Wiring of Photosystem II to Hydrogenase for Photoelectrochemical Water Splitting

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• 作者：Dirk Mersch ; Chong-Yong Lee ; Jenny Zhenqi Zhang ; Katharina Brinkert ; Juan C. Fontecilla-Camps ; A. William Rutherford ; Erwin Reisner
• 刊名：Journal of the American Chemical Society
• 出版年：2015
• 出版时间：July 8, 2015
• 年：2015
• 卷：137
• 期：26
• 页码：8541-8549
• 全文大小：489K
• ISSN：1520-5126

文摘

In natural photosynthesis, light is used for the production of chemical energy carriers to fuel biological activity. The re-engineering of natural photosynthetic pathways can provide inspiration for sustainable fuel production and insights for understanding the process itself. Here, we employ a semiartificial approach to study photobiological water splitting via a pathway unavailable to nature: the direct coupling of the water oxidation enzyme, photosystem II, to the H₂ evolving enzyme, hydrogenase. Essential to this approach is the integration of the isolated enzymes into the artificial circuit of a photoelectrochemical cell. We therefore developed a tailor-made hierarchically structured indium鈥搕in oxide electrode that gives rise to the excellent integration of both photosystem II and hydrogenase for performing the anodic and cathodic half-reactions, respectively. When connected together with the aid of an applied bias, the semiartificial cell demonstrated quantitative electron flow from photosystem II to the hydrogenase with the production of H₂ and O₂ being in the expected two-to-one ratio and a light-to-hydrogen conversion efficiency of 5.4% under low-intensity red-light irradiation. We thereby demonstrate efficient light-driven water splitting using a pathway inaccessible to biology and report on a widely applicable in vitro platform for the controlled coupling of enzymatic redox processes to meaningfully study photocatalytic reactions.