Copper Phosphide-Enhanced Lower Charge Trapping Occurrence in Graphitic-C₃N₄ for Efficient Noble-Metal-Free Photocatalytic H₂ Evolution

Abstract

Graphitic carbon nitride (g-C₃N₄) fundamental photophysical processes exhibit a high frequency of charge trapping due to physicochemical defects. In this study, a copper phosphide (Cu₃P) and g-C₃N₄ hybrid was synthesized via a facile phosphorization method. Cu₃P, as an electron acceptor, efficiently captures the photogenerated electrons and drastically improved the charge separation rate to cause a significantly enhanced photocatalytic performance. Moreover, the robust and intimate chemical interactions between Cu₃P and g-C₃N₄ offers a rectified charge-transfer channel that can lead to a higher H₂ evolution rate (HRE, 277.2 μmol h^-1 g^-1) for this hybrid that is up to 370 times greater than that achieved from using bare g-C₃N₄ (HRE, 0.75 μmol h^-1 g^-1) with a quantum efficiency of 3.74% under visible light irradiation (λ = 420 nm). To better determine the photophysical characteristics of the Cu₃P-induced charge antitrapping behavior, ultrafast time-resolved spectroscopy measurements were used to investigate the charge carriers' dynamics from femtosecond to nanosecond time domains. The experimental results clearly revealed that Cu₃P can effectively enhance charge transfer and suppress photoelectron-hole recombination.