Triplet State Photosensitization of Nanocrystalline Metal Oxide Electrodes by Zinc-Substituted Cytochrome c: Application to Hydrogen Evolution
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- 作者：Yeni Astuti ; Emilio Palomares ; Saif Ahmed Haque ; and James Robert Durrant
- 刊名：Journal of the American Chemical Society
- 出版年：2005
- 出版时间：November 2, 2005
- 年：2005
- 卷：127
- 期：43
- 页码：15120 - 15126
- 全文大小：356K
- 年卷期：v.127,no.43(November 2, 2005)
- ISSN：1520-5126
文摘
The interfacing of nanostructured semiconductor photoelectrodes with redox proteins is aninnovative approach to the development of artificial photosynthetic systems. In this paper, we haveinvestigated the photoinduced electron-transfer reactions of zinc-substituted cytochrome c, ZnCyt-c,immobilized on mesoporous, nanocrystalline metal oxide electrodes. Efficient electron injection from thetriplet state of ZnCyt-c is observed into TiO2 electrodes (t50% ~ 100 
s) resulting in a long-lived charge-separated state (lifetime of up to 0.4 s). Further studies were undertaken as a function of electrolyte pHand metal oxide employed. Optimum yield of a long-lived charge-separated state was observed employingTiO2 electrodes at pH 5, consistent with our previous studies of analogous dye-sensitized metal oxideelectrodes. The addition of EDTA as a sacrificial electron donor to the electrolyte resulted in efficientphotogeneration of molecular hydrogen, with a quantum yield per one absorbed photon of 10 ± 5%.
s) resulting in a long-lived charge-separated state (lifetime of up to 0.4 s). Further studies were undertaken as a function of electrolyte pHand metal oxide employed. Optimum yield of a long-lived charge-separated state was observed employingTiO2 electrodes at pH 5, consistent with our previous studies of analogous dye-sensitized metal oxideelectrodes. The addition of EDTA as a sacrificial electron donor to the electrolyte resulted in efficientphotogeneration of molecular hydrogen, with a quantum yield per one absorbed photon of 10 ± 5%.