Oxygen-vacancy mediated acidity and redox properties on WOx/Cu-doped CeO2 for the removal of NOx

被引:27
作者
Hao, Zhifei [1 ]
Liu, Guoquan [1 ]
Zhang, He [1 ]
Li, Yi [2 ]
Xia, Yuguo [3 ]
Zhang, Dongpeng [1 ]
Zhan, Sihui [1 ]
机构
[1] Nankai Univ, Coll Environm Sci & Engn, Tianjin Key Lab Environm Remediat & Pollut Contro, MOE Key Lab Pollut Processes & Environm Criteria, Tianjin 300350, Peoples R China
[2] Tianjin Univ, Sch Sci, Collaborat Innovat Ctr Chem Sci & Engn, Dept Chem,Tianjin Key Lab Mol Optoelect Sci, Tianjin 300072, Peoples R China
[3] Shandong Univ, Sch Chem & Chem Engn, Natl Engn Res Ctr Colloidal Mat, Jinan 250100, Peoples R China
来源
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING | 2021年 / 9卷 / 05期
基金
中国国家自然科学基金;
关键词
NOx removal; WOx/Cu-CeO2; Oxygen vacancy; Acid sites; Electronic interaction; SELECTIVE CATALYTIC-REDUCTION; MIXED-OXIDE CATALYST; ACTIVE-SITES; CO OXIDATION; NH3; PERFORMANCE; NH3-SCR; CERIA; SO2; COPPER;
D O I
10.1016/j.jece.2021.106024
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Acidity and redox properties of the catalyst are two crucial factors affecting the performance of NH3-SCR. Herein, we design a novel WOx/Cu-CeO2 oxide catalyst in which the WOx species are highly dispersed on the {111}/ {100}-terminated surface of Cu-doped CeO2 nanospheres, which exhibits great deNOx activity advantage and wide operating temperature window (200-400 degrees C, over 85% NOx conversion with a gas hourly space velocity (GHSV) of 60,000 h(-1)), as well as good sulfur resistance and N-2 selectivity. The relationship among the composition, acidity and redox properties of the WOx/Cu-CeO2 catalyst is established in the NH3-SCR reaction. The combined experimental studies and spectroscopic characterization reveal that the introduction of Cu into the lattice of CeO2 not only increases the surface Ce3+ and oxygen vacancy concentration but also provides more sites for capture and dispersion of WOx species, thus mediating and improving the Lewis and Bronsted acid sites and reducibility of catalyst. XPS and DFT calculations further demonstrate that electronic interaction between WOx and Cu-doped CeO2 is enhanced duo to the existence of interactions of short-range Ce-O-Cu and Ce-O-W. Moreover, the NH3-SCR reaction over WOx/Cu-CeO2 may follow both Langmuir-Hinshelwood and Eley-Rideal reaction pathway according to the in situ DRIFTS.
引用
收藏
页数:11
相关论文
共 49 条
[21]   Relationship between structure and performance of a novel cerium-niobium binary oxide catalyst for selective catalytic reduction of NO with NH3 [J].
Qu, Ruiyang ;
Gao, Xiang ;
Cen, Kefa ;
Li, Junhua .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 142 :290-297
[22]   Single-atom catalysts reveal the dinuclear characteristic of active sites in NO selective reduction with NH3 [J].
Qu, Weiye ;
Liu, Xiaona ;
Chen, Junxiao ;
Dong, Yangyang ;
Tang, Xingfu ;
Chen, Yaxin .
NATURE COMMUNICATIONS, 2020, 11 (01)
[23]   Ceria-based model catalysts: fundamental studies on the importance of the metal-ceria interface in CO oxidation, the water-gas shift, CO2 hydrogenation, and methane and alcohol reforming [J].
Rodriguez, Jose A. ;
Grinter, David C. ;
Liu, Zongyuan ;
Palomino, Robert M. ;
Senanayake, Sanjaya D. .
CHEMICAL SOCIETY REVIEWS, 2017, 46 (07) :1824-1841
[24]   EPR characterisation of carbon black in loose and tight contact with Al2O3 and CeO2 catalysts [J].
Saab, E. ;
Abi-Aad, E. ;
Bokova, M. N. ;
Zhilinskaya, E. A. ;
Aboukais, A. .
CARBON, 2007, 45 (03) :561-567
[25]   Oxidising CO to CO2 using ceria nanoparticles [J].
Sayle, TXT ;
Parker, SC ;
Sayle, DC .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2005, 7 (15) :2936-2941
[26]   A superior Ce-W-Ti mixed oxide catalyst for the selective catalytic reduction of NOx with NH3 [J].
Shan, Wenpo ;
Liu, Fudong ;
He, Hong ;
Shi, Xiaoyan ;
Zhang, Changbin .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 115 :100-106
[27]   The synergistic effects between Ce and Cu in CuyCe1-yW5Ox catalysts for enhanced NH3-SCR of NOx and SO2 tolerance [J].
Shi, Jian-Wen ;
Wang, Yao ;
Duan, Ruibin ;
Gao, Chen ;
Wang, Baorui ;
He, Chi ;
Niu, Chunming .
CATALYSIS SCIENCE & TECHNOLOGY, 2019, 9 (03) :718-730
[28]   Differentiating Surface Ce Species among CeO2 Facets by Solid-State NMR for Catalytic Correlation [J].
Tan, Zicong ;
Li, Guangchao ;
Chou, Hung-Lung ;
Li, Yiyang ;
Yi, Xianfeng ;
Mahadi, Abdul Hanif ;
Zheng, Anmin ;
Tsang, Shik Chi Edman ;
Peng, Yung-Kang .
ACS CATALYSIS, 2020, 10 (07) :4003-4011
[29]   Ceria-based catalysts for low-temperature selective catalytic reduction of NO with NH3 [J].
Tang, Changjin ;
Zhang, Hongliang ;
Dong, Lin .
CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (05) :1248-1264
[30]   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