Tetraphenyl-porphyrin decorated anatase TiO2 catalysts for the visible-light photocatalytic oxidation of gaseous ammonia at room temperature

被引:12
作者
Gao, Fengyu [1 ,2 ]
Song, Shuang [1 ]
Tang, Xiaolong [1 ,2 ]
Yi, Honghong [1 ,2 ]
Zhao, Shunzheng [1 ,2 ]
Yu, Qingjun [1 ,2 ]
机构
[1] Univ Sci & Technol Beijing, Sch Energy & Environm Engn, Beijing 100083, Peoples R China
[2] Univ Sci & Technol Beijing, Beijing Key Lab Resource Oriented Treatment Ind P, Beijing 100083, Peoples R China
基金
国家重点研发计划; 中国博士后科学基金; 中国国家自然科学基金;
关键词
TPP/TiO2; catalyst; One-step solvothermal; Photo-catalysis mechanism; NH3; oxidation; Visible light irradiation; PHOTO-SCR; NH3; REDUCTION; CARBON; NOX; MECHANISM; NITROGEN; NANOPARTICLES; DEGRADATION; COMPOSITE;
D O I
10.1016/j.apsusc.2019.144421
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Tetraphenyl-porphyrin (1 wt% TPP) decorated anatase TiO2 catalysts were optimized by one-step solvothermal method and presented high-efficient photo-catalytic activity of ammonia oxidation under visible-light irradiation with above 98% removal efficiency at room temperature within 8 h. TPP modifiers were successfully loaded onto TiO2 surface via Ti-O-C bands determining the transfer direction of photo-excited hot charge carriers. The surface radical species including (OH)-O-center dot and O-center dot(2)- generated from H2O/-OH and surface oxygen species were fleeting and hyperactive for the photocatalytic degradation of ammonia. TPP gave an evident promotion via the stimulative reactions due to the contributions of H+ and gave VB holes (h(+)), which had strong oxidation power for the direct oxidation of -OH/H2O and adsorbed oxygen to generate (OH)-O-center dot and O-center dot(2)- radicals, being beneficial to the fundamental NH3 oxidation reaction. Furthermore, the remaining electrons were transferred to the surface of TiO2 via Ti-O-C bonds, thus promoting the transformation of Ti4+ -> TiO2-n to generate oxygen vacancy defects for the efficient oxidation of gaseous NH3 and adsorbed -NHx species during photocatalytic reaction. However, the thermodynamic stable NH4NO3 products were generated via the combination of NH4+ and -NO3 species that could exist on the catalyst surface stably, resulting in the decline of photocatalytic activity.
引用
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页数:10
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