Caputo Christine A, Wang Lidong, Beranek Radim, Reisner Erwin
Christian Doppler Laboratory for Sustainable SynGas Chemistry , Department of Chemistry , Cambridge University , Lensfied Road , Cambridge CB2 1EW , UK . Email:
Faculty of Chemistry and Biochemistry , Ruhr-Universität Bochum , Universitätsstraße 150 , 44780 Bochum , Germany.
Chem Sci. 2015 Oct 1;6(10):5690-5694. doi: 10.1039/c5sc02017d. Epub 2015 Jun 29.
A system consisting of a [NiFeSe]-hydrogenase (Hase) grafted on the surface of a TiO nanoparticle modified with polyheptazine carbon nitride polymer, melon (CN ) is reported. This semi-biological assembly shows a turnover number (TON) of more than 5.8 × 10 mol H (mol Hase) after 72 h in a sacrificial electron donor solution at pH 6 during solar AM 1.5 G irradiation. An external quantum efficiency up to 4.8% for photon-to-hydrogen conversion was achieved under irradiation with monochromatic light. The CN -TiO-Hase construct was also active under UV-free solar light irradiation ( > 420 nm), where it showed a substantially higher activity than TiO-Hase and CN -Hase due, in part, to the formation of a CN -TiO charge transfer complex and highly productive electron transfer to the Hase. The CN -TiO-Hase system sets a new benchmark for photocatalytic H production with a Hase immobilised on a noble- and toxic-metal free light absorber in terms of visible light utilisation and stability.
报道了一种由接枝在经聚七嗪碳氮聚合物（密勒胺，CN ）修饰的TiO纳米颗粒表面的[NiFeSe] -氢化酶（Hase）组成的系统。在模拟太阳AM 1.5 G光照下，该半生物组件在pH值为6的牺牲电子供体溶液中经过72小时后，显示出超过5.8×10 mol H₂/（mol Hase）的周转数（TON）。在单色光照射下，实现了高达4.8%的光子到氢气转换的外部量子效率。CN -TiO - Hase结构在无紫外光的太阳光照射（>420 nm）下也具有活性，部分由于形成了CN -TiO电荷转移复合物以及向Hase的高效电子转移，其显示出比TiO - Hase和CN -Hase更高的活性。就可见光利用和稳定性而言，CN -TiO - Hase系统为将Hase固定在无贵金属和有毒金属的光吸收剂上进行光催化产氢树立了新的标杆。
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