Use of naturally abundant solar light for CO2 reduction is a green pathway to reduce carbon footprint. C3N5 is a promising visible-light photocatalyst with enhanced local electron concentration and more active N[dbnd]N sites compared to g-C3N4. We herein report development of mesoporous C-doped C3N5 through a simple copolymerisation of 3-amino-1,2,4-triazole with trimesic acid via hard-templating method, which demonstrated enhanced light absorption ability and delocalised π-electron density (as evident from density functional theory calculation), resulting in efficient charge transfer to the active surface sites of the photocatalyst. The optimised C-doped mesoporous C3N5 exhibited a superior photocatalytic CO2 reduction activity with the CO evolution of 116.6 µmol·g<sup>−1</sup>, which is 4-fold and 12-fold times higher than that of C3N5 and g-C3N4 respectively. The enhanced photocatalytic CO2 conversion efficiency can be attributed to the synergetic effects of π-electron modulation by C-doping and enhanced surface-active sites brought by mesoporosity.
Funding
This research was supported by a grant from the National Research Foundation of Korea and funded by the Ministry of Science, ICT, and Future Planning (Grant No.: 2022K1A4A8A01080312). A.V. and J-H.Y would like to thank ANSTO Australian Synchrotron research facilities. Financial support from the Slovenian Research and Innovation Agency (ARIS) through core funding P2-0152 (B. L.), project funding N1-0303, J2-4424 (M. H.) and J7-4638 (B. L.) and infrastructure funding I0-0039 (M. H.) is greatly appreciated. The computational resources were provided by the HPC RIVR consortium and EuroHPC JU through the HPC system Vega at the Institute of Information Science, Maribor, Slovenia.
National Research Foundation of Korea
Ministry of Science, ICT, and Future Planning | 2022K1A4A8A01080312
Slovenian Research and Innovation Agency (ARIS) | P2-0152
Slovenian Research and Innovation Agency (ARIS) | N1-0303
Slovenian Research and Innovation Agency (ARIS) | J2-4424
Slovenian Research and Innovation Agency (ARIS) | J7-4638
Slovenian Research and Innovation Agency (ARIS) | I0-0039