期刊
CHEMSUSCHEM
卷 8, 期 4, 页码 603-608出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201403345
关键词
carbon dioxide reduction; hydrogen; metal-organic frameworks; photocatalysis; rhodium
资金
- Fondation de l'Orangerie for individual philanthropy
- French National Research Agency [Carbiored ANR-12-BS07-0024-03]
- French State Program Investissements d'Avenir (Grant LABEX DYNAMO) [ANR-11-LABEX-0011]
- CNRS-Cellule Energie
- Direction Generale de l'Armement (DGA)
- Engineering and Physical Sciences Research Council [EP/L000202/1] Funding Source: researchfish
- EPSRC [EP/L000202/1] Funding Source: UKRI
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.
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