The immobilization of a photocatalyst on a proper support is pivotal for practical environmental applications. In this work, graphitic carbon nitride (g-C3N4) as a rising visible light photocatalyst was first immobilized on structured Al2O3 ceramic foam by a novel in situ approach. Immobilized g-C3N4 was applied for photocatalytic removal of 600 ppb level NO in air under real indoor illumination of an energy-saving lamp. The photocatalytic activity of immobilized g-C3N4 was gradually improved as the pyrolysis temperature was increased from 450 to 600 °C. The optimized conditions for g-C3N4 immobilization on Al2O3 supports can be achieved at 600 °C for 2 h. The NO removal ratio could reach up to 77.1%, exceeding that of other types of well-known immobilized photocatalysts. Immobilized g-C3N4 was stable in activity and can be used repeatedly without deactivation. The immobilization of g-C3N4 on Al2O3 ceramic foam was found to be firm enough to overwhelm the continuous air flowing, which can be ascribed to the special chemical interaction between g-C3N4 and Al2O3. On the basis of the 5,5'-dimethyl-1-pirroline-N-oxide electron spin resonance (DMPO ESR) spin trapping and reaction intermediate monitoring, the active species produced from g-C3N4 under illumination were confirmed and the reaction mechanism of photocatalytic NO oxidation by g-C3N4 was revealed. The present work could provide new perspectives for promoting large-scale environmental applications of supported photocatalysts.

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Graphitic carbon nitride (g-C3N4) is a visible light photocatalyst, limited by low activity mainly caused by rapid recombination of charge carriers. In the present work, honeycomb-like g-C3N4 was synthesized via thermal condensation of urea with addition of water at 450 °C for 1 h. Prolonging the condensation time caused the morphology of g-C3N4 to change from a porous honeycomb structure to a velvet-like nanoarchitecture. Unlike in previous studies, the photocatalytic activity of g-C3N4 decreased with increasing surface area. The honeycomb-like g-C3N4 with a relatively low surface area showed highly enhanced photocatalytic activity with an NO removal ratio of 48%. The evolution of NO2 intermediate was dramatically inhibited over the honeycomb-like g-C3N4. The short and long lifetimes of the charge carriers for honeycomb-like g-C3N4 were unprecedentedly prolonged to 22.3 and 165.4 ns, respectively. As a result, the honeycomb-like g-C3N4 was highly efficient and stable in activity and could be used repeatedly. Addition of water had the following multiple positive effects on g-C3N4: (1) formation of the honeycomb structure, (2) promotion of charge separation and migration, (3) enlargement of the band gap, (4) increase in production yield, and (5) decrease in energy cost. These advantages make the present preparation method for highly efficient g-C3N4 extremely appealing for large-scale applications. The active species produced from g-C3N4 under illumination were confirmed using DMPO-ESR spin-trapping, the reaction intermediate was monitored, and the reaction mechanism of photocatalytic NO oxidation by g-C3N4 was revealed. This work could provide an attractive alternative method for mass-production of highly active g-C3N4-based photocatalysts for environmental and energetic applications.

The development of catalysts that effectively activate target pollutants and promote their complete conversion is an admirable objective in the environmental photocatalysis field. In this work, graphitic carbon nitride (g-C 3 N 4 ) microtubes with tunable N-vacancy concentrations were controllably fabricated using an in situ soft-chemical method. The morphological evolution of g-C 3 N 4 , from the bulk to the porous tubular architecture, is discussed in detail with the aid of time-resolved hydrothermal experiments. We found that the NO removal ratio and apparent reaction rate constant of the g-C 3 N 4 microtubes were 1.8 and 2.6 times higher than those of pristine g-C 3 N 4 , respectively. By combining detailed experimental characterization and density functional theory calculations, the effects of N-vacancies in the g-C 3 N 4 microtubes on O 2 and NO adsorption activation, electron capture, and electronic structure were systematically investigated. These results demonstrate that surface N-vacancies act as specific sites for the adsorption activation of reactants and photoinduced electron capture, while enhancing the light-absorbing capability of g-C 3 N 4 . Moreover, the porous wall structures of the as-prepared g-C 3 N 4 microtubes facilitate the diffusion of reactants, and their tubular architectures favor the oriented transfer of charge carriers. The intermediates formed during photocatalytic NO removal processes were identified by in situ diffuse reflectance infrared Fourier transform spectroscopy, and different reaction pathways over pristine and N-deficient g-C 3 N 4 are proposed. This study provides a feasible strategy for air pollution control over g-C 3 N 4 by introducing N-vacancy and porous tubular architecture simultaneously. KEYWORDS: N-vacancy, tubular g-C 3 N 4 , porosity, photocatalytic NO x removal