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Photocatalytic Hydrogen Production using Polymeric Carbon Nitride with a Hydrogenase and a Bioinspired Synthetic Ni Catalyst.

ABSTRACT: Solar-light-driven H₂ production in water with a [NiFeSe]-hydrogenase (H₂ase) and a bioinspired synthetic nickel catalyst (NiP) in combination with a heptazine carbon nitride polymer, melon (CN_x), is reported. The semibiological and purely synthetic systems show catalytic activity during solar light irradiation with turnover numbers (TONs) of more than 50 000 mol H₂ (mol H₂ase)^-1 and approximately 155 mol H₂ (mol NiP)^-1 in redox-mediator-free aqueous solution at pH 6 and 4.5, respectively. Both systems maintained a reduced photoactivity under UV-free solar light irradiation (?>420 nm).

SUBMITTER: Caputo CA

PROVIDER: S-EPMC4535659 | biostudies-literature | 2014 Oct

REPOSITORIES: biostudies-literature

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Photocatalytic Hydrogen Production using Polymeric Carbon Nitride with a Hydrogenase and a Bioinspired Synthetic Ni Catalyst.

Caputo Christine A CA Gross Manuela A MA Lau Vincent W VW Cavazza Christine C Lotsch Bettina V BV Reisner Erwin E

Angewandte Chemie (Weinheim an der Bergstrasse, Germany) 20140909 43

Solar-light-driven H2 production in water with a [NiFeSe]-hydrogenase (H2ase) and a bioinspired synthetic nickel catalyst (NiP) in combination with a heptazine carbon nitride polymer, melon (CNx), is reported. The semibiological and purely synthetic systems show catalytic activity during solar light irradiation with turnover numbers (TONs) of more than 50 000 mol H2 (mol H2ase)-1 and approximately 155 mol H2 (mol NiP)<s ...[more]

PMID: 26300567

Similar Datasets

Photocatalytic hydrogen production using polymeric carbon nitride with a hydrogenase and a bioinspired synthetic Ni catalyst.

Project description:Solar-light-driven H2 production in water with a [NiFeSe]-hydrogenase (H2ase) and a bioinspired synthetic nickel catalyst (NiP) in combination with a heptazine carbon nitride polymer, melon (CN(x)), is reported. The semibiological and purely synthetic systems show catalytic activity during solar light irradiation with turnover numbers (TONs) of more than 50,000?mol?H2(mol?H2ase)(-1) and approximately 155?mol?H2?(mol?NiP)(-1) in redox-mediator-free aqueous solution at pH?6 and 4.5, respectively. Both systems maintained a reduced photoactivity under UV-free solar light irradiation (?>420?nm).

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Project description:Visible light-driven photocatalytic reduction of protons to H2 is considered a promising way of solar-to-chemical energy conversion. Effective transfer of the photogenerated electrons and holes to the surface of the photocatalyst by minimizing their recombination is essential for achieving a high photocatalytic activity. In general, a sacrificial electron donor is used as a hole scavenger to remove photogenerated holes from the valence band for the continuation of the photocatalytic hydrogen (H2 ) evolution process. Here, for the first time, the hole-transfer dynamics from Pt-loaded sol-gel-prepared graphitic carbon nitride (Pt-sg-CN) photocatalyst were investigated using different adsorbed hole acceptors along with a sacrificial agent (ascorbic acid). A significant increment (4.84 times) in H2 production was achieved by employing phenothiazine (PTZ) as the hole acceptor with continuous H2 production for 3 days. A detailed charge-transfer dynamic of the photocatalytic process in the presence of the hole acceptors was examined by time-resolved photoluminescence and in situ electron paramagnetic resonance studies.

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Project description:In addition to the significance of photocatalytic hydrogen evolution, the utilization of the in situ generated H/D (deuterium) active species from water splitting for artificial photosynthesis of high value-added chemicals is very attractive and promising. Herein, photocatalytic water splitting technology is utilized to generate D-active species (i.e., Dad) that can be stabilized on anchored 2nd metal catalyst and are readily for tandem controllable deuterations of carbon-carbon multibonds to produce high value-added D-labeled chemicals/pharmaceuticals. A highly crystalline K cations intercalated polymeric carbon nitride (KPCN), rationally designed, and fabricated by a solid-template induced growth, is served as an ultraefficient photocatalyst, which shows a greater than 18-fold enhancement in the photocatalytic hydrogen evolution over the bulk PCN. The photocatalytic in situ generated D-species by superior KPCN are utilized for selective deuteration of a variety of alkenes and alkynes by anchored 2nd catalyst, Pd nanoparticles, to produce the corresponding D-labeled chemicals and pharmaceuticals with high yields and D-incorporation. This work highlights the great potential of developing photocatalytic water splitting technology for artificial photosynthesis of value-added chemicals instead of H2 evolution.

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