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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Electron-transfer sensitization of H_2 oxidation and CO_2 reduction catalysts using a single chromophore
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Electron-transfer sensitization of H_2 oxidation and CO_2 reduction catalysts using a single chromophore

机译：Electron-transfer sensitization of H_2 oxidation and CO_2 reduction catalysts using a single chromophore

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Energy-storing artificial-photosynthetic systems for CO_2 reduction must derive the reducing equivalents from a renewable source rather than from sacrificial donors. To this end, a homogeneous, integrated chromophore/two-catalyst system is described that is thermodynamically capable of photochemically driving the energy-storing reverse water–gas shift reaction (CO_2 + H_2 → CO + H_2O), where the reducing equivalents are provided by renewable H_2. The system consists of the chromophore zinc tetraphenylporphyrin (ZnTPP), H_2 oxidation catalysts of the form CpRCr(CO)3–, and CO_2 reduction catalysts of the type Re(bpy-4,4′-R2)(CO)3Cl. Using time-resolved spectroscopic methods, a comprehensive mechanistic and kinetic picture of the photoinitiated reactions of mixtures of these compounds has been developed. It has been found that absorption of a single photon by broadly absorbing ZnTPP sensitizes intercatalyst electron transfer to produce the substrate- active forms of each. The initial photochemical step is the heretofore unobserved reductive quenching of the low-energy T1 state of ZnTPP. Under the experimental conditions, the catalytically competent state decays with a second-order half-life of ～15 μs, which is of the right magnitude for substrate trapping of sensitized catalyst intermediates.

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