Introduction of a Hydroxyl Self-Sacrificing Surface on Ultrathin Poly(heptazine imide) Nanosheets by KCl Grafting: A New Strategy to Improve the Photocatalytic Production of HO.

The generation of HO through photocatalysis is increasingly recognized as a viable approach for addressing the energy and environmental challenges encountered in industrial production processes. In this research, we synthesized ultrathin (1 nm) poly(heptazine imide) (PHI) nanosheets as a photocatalyst by a one-step KCl molten salt process. The utilization of Fourier transform infrared and X-ray photoelectron spectroscopy substantiated that the interlayer-bonded potassium atoms induce polarization in water molecules, facilitating the attachment of hydroxyl groups on the surfaces of nanosheets. These groups serve as self-sacrificing entities, promoting the reaction that leads to the generation of HO. The preparation temperature and KCl doping amount factors for the HO generation rate were investigated, and the mechanism of the KCl-bonded structure on photogeneration charge separation transport was analyzed. Owing to the elevated crystallization and the presence of surface self-sacrificing hydroxyl groups, the rate of HO production reaches 6117.5 and 308.35 μmol·g·h under visible-light irradiation (λ ≥ 420 nm) in isopropanol solution and pure water, respectively. These rates are 30 and 18.7 times higher than those observed for bulk g-CN, respectively. The photocatalytic kinetic processes for HO formation and decomposition were also calculated to investigate the catalyst activities.