Unveiling the Remarkable Arsenic Resistance Origin of Alumina Promoted Cerium-Tungsten Catalysts for NH3-SCR

被引:57
作者
Jiang, Si [1 ]
Li, Teng [2 ]
Zheng, JiKai [1 ]
Zhang, Hao [1 ]
Li, Xiang [1 ]
Zhu, Tianle [1 ]
机构
[1] Beihang Univ, Sch Space & Environm, Beijing 100191, Peoples R China
[2] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
NH3-SCR; CeO2-WO3-Al2O3; arsenic resistance; Lewis acid sites; oxygen vacancies;
D O I
10.1021/acs.est.0c05152
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The deactivation of selective catalytic reduction (SCR) catalysts by arsenic is a serious problem for NH3-SCR. However, it is tough to design catalysts with good resistance to arsenic compared to other poisons such as alkali metal, SO2, etc., because As not only deteriorates surface acidity but also redox property, causing excessive N2O generation. A novel CeO2-WO3-Al2O3 catalyst is developed with excellent arsenic resistance in this study, which presents only less than 10% activity loss compared to nearly 40% loss for CeO2-WO3 with same arsenic loading (As: 2.1 wt %). Moreover, a significant negative impact on the N2O generation for poisoning catalysts from 26.7 to 7.5 ppm has also been found. The characterization results demonstrated that the interaction between cerium and arsenic lead to Lewis acid sites and oxygen vacancies loss as well as unexpected oxidation sites formation. However, the introduction of Al weakens the deactivation effect by replacing cerium to interact with arsenic. Three aspects are proposed for obtaining excellent arsenic-resistant performance: (1) the protection of Lewis acid sites, (2) release of oxygen vacancies from As restriction, and (3) confinement of As5+ oxidizing capacity. This study may provide an effective strategy to design and develop novel virtuous antipoisoning catalysts.
引用
收藏
页码:14740 / 14749
页数:10
相关论文
共 63 条
[51]   Modeling arsenic partitioning in coal-fired power plants [J].
Senior, Constance L. ;
Lignell, David O. ;
Sarofim, Adel F. ;
Mehta, Arun .
COMBUSTION AND FLAME, 2006, 147 (03) :209-221
[52]   Novel cerium-tungsten mixed oxide catalyst for the selective catalytic reduction of NOx with NH3 [J].
Shan, Wenpo ;
Liu, Fudong ;
He, Hong ;
Shi, Xiaoyan ;
Zhang, Changbin .
CHEMICAL COMMUNICATIONS, 2011, 47 (28) :8046-8048
[53]   A quantum chemical study of nitric oxide reduction by ammonia (SCR reaction) on V2O5 catalyst surface [J].
Soyer, Sezen ;
Uzun, Alper ;
Senkan, Selim ;
Onal, Isik .
CATALYSIS TODAY, 2006, 118 (3-4) :268-278
[54]   MECHANISM OF THE SELECTIVE CATALYTIC REDUCTION OF NITRIC-OXIDE BY AMMONIA ELUCIDATED BY IN-SITU ONLINE FOURIER-TRANSFORM INFRARED-SPECTROSCOPY [J].
TOPSOE, NY .
SCIENCE, 1994, 265 (5176) :1217-1219
[55]   Raman spectroscopic characterization of tellurite glasses containing heavy metal oxides [J].
Upender, G. ;
Sathe, Vasant G. ;
Mouli, V. Chandra .
PHYSICA B-CONDENSED MATTER, 2010, 405 (05) :1269-1273
[56]   Iron doped effects on active sites formation over activated carbon supported Mn-Ce oxide catalysts for low-temperature SCR of NO [J].
Yang, Jie ;
Ren, Shan ;
Zhang, Tianshi ;
Su, Zenghui ;
Long, Hongming ;
Kong, Ming ;
Yao, Lu .
CHEMICAL ENGINEERING JOURNAL, 2020, 379
[57]   Low-temperature selective catalytic reduction of N2O by CO over Fe-ZSM-5 catalysts in the presence of O2 [J].
You, Yanchen ;
Chen, Siyu ;
Li, Jiayin ;
Zeng, Jie ;
Chang, Huazhen ;
Ma, Lei ;
Li, Junhua .
JOURNAL OF HAZARDOUS MATERIALS, 2020, 383
[58]   Asymmetric Oxygen Vacancies: the Intrinsic Redox Active Sites in Metal Oxide Catalysts [J].
Yu, Kai ;
Lou, Lan-Lan ;
Liu, Shuangxi ;
Zhou, Wuzong .
ADVANCED SCIENCE, 2020, 7 (02)
[59]   A novel Ce-Ta mixed oxide catalyst for the selective catalytic reduction of NOx with NH3 [J].
Zhang, Tao ;
Qu, Ruiyang ;
Su, Wenkang ;
Li, Junhua .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 176 :338-346
[60]  
Zhang Y., 2017, ENVIRON TECHNOL, V39, P1