We report soft-oxometalate catalytic systems based on various metal oxide catalysts to oxidize H2O and utilize the generated H+s and e−s for reduction of CO2 with a TON of 1366 (effectively 1.4 x 106).
Photocatalytic CO2 reduction in water is one of the most attractive research pursuits of our time. In this article we report a giant polyoxometalate {Mo368} based homogeneous catalytic system, which efficiently reduces CO2 to formic acid with a maximum turnover number (TON) of 27,666, turnover frequency (TOF) of 4,611 h−1 and external quantum efficiency of the reaction is 0.6%. The catalytic system oxidizes water and releases electrons, and these electrons are further utilized for the reduction of CO2 to formic acid. A maximum of 8.3 mmol of formic acid was observed with the loading of 0.3 μmol of the catalyst. Our catalyst material is also stable throughout the reaction. The starting materials for this experiment are CO2 and H2O and the end products are HCOOH and O2. The formic acid formed in this reaction is an important H2 gas carrier and thus significant in renewable energy research.
Currently, photochemical carbon dioxide reduction is a most sought‐after process as it involves the simultaneous removal of greenhouse CO2 gas and the production of useful products. In this study, we report the selective formation of formaldehyde in photochemical carbon dioxide reduction using a reduced polyoxometalate (POM) based catalyst. By simply tuning the redox state of the metal centre in the POM, we can obtain the more reduced product formaldehyde from carbon dioxide. As a result of the high MoV/MoVI ratio in the cluster, formaldehyde is obtained as the major product as opposed to formic acid. Since the catalyst POM 1 itself readily absorbs light, no external photosensitizer is used. In the reduction process of carbon dioxide, water acts as the electron donor and is oxidized to oxygen rendering the whole process viable and green. (1=Mo16=[{(CH3)NH2}4{(MoV2O4)6(μ2‐OH)10(μ2‐O)2(μ3‐OH)2(μ3‐O)2(MoVIO3H)4}]0.94[{(MoV2O4)6(μ2‐OH)10(μ2‐O)2(MoVIO3H)4}{MoVI(μ3‐O)4}]0.06).
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