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The mechanism of ammonium bisulfate formation and decomposition over V/WTi catalysts for NH3-selective catalytic reduction at various temperatures
Li, Chenxu1; Shen, Meiqing1,2,3; Yu, Tie1,4; Wang, Jianqiang1; Wang, Jun1; Zhai, Yanping5
刊名PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2017-06-21
DOI10.1039/c7cp02324c
19页:15194-15206
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
研究领域[WOS]Chemistry ; Physics
关键词[WOS]NITRIC-OXIDE ; V2O5-WO3/TIO2 CATALYSTS ; V2O5/TIO2 CATALYST ; CE/TIO2 CATALYST ; SULFUR-DIOXIDE ; NOX REDUCTION ; NH3 ; SO2 ; TIO2 ; OXIDATION
英文摘要In this study, the mechanism of ammonium bisulfate (ABS) formation and decomposition over V/WTi for the NH3-selective catalytic reduction (SCR) at various temperatures was deeply investigated. Bridged bidentate, chelating bidentate, and tridentate sulfates bound to TiO2 were formed as dominant intermediates at 200, 250, and 300 C-omicron, respectively. These sulfates reacted with affinitive ammonium species to form ammonium (bi)sulfate species and also covered the active sites and embedded the VOSO4 intermediates, which resulted in an inferior intrinsic NH3-SCR conversion rate at 200 C-omicron and 250 C-omicron. At 300 C-omicron, trace amounts of ABS on TiO2 presented no influence on the NH3-SCR performance. The electrons deviating towards sulfates through the bond between ABS and metal oxides (WO3 and TiO2) weakened the stability of ABS and lowered its decomposition temperature, whereas the vanadia species played the opposite role due to the sulfur species existing in an electron saturation state with the formation of the VOSO4 intermediate. The presence of NO + O-2 could break the bonds inside ABS and it could react with the ammonium species originating from ABS, which pulls NH3 out of the ABS formation equilibrium and accelerates its decomposition and competitively inhibits its formation. Correspondingly, the faster NH3-SCR conversion rate and higher N-2 selectivity improve the ABS poisoning resistance of the V/WTi catalyst at low temperatures.
语种英语
WOS记录号WOS:000403561200034
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/152091
专题中国科学院大连化学物理研究所
作者单位1.Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, State Educ Minist, Tianjin 300072, Peoples R China
2.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
3.Tianjin Univ, State Key Lab Engines, Tianjin 300072, Peoples R China
4.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
5.China Huadian Sci & Technol Inst, Beijing 100070, Peoples R China
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Li, Chenxu,Shen, Meiqing,Yu, Tie,et al. The mechanism of ammonium bisulfate formation and decomposition over V/WTi catalysts for NH3-selective catalytic reduction at various temperatures[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2017,19:15194-15206.
APA Li, Chenxu,Shen, Meiqing,Yu, Tie,Wang, Jianqiang,Wang, Jun,&Zhai, Yanping.(2017).The mechanism of ammonium bisulfate formation and decomposition over V/WTi catalysts for NH3-selective catalytic reduction at various temperatures.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,19,15194-15206.
MLA Li, Chenxu,et al."The mechanism of ammonium bisulfate formation and decomposition over V/WTi catalysts for NH3-selective catalytic reduction at various temperatures".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 19(2017):15194-15206.
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