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Pore confinement effects and stabilization of carbon nitride oligomers in macroporous silica for photocatalytic hydrogen production

Qiao, S; Mitchell, RW; Coulson, B; Jowett, DV; Johnson, BRG; Brydson, R; Isaacs, M; ... Douthwaite, RE; + view all (2016) Pore confinement effects and stabilization of carbon nitride oligomers in macroporous silica for photocatalytic hydrogen production. Carbon , 106 pp. 320-329. 10.1016/j.carbon.2016.05.039. Green open access

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Abstract

An ordered macroporous host (mac-SiO2) has been used to prevent aggregation of layered photocatalysts based on carbon nitride. Using typical carbon nitride synthesis conditions, cyanamide was condensed at 550 °C in the presence and absence of mac-SiO2. Condensation in the absence of mac-SiO2 results in materials with structural characteristics consistent with the carbon nitride, melon, accompanied by ca. 2 wt% carbonization. For mac-SiO2 supported materials, condensation occurs with greater carbonization (ca. 6 wt%). On addition of 3 wt% Pt cocatalyst photocatalytic hydrogen production under visible light is found to be up to 10 times greater for the supported composites. Time-resolved photoluminescence spectroscopy shows that excited state relaxation is more rapid for the mac-SiO2 supported materials suggesting faster electron-hole recombination and that supported carbon nitride does not exhibit improved charge separation. CO2 temperature programmed desorption indicates that enhanced photoactivity of supported carbon nitride is attributable to an increased surface area compared to bulk carbon nitride and an increase in the concentration of weakly basic catalytic sites, consistent with carbon nitride oligomers.

Type: Article
Title: Pore confinement effects and stabilization of carbon nitride oligomers in macroporous silica for photocatalytic hydrogen production
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.carbon.2016.05.039
Publisher version: https://doi.org/10.1016/j.carbon.2016.05.039
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
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/10061537
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