Promoting the photocatalytic NO oxidation activity of hierarchical porous g-C3N4 by introduction of nitrogen vacancies and charge channels

Abstract

Sluggish charge kinetics and moderate adsorption–desorption ability of gas molecules are major limitations for photocatalytic NOx elimination of bulk g-C3N4. A hierarchical porous g-C3N4 photocatalyst modified with N vacancies and charge channels (KCNN) was prepared by thermal polymerisation in KCl medium followed by quenching to increase the photocatalytic efficiency. The optimized KCNN sample exhibits highly enhanced photocatalytic NO removal rate (70.5%), which is superior to those of bulk g-C3N4 (38.1%), porous g-C3N4 (54.5%) and K-doped g-C3N4 (58.6%), respectively. X-ray photoelectron spectroscopy and electron paramagnetic resonance data reveal the successful formation of N vacancy in g-C3N4 framework. The enhanced activity of KCNN is ascribed to the enlarged surface area, expanded light absorption, low charge recombination efficiency and strong oxidation capability, respectively. In situ DRIFTS and density functional theory results suggest that the introduction of N vacancies and K+ ions enable control over NO adsorption and activation, leading to the implementation of a preferred pathway (NO → NO+ → NO3‾) and reduction in the emission of toxic intermediates. This work presents a potential idea for improving the charge transfer of layered materials and optimising the diffusion/adsorption/activation of gas molecules for photocatalytic NO oxidation.