Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, Oxford, OX1 3QR, United Kingdom.
J Am Chem Soc. 2009 Dec 30;131(51):18457-66. doi: 10.1021/ja907923r.
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.
已经开展了一项关于能够利用可见光作为能源产生 H(2)的混合、酶修饰纳米粒子的研究，旨在为能够在环境条件下运行的 H(2)生产催化剂建立每个位点的性能标准。从脱硫微菌属 (Db [NiFeSe]-H) 中鉴定出 [NiFeSe]-氢化酶是一种特别有效的催化剂。优化后的系统由附着在 Ru 敏化染料 TiO(2)上的 Db [NiFeSe]-H 组成，三乙醇胺作为牺牲电子供体，在 pH 7 和 25 摄氏度下，即使在北欧典型的太阳辐射下，其 H(2)的周转频率也约为 50(mol H(2)) s(-1)(mol 总氢化酶)(-1)。该系统不仅在厌氧条件下，而且在长时间暴露于空气后也表现出高的电催化稳定性，因此使其足够坚固，可用于台式应用。
