Utilizing artificial photosynthesis
for the conversion
of CO2 into value-added fuels has been recognized as a
promising
strategy for the ever-increasing energy crisis and the greenhouse
effect. Herein, the element doping engineering of red spherical g-C3N4 having oxygen bonded with compositional carbon
(C–O–C) for CO2 photoreduction has been explored
to address this challenge. The C–O bond was formed by hydrothermal
treatment with dicyandiamide and 1,3,5-trichlorotriazine. The experimental
and DFT results displayed the optimum oxygen substitution sites and
demonstrated that the oxygen doping greatly improved the light utilization
efficiency, CO2 affinity, and charge carrier transfer,
which enhanced photoreduction efficiency of CO2. The evolution
rates of CO (47.2 μmol g–1) and CH4 (9.1 μmol g–1) using O–CN were much
higher than that of bulk-CN without a cocatalyst. The main reason
was the contribution of the O 2p orbital to the conduction band (CB)
and valence band of O–CN, which effectively reduced the electron
mass, facilitating electron/hole separation and enhancing its fluidity.
Furthermore, the Fermi level also shifted to the bottom of the CB,
leading to higher electron density, which further improved the CO2 reduction ability. Our study marks an important step for
developing high-performance photocatalysts for reduction of CO2.