title: Visible light-driven H(2) production by hydrogenases attached to dye-sensitized TiO(2) nanoparticles.
abstract: A study of hybrid, enzyme-modified nanoparticles able to produce H(2) using visible light as the energy source has been carried out to establish per-site performance standards for H(2) production catalysts able to operate under ambient conditions. The [NiFeSe]-hydrogenase from Desulfomicrobium baculatum (Db [NiFeSe]-H) is identified as a particularly proficient catalyst. The optimized system consisting of Db [NiFeSe]-H attached to Ru dye-sensitized TiO(2), with triethanolamine as a sacrificial electron donor, produces H(2) at a turnover frequency of approximately 50 (mol H(2)) s(-1) (mol total hydrogenase)(-1) at pH 7 and 25 degrees C, even under the typical solar irradiation of a northern European sky. The system shows high electrocatalytic stability not only under anaerobic conditions but also after prolonged exposure to air, thus making it sufficiently robust for benchtop applications.
authors.affiliation: Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, Oxford, OX1 3QR, United Kingdom.
authors.forename: Erwin
authors.initials: E
authors.lastname: Reisner
authors.forename: Daniel J
authors.initials: DJ
authors.lastname: Powell
authors.forename: Christine
authors.initials: C
authors.lastname: Cavazza
authors.forename: Juan C
authors.initials: JC
authors.lastname: Fontecilla-Camps
authors.forename: Fraser A
authors.initials: FA
authors.lastname: Armstrong
mesh_terms: D001426:Bacterial Proteins; D004396:Coloring Agents; D004800:Enzymes, Immobilized; D006859:Hydrogen / Q000378:metabolism*; D006864:Hydrogenase / Q000378:metabolism*; D007700:Kinetics; D008027:Light; D053758:Nanoparticles / Q000737:chemistry*; D014025:Titanium / Q000737:chemistry*
chemical_list: D001426:Bacterial Proteins; D004396:Coloring Agents; D004800:Enzymes, Immobilized; C009495:titanium dioxide; D006859:Hydrogen; D014025:Titanium; C058560:nickel-iron-selenium hydrogenase; D006864:Hydrogenase