Construction of three-coordinated (N3C) nitrogen vacancies in g-C3N4 for efficient photocatalytic CO2 reduction

Abstract

Defect engineering has been widely applied in the field of photocatalysis, and defects can be used to modify the surface structure and photoelectric properties of catalysts so as to achieve the purpose of regulating the activity and stability of catalysts. However, design of a highly efficient photocatalyst with abundant defects remains a challenging task in current research. Therefore, in this study, graphitic carbon nitride (g-C3N4) with abundant three-coordinated nitrogen (N3C) vacancies and pore structures was obtained using a facile hydrothermal method with the assistance of glycerol. Under visible light (λ > 420 nm) irradiation, the 50CN (volume ratio of glycerol/water is 50/10) catalyst exhibits a superior CO release rate (4.18 μmol g−1 h−1), which is 12.06 times higher than the reference GCN (0.32 μmol g−1 h−1), and the corresponding apparent quantum yields (AQY) of 50CN is 0.24 %, which is significantly higher than that of GCN (0.045 %). Successful introduction of N3C vacancies is conducive to broaden light response range of the catalyst, enhancing the separation and migration efficiency of photogenerated charges, and providing more adsorption active sites to promote the adsorption and activation of CO2 molecules, thus effectively boosting photocatalytic CO2 reduction activity. In addition, the N3C vacancies can effectively lower the CO2 activation energy barrier and reduce the energy consumption required for the reaction. This work offers valuable new insights into defect engineering in g-C3N4 for the development of high-performance photocatalysts for CO2 reduction.