Journal
ACS APPLIED ENERGY MATERIALS
Volume 1, Issue 11, Pages 6524-6534Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.8b01441
Keywords
g-C3N4; H-2 evolution CO2; photoreduction; optoelectronic properties; solar fuels; photocatalysis
Funding
- Engineering and Physical Sciences Research Council [EP/1508320]
- EU [658270]
- Department of Chemical Engineering at Imperial College London
- EPSRC [EP/N024206/1] Funding Source: UKRI
- Marie Curie Actions (MSCA) [658270] Funding Source: Marie Curie Actions (MSCA)
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Graphitic carbon nitride (g-C3N4) is regarded as an attractive photocatalyst for solar fuel production, i.e., H-2 evolution and CO, photoreduction. Yet, its structural, chemical and optoelectronic properties are very much dependent on the synthesis method and are likely to contribute differently whether H-2 evolution or CO, reduction is considered. Little is known about this aspect making it difficult to tailor g-C3N4 structure and chemistry for a specific photoreaction. Herein, we create g-C3N4 of varying chemical, structural and optical features by applying specific thermal treatments and investigating the effects of the materials properties on solar fuel production. The samples were characterized across scales using spectroscopic, analytical and imaging tools, with particular attention given to the analyses of trap states. In the case of H-2 evolution, the reaction is controlled by light absorption and charge separation enabled by the presence of trap states created by N vacancies. In the case of CO, photoreduction, reactant adsorption appears as a dominating factor. The analyses also suggest that the thermal treatment leads to the formation of trap states located close to the valence band of g-C3N4.
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