Insight into the Synergic Effect of Fe-SSZ-13 Zeolite and FeMnTiZrOx Catalyst with Enhanced Reactivity in NH3-SCR of NOx

被引:35
|
作者
Yu, Rui [1 ]
Zhao, Zhenchao [1 ]
Shi, Chuan [1 ]
Zhang, Weiping [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2019年 / 123卷 / 04期
基金
中国国家自然科学基金;
关键词
ORGANOTEMPLATE-FREE SYNTHESIS; HYBRID CATALYSTS; N2O DECOMPOSITION; REDUCTION SCR; SO2; TOLERANCE; SITU-DRIFTS; NH3; PERFORMANCE; MECHANISM; FE-ZSM-5;
D O I
10.1021/acs.jpcc.8b10122
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
The relatively low activity at low temperatures and poor performance at high temperatures with low N-2 selectivity are the major problems of Fe-SSZ-13 zeolite and Mn-based metal oxides for NH3 selective catalytic reduction (SCR) of NOx, respectively. Hybrid catalysts have been prepared by mechanically mixing Fe(1.6)-SSZ-13 zeolite and Fe0.2Mn0.4TiZr0.03Ox to remedy the defects of both catalysts. The optimized mass ratio of zeolite and metal oxide components in hybrid catalysts is 7:1, which shows superior NH3 SCR performances with NO conversion above 80% and N2O yield below 12 ppm at wide-temperature window ranging from 200 to 550 degrees C. NO-TPD and in situ DRIFTS studies indicate that the metal oxide component in hybrid catalyst can provide more active nitrite/nitrate species as well as more active sites for NH3 activation to promote low-temperature activity. The migration of active intermediate from NO on the metal oxide component to react with NH3 adsorbed on zeolite component may be responsible for the enhancement of low-temperature activity. Strong adsorption of NH3 on zeolite component during SCR reaction can hinder NH3 oxidation, so high NO conversions and N-2 selectivity at high temperatures are maintained for hybrid catalyst. These insightful understandings on the synergic effect may be beneficial to rational design of high-performance hybrid catalysts in NH3-SCR reaction.
引用
收藏
页码:2216 / 2227
页数:12
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