Oxygen Doping in Graphitic Carbon Nitride for Enhanced Photocatalytic Hydrogen Evolution

ChemSusChem. 2020 Sep 18;13(18):5041-5049. doi: 10.1002/cssc.202001317. Epub 2020 Aug 3.

Abstract

The incorporation of oxygenic groups could remarkably enhance the light absorption and charge separation of graphitic carbon nitride (g-C3 N4 ). The intrinsic role of oxygenic species on photocatalytic activity in g-C3 N4 has been intensively studied, but it is still not fully explored. Herein, the essential relationships between oxygenic functionalities and the catalytic performance are revealed. Results demonstrate that C-O-C functionality as an electron trap could help to increase the resistance of conduction transfer (Rct ) by limiting electrons transfer in CNx. In contrast, N-C-O functionality between different tri-s-triazine unites could promote the electrons transfer, leading to a reduced Rct in CNx. The best H2 production rate (3.70 mmol h-1 g-1 , 12.76-fold higher than that of CN) is obtained over CN3, because of the highest N-C-O ratio (rN-C-O ). The apparent quantum efficiency (AQE) of CN3 at 405 nm, 420 nm, 450 nm, 500 nm and 550 nm is 33.90 %, 20.88 %, 8.25 %, 3.66 % and 1.01 %, respectively.

Keywords: charge separation; graphitic carbon nitride; hydrogen production; photocatalysis; surface oxygen groups.