Robust Photogeneration of H2 in Water Using Semiconductor Nanocrystals and a Nickel Catalyst

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Science  07 Dec 2012:
Vol. 338, Issue 6112, pp. 1321-1324
DOI: 10.1126/science.1227775

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Homogeneous systems for light-driven reduction of protons to H2 typically suffer from short lifetimes because of decomposition of the light-absorbing molecule. We report a robust and highly active system for solar hydrogen generation in water that uses CdSe nanocrystals capped with dihydrolipoic acid (DHLA) as the light absorber and a soluble Ni2+-DHLA catalyst for proton reduction with ascorbic acid as an electron donor at pH = 4.5, which gives >600,000 turnovers. Under appropriate conditions, the precious-metal–free system has undiminished activity for at least 360 hours under illumination at 520 nanometers and achieves quantum yields in water of over 36%.

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