New Insights on Competitive Adsorption of NO/SO2 on TiO2 Anatase for Photocatalytic NO Oxidation

被引:31
|
作者
Chen, Zhen [1 ,2 ]
Yin, Haibo [1 ]
Wang, Chizhong [1 ]
Wang, Rong [2 ]
Peng, Yue [1 ]
You, Changfu [2 ]
Li, Junhua [1 ]
机构
[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
[2] Tsinghua Univ, Dept Energy & Power Engn, Key Lab Thermal Sci & Power Engn, Minist Educ, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
photocatalytic NO oxidation; competitive adsorption; SO2; catalyst deactivation; DFT; IN-SITU FTIR; FLUE-GAS; BI METAL; SO2; REMOVAL; MECHANISM; DESULFURIZATION; PERFORMANCE; OXIDE;
D O I
10.1021/acs.est.1c01749
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Here, we investigate competitive adsorption and photocatalytic reaction over TiO2@SiO2: NO conversion efficiency decreases by 29.1%, and the adsorption capacity decreases from 0.125 to 0.095 mmol/g due to the influence of SO2. According to identification and comparative analysis of the IR signal, SO2 has little effect on the NO conversion route and intermediates (adsorbed NO -> nitrite -> nitrate), but accelerates the deactivation of catalysts. The electronic interaction scheme from density functional theory (DFT) confirms that surface hydroxyls create an unsaturated coordination of neighboring Ti or O atoms, which is favorable for NO/SO2 adsorption on anatase (101). In addition, the lone pair electrons of N or S atoms prefer to be delocalized and form covalent bonds with active surface-O on the (101) facet with terminal hydroxyls. However, preadsorbed SO2 could offset the increase of hydroxyls and strongly inhibit NO adsorption, which is consistent with the result performance evaluation. A possible reaction mechanism characterized by oxygen vacancies and center dot O-2(-) is proposed, while the essential reason of catalyst deactivation and regeneration is theoretically analyzed based on the experimental and DFT calculation.
引用
收藏
页码:9285 / 9292
页数:8
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