Journal
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
Volume 305, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.121018
Keywords
Hydrothermal-transverse thermal stripping; Cl/S co-doping; Carbon nitride; Photocatalytic denitrification; Photogenerated electrons
Funding
- CNPC safety and environmental protection key technology research and promotion project [2017D-4613]
- Sub project of National Science and Technology major project [2016ZX05040-003]
- China University of Petroleum (East China) Graduate Innovative Engineering Project [YCX2020039]
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In this study, metal-free polymeric catalysts were used for the photocatalytic denitrification (PCDN) reaction under visible light. A hydrothermal-transverse thermal stripping method was developed to prepare Cl/S co-doped metal-free carbon nitride nanotubes as efficient photocatalysts. The results showed that the PCDN performance of Cl/S-TCN was 19 times higher than that of carbon nitride under visible light, and the PCDN reaction was dominated by photo-generated electrons (e(-)) in acidic solutions.
In this work, we first applied metal-free polymeric catalysts to drive the photocatalytic denitrification (PCDN) reaction under visible light. We developed a hydrothermal-transverse thermal stripping method to prepare Cl/S co-doped metal-free carbon nitride nanotubes as the photocatalysts (Cl/S-TCN). With larger specific surface area, stronger light response intensity and wider light absorption range, the PCDN performance of Cl/S-TCN was 19 times higher than that of carbon nitride (GCN, obtained by direct calcination of melamine) under visible light. In hole scavenger experiments, the PCDN reaction was dominated by photo-generated electrons (e(-)) over Cl/S-TCN in acidic solutions. DFT calculations showed that surface Cl and S dopants preferentially adsorbed the O atoms in NO3- and delivered photoinduced-e(-) to N atoms through O atoms, ultimately breaking the N-O bond. Such reaction pathway was rarely reported in previous studies. Hence, this work contributes to the first insight into PCDN catalyzed by atomically modified metal-free photocatalyst under visible light.
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