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

Physical Chemistry Chemical Physics : PCCP
Johannes EhrmaierWolfgang Domcke

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.

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Citations

May 27, 2020·Physical Chemistry Chemical Physics : PCCP·Xiang HuangWolfgang Domcke
Mar 13, 2021·Physical Chemistry Chemical Physics : PCCP·S Alireza GhasemiThomas D Kühne
Sep 29, 2018·The Journal of Physical Chemistry Letters·Emily J RabeCody W Schlenker
Apr 22, 2020·The Journal of Physical Chemistry. a·Johannes EhrmaierWolfgang Domcke
Apr 13, 2019·The Journal of Physical Chemistry. a·Kentaro Yamamoto, Kazuo Takatsuka
Jan 1, 2019·Accounts of Chemical Research·Mohammad Z Rahman, C Buddie Mullins

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