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Carbon nitride-TiO2 hybrid modified with hydrogenase for visible light driven hydrogen production.


ABSTRACT: A system consisting of a [NiFeSe]-hydrogenase (H2ase) grafted on the surface of a TiO2 nanoparticle modified with polyheptazine carbon nitride polymer, melon (CN x ) is reported. This semi-biological assembly shows a turnover number (TON) of more than 5.8 × 105 mol H2 (mol H2ase)-1 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 x -TiO2-H2ase construct was also active under UV-free solar light irradiation (? > 420 nm), where it showed a substantially higher activity than TiO2-H2ase and CN x -H2ase due, in part, to the formation of a CN x -TiO2 charge transfer complex and highly productive electron transfer to the H2ase. The CN x -TiO2-H2ase system sets a new benchmark for photocatalytic H2 production with a H2ase immobilised on a noble- and toxic-metal free light absorber in terms of visible light utilisation and stability.

SUBMITTER: Caputo CA 

PROVIDER: S-EPMC5512016 | biostudies-literature | 2015 Oct

REPOSITORIES: biostudies-literature

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Carbon nitride-TiO<sub>2</sub> hybrid modified with hydrogenase for visible light driven hydrogen production.

Caputo Christine A CA   Wang Lidong L   Beranek Radim R   Reisner Erwin E  

Chemical science 20150629 10


A system consisting of a [NiFeSe]-hydrogenase (H<sub>2</sub>ase) grafted on the surface of a TiO<sub>2</sub> nanoparticle modified with polyheptazine carbon nitride polymer, melon (CN <sub><i>x</i></sub> ) is reported. This semi-biological assembly shows a turnover number (TON) of more than 5.8 × 10<sup>5</sup> mol H<sub>2</sub> (mol H<sub>2</sub>ase)<sup>-1</sup> 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  ...[more]

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