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Porous Mn doped g-C_3N_4 photocatalysts for enhanced synergetic degradation under visible-light illumination

Weina Shi  Chenyu Song  Xuezhe Li  Yaxin Li  Gairong Chen  
【摘要】:Photocatalytic degradation by semiconductors is an ideal way to solve the environmental problem.Among diversified photocatalysts,graphitic carbon nitrides(g-C_3N_4),as an ideal visible-light-driven semiconductor,exhibits excellent photocatalytic performance and photo-stability.Nonetheless,the fast electron-hole recombination limits its photocatalytic activity.The combined effect of the ion doping and nano-structuralization of g-C_3N_4 semiconductor would be of significance to promote the photocatalytic performance.Here,the porous Mn doped g-C_3N_4photocatalyst was synthesized by the calcination-refluxing method.The as-prepared g-C_3N_4 exhibits the high activity of photocatalytic degradation under visible light irradiation(400 nm)in the mixed system of Cr(VI)and organic pollutants.Especially,the photocatalytic activity of Cr(VI)reduction was increased from 9.5%to 76.5%,while that of Rhodamine B(RhB)degradation was enhanced from 15.3%to 88.9%after 60 min irradiation.The porous Mn doped g-C_3N_4 still keeps the high degradation efficiency of mixed pollutants in the 7th running.Based on the computational modeling,the Mn doping and carboxyl modification affect the atomic arrangement and molecular orbital distribution of the g-C_3N_4 semiconductor,leading to the enhancement of photo-induced carrier separation.Additionally,the active oxygen species and intermediates in the photoreaction process were discovered by ESR measurement and UV-Vis test.The Rh B degradation in synergistic photocatalysis not only inhibits the reverse reaction of Cr(VI)reduction,but also validly supply the photogenerated electrons by the photosensitization effect.This work may be useful for rationally designing photocatalysts and providing illuminating insights into the photocatalytic mechanism.

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