A Rapid Microwave‐Assisted Thermolysis Route to Highly Crystalline Carbon Nitrides for Efficient Hydrogen Generation

Abstract

Highly crystalline graphitic carbon nitride (g-C₃N₄) with decreased structural imperfections benefits from the suppression of electron–hole recombination, which enhances its hydrogen generation activity. However, producing such g-C₃N₄ materials by conventional heating in an electric furnace has proven challenging. Herein, we report on the synthesis of high-quality g-C₃N₄ with reduced structural defects by judiciously combining the implementation of melamine–cyanuric acid (MCA) supramolecular aggregates and microwave-assisted thermolysis. The g-C₃N₄ material produced after optimizing the microwave reaction time can effectively generate H₂ under visible-light irradiation. The highest H₂ evolution rate achieved was 40.5 μmol h⁻¹, which is two times higher than that of a g-C₃N₄ sample prepared by thermal polycondensation of the same supramolecular aggregates in an electric furnace. The microwave-assisted thermolysis strategy is simple, rapid, and robust, thereby providing a promising route for the synthesis of high-efficiency g-C₃N₄ photocatalysts.