Fabricating the Robust g-C₃N₄ Nanosheets/Carbons/NiS Multiple Heterojunctions for Enhanced Photocatalytic H₂ Generation: An Insight into the Trifunctional Roles of Nanocarbons

Abstract

In this work, robust nanocarbons, including graphite (G), carbon nanotube (CNT), reduced graphene oxide (rGO), carbon black (CB), and acetylene black (AB), have been successfully coupled into the interfaces between g-C3N4 and NiS using a facile precipitation method. The results demonstrated that nanocarbons played trifunctional roles in boosting the photocatalytic H2 evolution over g-C3N4, which can not only act as effective H2-evolution co-catalysts but can also serve as conductive electron bridges to collect photogenerated electrons and boost the H2-evolution kinetics over the NiS co-catalysts. More interestingly, the nanocarbons can also result in the downshift of valence band of g-C3N4, thus facilitating the fast oxidation of triethanolamine and charge-carrier separation. Particularly, in all five ternary multiheterostructured systems, the g-C3N4-0.5%CB-1.0%NiS (weight ratio) and g-C3N4-0.5%AB-1.0%NiS photocatalysts exhibited the highest H2-evolution rates of 366.4 and 297.7 μmol g–1 h–1, which are 3.17 and 2.57 times higher than that of g-C3N4-1.0%NiS, respectively. Apparently, the significantly enhanced H2-evolution activity of multiheterostructured g-C3N4/carbon/NiS composite photocatalysts can be mainly ascribed to the trifunctional nanocarbons, which serve as the conductive electron bridges rather than the general co-catalysts. More importantly, it is revealed that the amorphous carbons with higher electrical conductivity and weaker electrocatalytic H2-evolution activity are more suitable interfacial bridges between g-C3N4 and NiS co-catalysts for maximizing the H2 generation. This work may give a new mechanistic insight into the development of multiheterostructured g-C3N4-based composite photocatalysts using the combination of trifunctional nanocarbon bridges and earth-abundant co-catalysts/semiconductors for various photocatalytic applications.