Effect of oxygen vacancies on ceria catalyst for selective catalytic reduction of NO with NH3

被引:93
作者
Zhang, Bolin [1 ,2 ]
Zhang, Shengen [1 ]
Liu, Bo [1 ]
机构
[1] Univ Sci & Technol Beijing, Inst Adv Mat & Technol, Beijing 100083, Peoples R China
[2] Jiangsu LongkingCotech Co Ltd, Yancheng 224000, Peoples R China
基金
中国国家自然科学基金;
关键词
Oxygen vacancy; Ceria; Surface adsorbed oxygen; Selective catalytic reduction; Redox; MIXED-OXIDE CATALYST; SURFACE-CHEMISTRY; RAMAN-SCATTERING; LATTICE-DEFECTS; SO2; TOLERANCE; CEO2; PERFORMANCE; MECHANISM; SCR; NANOPOWDERS;
D O I
10.1016/j.apsusc.2020.147068
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 effect of oxygen vacancies on ceria catalyst for selective catalytic reduction with NH3 (NH3-SCR) of NO was investigated. The characterizations indicated that CeO2-Ar catalyst calcined in Ar atmosphere possessed more oxygen vacancies than CeO2 catalyst calcined in ambient air. XPS results showed that the surface oxygen contents of CeO2 and CeO2-Ar catalysts were 70.2 and 67.9% respectively, indicative of the loss of surface oxygen and existence of oxygen vacancies on CeO2-Ar catalyst. The H-2-TPR and O-2-TPO experiments suggested that the presence of abundant oxygen vacancies improved the redox behavior, providing CeO2-Ar catalyst a superior ability to oxygen uptake and release. Furthermore, the adsorption capacity for NH3 and NO of CeO2-Ar catalyst was enhanced by oxygen vacancies. As a result, CeO2-Ar catalyst showed a quite higher NO conversion (> 90% above 260 degrees C) than CeO2 catalyst at 120 - 400 degrees C. The proposed mechanism suggested that the oxygen vacancies accelerated the acidity cycle and redox cycle during NH3-SCR reaction. Under the action of surface adsorbed oxygen on oxygen vacancies, the adsorption and activation of NH3 and NO were promoted and the restore of Ce4+ from Ce3+ was facilitated, which were responsible for the enhancement of catalytic performance of CeO2-Ar catalyst.
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页数:9
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共 65 条
[1]   The State of the Art in Selective Catalytic Reduction of NOx by Ammonia Using Metal-Exchanged Zeolite Catalysts [J].
Brandenberger, Sandro ;
Kroecher, Oliver ;
Tissler, Arno ;
Althoff, Roderik .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2008, 50 (04) :492-531
[2]   Gravity-Driven Multiple Collision-Enhanced Catalytic Soot Combustion over a Space-Open Array Catalyst Consisting of Ultrathin Ceria Nanobelts [J].
Cao, Chunmei ;
Zhang, Yuxia ;
Liu, Dongsheng ;
Meng, Ming .
SMALL, 2015, 11 (30) :3659-3664
[3]   Characterization of Nb-Containing MnOx-CeO2 Catalyst for Low-Temperature Selective Catalytic Reduction of NO with NH3 [J].
Casapu, Maria ;
Kroecher, Oliver ;
Mehring, Max ;
Nachtegaal, Maarten ;
Borca, Camelia ;
Harfouche, Messaoud ;
Grolimund, Daniel .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (21) :9791-9801
[4]   Comparison of preparation methods for ceria catalyst and the effect of surface and bulk sulfates on its activity toward NH3-SCR [J].
Chang, Huazhen ;
Ma, Lei ;
Yang, Shijian ;
Li, Junhua ;
Chen, Liang ;
Wang, Wei ;
Hao, Jiming .
JOURNAL OF HAZARDOUS MATERIALS, 2013, 262 :782-788
[5]   Review on the latest developments in modified vanadium-titanium-based SCR catalysts [J].
Chen, Chuanmin ;
Cao, Yue ;
Liu, Songtao ;
Chen, Jianmeng ;
Jia, Wenbo .
CHINESE JOURNAL OF CATALYSIS, 2018, 39 (08) :1347-1365
[6]   Design of a hierarchical Fe-ZSM-5@CeO2 catalyst and the enhanced performances for the selective catalytic reduction of NO with NH3 [J].
Chen, Liang ;
Wang, Xiaoxiang ;
Cong, Qiliang ;
Ma, Heyao ;
Li, Sujing ;
Li, Wei .
CHEMICAL ENGINEERING JOURNAL, 2019, 369 :957-967
[7]   Promotional Effect of Ce-doped V2O5-WO3/TiO2 with Low Vanadium Loadings for Selective Catalytic Reduction of NOx by NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (50) :21177-21184
[8]   Ce3+ and oxygen vacancy mediated tuning of structural and optical properties of CeO2 nanoparticles [J].
Choudhury, Biswajit ;
Choudhury, Amarjyoti .
MATERIALS CHEMISTRY AND PHYSICS, 2012, 131 (03) :666-671
[9]   Gd-modified MnOx for the selective catalytic reduction of NO by NH3: The promoting effect of Gd on the catalytic performance and sulfur resistance [J].
Fan, Zhaoyang ;
Shi, Jian-Wen ;
Gao, Chen ;
Gao, Ge ;
Wang, Baorui ;
Wang, Yao ;
He, Chi ;
Niu, Chunming .
CHEMICAL ENGINEERING JOURNAL, 2018, 348 :820-830
[10]   Selective Catalytic Reduction of NOx with NH3 by Using Novel Catalysts: State of the Art and Future Prospects [J].
Han, Lupeng ;
Cai, Sixiang ;
Gao, Min ;
Hasegawa, Jun-ya ;
Wang, Penglu ;
Zhang, Jianping ;
Shi, Liyi ;
Zhang, Dengsong .
CHEMICAL REVIEWS, 2019, 119 (19) :10916-10976