Edge electron-rich carbon nitride via π-acceptor frame with high-efficient charge separation for photocatalytic hydrogen evolution and environmental remediation

Abstract

Carbon nitride (g-C3N4) has broad application prospects in photocatalytic hydrogen production, but its photocatalytic efficiency is not ideal because of the rapid recombination of photogenerated electrons and holes. Herein, we developed a green strategy to fabricate hydroxyls and carbon-bridging co-modified g-C3N4 (CCN-OH) through a one-pot copolymerization and hydrothermal treatment. Experiments and density functional theory (DFT) calculations illustrated that carbon substitution of partial bridge nitrogen can improve the degree of electron delocalization to enhance the electron supply capacity of g-C3N4, and the exsitence of the electron-withdrawing OH group induces electron migration from carbon nitride to hydroxyl group, which further improves the efficiency of photogenerated charge separation. In addition, CCN-OH possess narrower band structure, resulting in an increased visible light utilization efficiency. The as-synthesized CCN-OH9 samples displayed an excellent photocatalytic activity for degradation of tetracycline with apparent reaction rate constant (k) of 0.018 min−1 and photocatalytic hydrogen evolution of 1880.3 μmol g-1h−1, which was respectively 2.2 and 9.8 times higher than that of CN.