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题名: The mechanism of ammonium bisulfate formation and decomposition over V/WTi catalysts for NH3-selective catalytic reduction at various temperatures
作者: Li, Chenxu1;  Shen, Meiqing1, 2, 3;  Yu, Tie1, 4;  Wang, Jianqiang1;  Wang, Jun1;  Zhai, Yanping5
刊名: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
发表日期: 2017-06-21
DOI: 10.1039/c7cp02324c
卷: 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
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.
关键词[WOS]: NITRIC-OXIDE ;  V2O5-WO3/TIO2 CATALYSTS ;  V2O5/TIO2 CATALYST ;  CE/TIO2 CATALYST ;  SULFUR-DIOXIDE ;  NOX REDUCTION ;  NH3 ;  SO2 ;  TIO2 ;  OXIDATION
语种: 英语
WOS记录号: WOS:000403561200034
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152091
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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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

Recommended Citation:
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.
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