Photocatalytic oxidation of aqueous ammonia by Ag2O/TiO2 (P25): New insights into selectivity and contributions of different oxidative species

被引:27
|
作者
Ren, Hai-Tao [1 ]
Liang, Yu [1 ]
Han, Xu [2 ]
Liu, Yong [3 ]
Wu, Song-Hai [2 ]
Bai, He [4 ]
Jia, Shao-Yi [2 ]
机构
[1] Tiangong Univ, Sch Text Sci & Engn, State Key Lab Separat Membranes & Membrane Proc, Tianjin, Peoples R China
[2] Tianjin Univ, Sch Chem Engn & Technol, Tianjin, Peoples R China
[3] Tianjin Univ Technol, Sch Chem & Chem Engn, Tianjin, Peoples R China
[4] China Offshore Environm Serv Ltd, Tianjin, Peoples R China
基金
中国国家自然科学基金;
关键词
Ag2O; P25; Photocatalysis; Ammonia oxidation; Reactive oxidative species; VISIBLE-LIGHT; NITROGEN; REMOVAL; TIO2; NANOPARTICLES; DEGRADATION; DEPOSITION; REDUCTION; CATALYST; HYDROGEN;
D O I
10.1016/j.apsusc.2019.144433
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
Oxidation of ammonia (NH4+/NH3) from wastewater is a challenge due to its high stability and solubility in aqueous environments. A simple Ag2O/TiO2 (P25) catalyst was synthesized and used for photocatalytic oxidation of aqueous NH4+/NH3. Under UV illumination, the oxidation rate of NH4+/NH3 by 1% Ag2O/P25 is increased with increasing pHs, with a rate constant of 0.383 h(-1) at pH 11.8. (OH)-O-./h(+) are important oxidative species that dominate the oxidation of NH4+/NH3. The respective contributions of Pathway I (the h(+) mediated process) and Pathway II (the e(-) mediated process) are 66.2% and 33.8% to the oxidation of NH4+/NH3. Oxidation selectivity toward N-2 is more favorable under high concentrations of NH4+/NH3 and low concentrations of Ag2O/P25. The improved separation of e(-)-h(+) pairs on Ag2O/P25 facilitates generation of (OH)-O-. and h(+), thus triggering the high conversion yield of NH4+/NH3. XPS analysis further suggests that Ag(I), instead of the photogenerated Ag(0), plays the predominant role in photocatalytic oxidation of NH4+/NH3. This work enriches our understanding on the photooxidation mechanism of NH4+/NH3 by Ag2O/P25.
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页数:10
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