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Article Dans Une Revue ChemSusChem Année : 2015

Photocatalytic Carbon Dioxide Reduction with Rhodium-based Catalysts in Solution and Heterogenized within Metal-Organic Frameworks

M. B. Chambers
  • Fonction : Auteur
X. Wang
  • Fonction : Auteur
N. Elgrishi
  • Fonction : Auteur
C. H. Hendon
  • Fonction : Auteur
A. Walsh
  • Fonction : Auteur
J. Bonnefoy
  • Fonction : Auteur
E. A. Quadrelli
C. Mellot-Draznieks

Résumé

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 H-2-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 approximate to 10% molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H-2. There is no precedent for a MOF catalyzing the latter reaction so far.

Dates et versions

hal-01149254 , version 1 (06-05-2015)

Identifiants

Citer

M. B. Chambers, X. Wang, N. Elgrishi, C. H. Hendon, A. Walsh, et al.. Photocatalytic Carbon Dioxide Reduction with Rhodium-based Catalysts in Solution and Heterogenized within Metal-Organic Frameworks. ChemSusChem, 2015, 8 (4), pp.603-608. ⟨10.1002/cssc.201403345⟩. ⟨hal-01149254⟩
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