fingerprint

formic acid
rhodium
Rhodium
Carbon Dioxide
Carbon dioxide
carbon dioxide
Metals
catalyst
Catalysts
metal
thermal decomposition
fuel cell
Industrial applications
Fuel cells
Catalyst activity
Ion exchange
Pyrolysis
Carbon
carbon

All Science Journal Classification (ASJC) codes

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

Cite this

Chambers, Matthew B. ; Wang, Xia ; Elgrishi, Noémie ; Hendon, Christopher H. ; Walsh, Aron ; Bonnefoy, Jonathan ; Canivet, Jérôme ; Quadrelli, Elsje Alessandra ; Farrusseng, David ; Mellot-Draznieks, Caroline ; Fontecave, Marc. / Photocatalytic Carbon Dioxide Reduction with Rhodium-based Catalysts in Solution and Heterogenized within Metal-Organic Frameworks. In: ChemSusChem. 2015 ; Vol. 8, No. 4. pp. 603-608.
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Chambers, MB, Wang, X, Elgrishi, N, Hendon, CH, Walsh, A, Bonnefoy, J, Canivet, J, Quadrelli, EA, 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, vol. 8, no. 4, pp. 603-608. https://doi.org/10.1002/cssc.201403345

Photocatalytic Carbon Dioxide Reduction with Rhodium-based Catalysts in Solution and Heterogenized within Metal-Organic Frameworks. / Chambers, Matthew B.; Wang, Xia; Elgrishi, Noémie; Hendon, Christopher H.; Walsh, Aron; Bonnefoy, Jonathan; Canivet, Jérôme; Quadrelli, Elsje Alessandra; Farrusseng, David; Mellot-Draznieks, Caroline; Fontecave, Marc.

In: ChemSusChem, Vol. 8, No. 4, 01.02.2015, p. 603-608.

Research output: Contribution to journalArticle

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