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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
Source PublicationPHYSICAL CHEMISTRY CHEMICAL PHYSICS
2017-06-21
DOI10.1039/c7cp02324c
Volume19Pages:15194-15206
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS Research AreaChemistry ; Physics
WOS KeywordNITRIC-OXIDE ; V2O5-WO3/TIO2 CATALYSTS ; V2O5/TIO2 CATALYST ; CE/TIO2 CATALYST ; SULFUR-DIOXIDE ; NOX REDUCTION ; NH3 ; SO2 ; TIO2 ; OXIDATION
AbstractIn 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.
Language英语
WOS IDWOS:000403561200034
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/152091
Collection中国科学院大连化学物理研究所
Affiliation1.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
Recommended Citation
GB/T 7714
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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