title: Robust photogeneration of H2 in water using semiconductor nanocrystals and a nickel catalyst.
abstract: Homogeneous systems for light-driven reduction of protons to H(2) 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 Ni(2+)-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%.
authors.affiliation: Department of Chemistry, University of Rochester, Rochester, NY 14627, USA.
authors.forename: Zhiji
authors.initials: Z
authors.lastname: Han
authors.forename: Fen
authors.initials: F
authors.lastname: Qiu
authors.forename: Richard
authors.initials: R
authors.lastname: Eisenberg
authors.forename: Patrick L
authors.initials: PL
authors.lastname: Holland
authors.forename: Todd D
authors.initials: TD
authors.lastname: Krauss
mesh_terms: D019187:Cadmium Compounds / Q000737:chemistry; D002384:Catalysis; D006859:Hydrogen / Q000737:chemistry*; D009532:Nickel / Q000737:chemistry*; D055668:Photochemical Processes; D045663:Quantum Dots; D018036:Selenium Compounds / Q000737:chemistry; D008063:Thioctic Acid / Q000031:analogs & derivatives / Q000737:chemistry; D014867:Water / Q000737:chemistry*
chemical_list: D019187:Cadmium Compounds; D018036:Selenium Compounds; D014867:Water; D008063:Thioctic Acid; C015144:dihydrolipoic acid; D009532:Nickel; D006859:Hydrogen; C058667:cadmium selenide