When 2D g-C3N4 meets 0D CNQDs and 1D CNTs: A strategy for photocatalytic hydrogen production over a ternary non-metallic catalyst

Abstract

Utilizing solar energy to facilitate photocatalytic hydrogen production holds great promise in addressing the energy crisis. One material that shows tremendous potential in this field is two-dimensional graphitic carbon nitride (2D g-C3N4). However, the fast recombination rate of photogenerated carriers and the limited specific surface area impede its photocatalytic activity. This research endeavors to address these limitations by developing a ternary composite photocatalyst, CNQDs/g-C3N4/CNTs, by employing the microwave hydrothermal method. g-C3N4 was co-modified with zero-dimensional g-C3N4 quantum dots (0D CNQDs) and one-dimensional carbon nanotubes (1D CNTs). Incorporating CNQDs and the g-C3N4 interface facilitates the separation of photogenerated carriers, while the tubular channel of CNTs provides favorable conditions for transferring photogenerated electrons. Additionally, the introduction of CNQDs and CNTs significantly increases the specific surface area of the sample, thereby enhancing the number of reaction active sites available for the photocatalytic production of hydrogen. The hydrogen generation rate of the CNQDs/g-C3N4/CNTs is 1109.388 μmol⋅g−1⋅h−1, surpassing that of the single g-C3N4 specimen by 3.62 times. The application of density functional theory (DFT) calculations reinforces the enhanced performance of the composite through the synergistic effect of CNQDs and CNTs. This effect optimizes the adsorption behavior of the active intermediate (H*) and reduces the Gibbs free energy ΔG(H*) associated with the photocatalytic hydrogen evolution reaction.