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Issue 21, 2018
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Mechanism of photocatalytic water splitting with triazine-based carbon nitrides: insights from ab initio calculations for the triazine–water complex

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Abstract

Polymeric carbon-nitride materials consisting of triazine or heptazine units have recently attracted vast interest as photocatalysts for water splitting with visible light. Adopting the hydrogen-bonded triazine–water complex as a model system, we explored the photochemical reaction mechanisms involved in the water splitting reaction in this system, using wavefunction-based ab initio electronic-structure methods. It is shown that photoexcited triazine can abstract a hydrogen atom from the water molecule by the sequential transfer of an electron and a proton from water to triazine, resulting in the triazinyl-hydroxyl biradical in the electronic ground state. It is furthermore shown that the excess hydrogen atom of the triazinyl radical can be photodetached by a second photon, which regenerates the triazine molecule. The hydrogen-bonded water molecule is thus decomposed into hydrogen and hydroxyl radicals in a biphotonic photochemical reaction. These results shed light on the molecular mechanisms of the water-oxidation reaction catalyzed by triazine-based organic polymers.

Graphical abstract: Mechanism of photocatalytic water splitting with triazine-based carbon nitrides: insights from ab initio calculations for the triazine–water complex

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Publication details

The article was received on 28 Mar 2018, accepted on 08 May 2018 and first published on 11 May 2018


Article type: Paper
DOI: 10.1039/C8CP01998C
Citation: Phys. Chem. Chem. Phys., 2018,20, 14420-14430
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    Mechanism of photocatalytic water splitting with triazine-based carbon nitrides: insights from ab initio calculations for the triazine–water complex

    J. Ehrmaier, M. J. Janicki, A. L. Sobolewski and W. Domcke, Phys. Chem. Chem. Phys., 2018, 20, 14420
    DOI: 10.1039/C8CP01998C

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