Selective catalytic oxidation of formaldehyde on single V- and Cr-atom decorated magnetic C₄N₃ substrate: A first...

Formaldehyde (HCHO) is the most common indoor hazardous pollutant and has attracted great concern because its long-term exposure has adverse health effects on humans. Retention and catalytic oxidation of highly hazardous HCHO is an efficient and environmentally friendly method to use for air remediation, but a major obstacle to this procedure is the lack of an appropriate catalyst. Herein, two-dimensional magnetic C₄N₃ material with a 3d-transition metal as activate sites was systemically investigated in HCHO oxidation using density functional theory calculations. The results show that V-C₄N₃ and Cr-C₄N₃ have high structural stability and shallow activation barriers for O₂ decomposition; these characteristics provide the necessary precursors for the subsequent oxidation reaction. Moreover, the V-C₄N₃ and Cr-C₄N₃ catalysts have unique selective adsorption and catalysis toward HCHO in a mixture of some typical in-door volatile organic compounds (VOCs) and air. The corresponding dynamic barrier for each reaction step was investigated and the mechanism involved in HCHO oxidation was revealed in detail. Aggregation of metal atoms in the V-C₄N₃ and Cr-C₄N₃ catalysts is prevented by enormous diffusion resistance, and this is further confirmed by AIMD simulations. These results provide insightful guidance for developing advanced magnetic catalysts for HCHO oxidation to improve the remediation of air contaminants.