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Carbon Nitride Photocatalysts for Water Splitting: A Computational Perspective

Butchosa, C; Guiglion, P; Zwijnenburg, MA; (2014) Carbon Nitride Photocatalysts for Water Splitting: A Computational Perspective. JOURNAL OF PHYSICAL CHEMISTRY C , 118 (43) 24833 - 24842. 10.1021/jp507372n. Green open access

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Abstract

We study the thermodynamic ability of carbon nitride materials to act as water splitting photocatalysts using a computational approach that involves a combination of density functional theory (DFT) and time-dependent DFT (TD-DFT) calculations on cluster models of both triazine- and heptazine-based structures. We first use TD-DFT to calculate the absorption spectra of the different cluster models and compare these spectra to those measured experimentally and then calculate using DFT and TD-DFT the reduction potentials of the free electron, free hole, and exciton in these models. We predict that all classes of carbon nitride structures considered should thermodynamically be able to reduce protons and oxidize water. We further provide evidence for the hypothesis that the experimental lack of overall water splitting activity for pure carbon nitride arises from the fact that water oxidation is a four-hole reaction and hence very susceptible to competition with electron–hole recombination. Finally, we propose that the recently reported overall water splitting activity of carbon nitride loaded with polypyrrole nanoparticles arises from a junction formed at the interface of both materials, which assists in keeping electrons and holes apart.

Type: Article
Title: Carbon Nitride Photocatalysts for Water Splitting: A Computational Perspective
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/jp507372n
Publisher version: http://dx.doi.org/10.1021/jp507372n
Language: English
Additional information: This is an open access article published under a Creative Commons Attribution (CC-BY)License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/1458728
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