Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 131, Issue 51, Pages 18457-18466Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja907923r
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Funding
- EPSRC [EP/H00338X/1]
- BBSRC [BB/D52222X/1]
- CEA
- CNRS
- ANR [PNRB2006]
- BBSRC [BB/H003878/1] Funding Source: UKRI
- EPSRC [EP/D047943/1, EP/H00338X/1] Funding Source: UKRI
- Biotechnology and Biological Sciences Research Council [BB/D52222X/1, BB/H003878/1] Funding Source: researchfish
- Engineering and Physical Sciences Research Council [EP/D047943/1, EP/H00338X/1] Funding Source: researchfish
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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 TiO2, 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.
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