Construction of Type-II Heterojunctions in Crystalline Carbon Nitride for Efficient Photocatalytic H2 Evolution.

Abstract

As an encouraging photocatalyst, crystalline carbon nitride (CCN) exhibits unsatisfactory photocatalytic activity and stability due to its rapid recombination of photo-generative carriers. Herein, high-crystalline g-C3N4 was prepared, including CCN obtained in KCl (K-CCN), LiCl-KCl mixture (Li/K-CCN), and LiCl-NaCl-KCl mixture (Li/Na/K-CCN), via the molten salt strategy using pre-prepared bulk carbon nitride (BCN) as a precursor. The obtained BCN sample was formed by heptazine-based units, which convert into triazine-based units for K-CCN. Heptazine and triazine are two isotypes that co-exist in the Li/K-CCN and Li/Na/K-CCN samples. Compared with BCN and other CCN samples, the as-prepared Li/Na/K-CCN sample exhibited the optimal photocatalytic hydrogen evolution rates (3.38 mmol·g-1·h-1 under simulated sunlight and 2.25 mmol·g-1·h-1 under visible light) and the highest apparent quantum yield (10.97%). The improved photocatalytic performance of the Li/Na/K-CCN sample is mainly attributed to the construction of type-II heterojunction and the institution of the built-in electric field between triazine-based CCN and heptazine-based BCN. This work provides a new strategy for the structural optimization and heterostructure construction of crystalline carbon nitride photocatalysts.