Protein Delivery of a Ni Catalyst to Photosystem I for Light-Driven Hydrogen Production

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• 作者：Sunshine C. Silver ; Jens Niklas ; Pingwu Du ; Oleg G. Poluektov ; David M. Tiede ; Lisa M. Utschig
• 刊名：Journal of the American Chemical Society
• 出版年：2013
• 出版时间：September 11, 2013
• 年：2013
• 卷：135
• 期：36
• 页码：13246-13249
• 全文大小：232K
• 年卷期：v.135,no.36(September 11, 2013)
• ISSN：1520-5126

文摘

The direct conversion of sunlight into fuel is a promising means for the production of storable renewable energy. Herein, we use Nature鈥檚 specialized photosynthetic machinery found in the Photosystem I (PSI) protein to drive solar fuel production from a nickel diphosphine molecular catalyst. Upon exposure to visible light, a self-assembled PSI-[Ni(P₂^PhN₂^Ph)₂](BF₄)₂ hybrid generates H₂ at a rate 2 orders of magnitude greater than rates reported for photosensitizer/[Ni(P₂^PhN₂^Ph)₂](BF₄)₂ systems. The protein environment enables photocatalysis at pH 6.3 in completely aqueous conditions. In addition, we have developed a strategy for incorporating the Ni molecular catalyst with the native acceptor protein of PSI, flavodoxin. Photocatalysis experiments with this modified flavodoxin demonstrate a new mechanism for biohybrid creation that involves protein-directed delivery of a molecular catalyst to the reducing side of Photosystem I for light-driven catalysis. This work further establishes strategies for constructing functional, inexpensive, earth-abundant solar fuel-producing PSI hybrids that use light to rapidly produce hydrogen directly from water.