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Visible Light-Driven H 2 Production by Hydrogenases Attached to Dye-Sensitized TiO 2 Nanoparticles

2009; American Chemical Society; Volume: 131; Issue: 51 Linguagem: Inglês

10.1021/ja907923r

1943-2984

Erwin Reisner, Daniel Powell, Christine Cavazza, Juan C. Fontecilla‐Camps, Fräser A. Armstrong,

Ammonia Synthesis and Nitrogen Reduction

A study of hybrid, enzyme-modified nanoparticles able to produce H2 using visible light as the energy source has been carried out to establish per-site performance standards for H2 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 TiO2, with triethanolamine as a sacrificial electron donor, produces H2 at a turnover frequency of approximately 50 (mol H2) s−1 (mol total hydrogenase)−1 at pH 7 and 25 °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.