title: Bioinspired molecular co-catalysts bonded to a silicon photocathode for solar hydrogen evolution.
abstract: The production of fuels from sunlight represents one of the main challenges in the development of a sustainable energy system. Hydrogen is the simplest fuel to produce and although platinum and other noble metals are efficient catalysts for photoelectrochemical hydrogen evolution, earth-abundant alternatives are needed for large-scale use. We show that bioinspired molecular clusters based on molybdenum and sulphur evolve hydrogen at rates comparable to that of platinum. The incomplete cubane-like clusters (Mo(3)S(4)) efficiently catalyse the evolution of hydrogen when coupled to a p-type Si semiconductor that harvests red photons in the solar spectrum. The current densities at the reversible potential match the requirement of a photoelectrochemical hydrogen production system with a solar-to-hydrogen efficiency in excess of 10%. The experimental observations are supported by density functional theory calculations of the Mo(3)S(4) clusters adsorbed on the hydrogen-terminated Si(100) surface, providing insights into the nature of the active site.
authors.affiliation: CINF, Department of Physics, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark.
authors.forename: Yidong
authors.initials: Y
authors.lastname: Hou
authors.forename: Billie L
authors.initials: BL
authors.lastname: Abrams
authors.forename: Peter C K
authors.initials: PC
authors.lastname: Vesborg
authors.forename: Mårten E
authors.initials: ME
authors.lastname: Björketun
authors.forename: Konrad
authors.initials: K
authors.lastname: Herbst
authors.forename: Lone
authors.initials: L
authors.lastname: Bech
authors.forename: Alessandro M
authors.initials: AM
authors.lastname: Setti
authors.forename: Christian D
authors.initials: CD
authors.lastname: Damsgaard
authors.forename: Thomas
authors.initials: T
authors.lastname: Pedersen
authors.forename: Ole
authors.initials: O
authors.lastname: Hansen
authors.forename: Jan
authors.initials: J
authors.lastname: Rossmeisl
authors.forename: Søren
authors.initials: S
authors.lastname: Dahl
authors.forename: Jens K
authors.initials: JK
authors.lastname: Nørskov
authors.forename: Ib
authors.initials: I
authors.lastname: Chorkendorff
mesh_terms: D002384:Catalysis; D006859:Hydrogen / Q000737:chemistry*; D010984:Platinum / Q000737:chemistry*; D012666:Semiconductors; D012825:Silicon / Q000737:chemistry*; D013472:Sunlight
chemical_list: D010984:Platinum; D006859:Hydrogen; D012825:Silicon