Ultrafast Hole Transfer in Graphitic Carbon Nitride Imide Enabling Efficient H2O2 Photoproduction

作者：Hu, Qiushi; Huang, Yuling; Yu, Xuemeng; Gong, Shaokuan; Wen, Yifan; Liu, Yong; Li, Geng; Zhang, Qiang; Ye, Ruquan^*; Chen, Xihan^*

来源：ACS applied materials & interfaces, 2023, 15(36): 42611-42621.

DOI：10.1021/acsami.3c08466

• metal-free photocatalysis
• ultrafast spectroscopy
• hydrogen peroxide
• graphitic carbon nitride
• charge transfer mechanism

Solar-driven photocatalysis is a promising approach for renewable energy application. H2O2 photocatalysis by metal free graphitic carbon nitride has been gaining attention. Compared with traditional thermal catalysis, metal-free graphitic carbon nitride photocatalysis could lower material cost and achieve greener production of H2O2 . Also, to better guide photocatalyst design, a fundamental understanding of the reaction mechanism is needed. Here, we develop a series of model cost-effective metal free H2O2 photocatalysts made from graphitic carbon nitride (melem) and common imide groups. With 4,4'-oxydiphthalic anhydride (ODPA)-modified g-C3N4 , a H2O2 yield rate of 10781 mu mol/h.g.L could be achieved. Transient absorption and ex situ Fourier transform infrared (FTIR) measurements revealed an ultrafast charge transfer from the melem core to water with similar to 3 ps to form unique N-OH intermediates. The electron withdrawing ability of the anhydride group plays a role in governing the rate of electron transfer, ensuring efficient charge separation. Our strategy represents a new way to achieve a low material cost, simple synthesizing strategy, good environment impact, and high H2O2 production for renewable energy application.