Visible light-driven H(2) production by hydrogenases attached to dye-sensitized TiO(2) nanoparticles.
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.
Reisner
Erwin
E
Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, Oxford, OX1 3QR, United Kingdom.
Powell
Daniel J
DJ
Cavazza
Christine
C
Fontecilla-Camps
Juan C
JC
Armstrong
Fraser A
FA
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*
D001426:Bacterial Proteins; D004396:Coloring Agents; D004800:Enzymes, Immobilized; C009495:titanium dioxide; D006859:Hydrogen; D014025:Titanium; C058560:nickel-iron-selenium hydrogenase; D006864:Hydrogenase