Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 20, Issue 12, Pages 3292-3296Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201304845
Keywords
carbon dioxide; monolith; platinum; reduction; silanes
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Here, we demonstrate the use of Pt-0 nanoparticles immobilised on a polymeric monolithic support as a ligand-free heterogeneous catalytic system for the reduction of (CO2)-C-13 at room temperature and atmospheric pressure. The described system effectively reduces (CO2)-C-13 with dihydrosilanes as the hydrogen source to yield a mixture of silylformates, silylacetals and methoxysilanes, which upon further hydrolysis with D2O, produces their respective C1-type products, that is (HCOOD)-C-13, (CH2)-C-13(OD)(2) and (CH3OD)-C-13. If a monohydrosilane was used as the hydrogen source, a selective reduction of (CO2)-C-13 to a product mixture of only silylformates was observed. Addition of diethylamine to this reaction mixture results in the formation of (HCOOH)-C-13 and (Et2NCHO)-C-13. This robust catalytic system is not only maintenance-free and simple to handle, as compared with organometallic and organocatalyst systems, but also shows 3- to 11-fold better catalytic activity and exhibits higher turnover numbers (TONs) up to 21900 (activity=6.22kgCO2g(Pt)(-1)bar(-1)).
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