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
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页数:11
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共 49 条
[1]   Synergistic effect between copper and cerium on the performance of Cux-Ce0.5-x-Zr0.5 (x=0.1-0.5) oxides catalysts for selective catalytic reduction of NO with ammonia [J].
Ali, Sher ;
Chen, Liqiang ;
Yuan, Fulong ;
Li, Rui ;
Zhang, Tianrui ;
Bakhtiar, Syed ul Hasnain ;
Leng, Xuesong ;
Niu, Xiaoyu ;
Zhu, Yujun .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 210 :223-234
[2]   Improvement of Activity and SO2 Tolerance of Sn-Modified MnOx-CeO2 Catalysts for NH3-SCR at Low Temperatures [J].
Chang, Huazhen ;
Chen, Xiaoyin ;
Li, Junhua ;
Ma, Lei ;
Wang, Chizhong ;
Liu, Caixia ;
Schwank, Johannes W. ;
Hao, Jiming .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (10) :5294-5301
[3]   Charge-redistribution-induced new active sites on (001) facets of α-Mn2O3 for significantly enhanced selective catalytic reduction of NOx by NH3 [J].
Fan, Zhaoyang ;
Wang, Zhenyu ;
Shi, Jian-Wen ;
Gao, Chen ;
Gao, Ge ;
Wang, Baorui ;
Wang, Yao ;
Chen, Xin ;
He, Chi ;
Niu, Chunming .
JOURNAL OF CATALYSIS, 2019, 370 :30-37
[4]   Initial Reduction of CO2 on Pd-, Ru-, and Cu-Doped CeO2(111) Surfaces: Effects of Surface Modification on Catalytic Activity and Selectivity [J].
Guo, Chen ;
Wei, Shuxian ;
Zhou, Sainan ;
Zhang, Tian ;
Wang, Zhaojie ;
Ng, Siu-Pang ;
Lu, Xiaoqing ;
Wu, Chi-Man Lawrence ;
Guo, Wenyue .
ACS APPLIED MATERIALS & INTERFACES, 2017, 9 (31) :26107-26117
[5]   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
[6]   The Role of Alkali Metal in -MnO2 Catalyzed Ammonia-Selective Catalysis [J].
Hao, Zhifei ;
Shen, Zhurui ;
Li, Yi ;
Wang, Haitao ;
Zheng, Lirong ;
Wang, Ruihua ;
Liu, Guoquan ;
Zhan, Sihui .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2019, 58 (19) :6351-6356
[7]   Polymeric vanadyl species determine the low-temperature activity of V-based catalysts for the SCR of NOx with NH3 [J].
He, Guangzhi ;
Lian, Zhihua ;
Yu, Yunbo ;
Yang, Yang ;
Liu, Kuo ;
Shi, Xiaoyan ;
Yan, Zidi ;
Shan, Wenpo ;
He, Hong .
SCIENCE ADVANCES, 2018, 4 (11)
[8]   Synergistic role of acid sites in the Ce-enhanced activity of mesoporous Ce-Al-MCM-41 catalysts in alkylation reactions: FTIR and TPD-ammonia studies [J].
Kalita, Pranjal ;
Gupta, Narendra M. ;
Kumar, Rajiv .
JOURNAL OF CATALYSIS, 2007, 245 (02) :338-347
[9]   Improved NOx Reduction in the Presence of SO2 by Using Fe2O3-Promoted Halloysite-Supported CeO2-WO3 Catalysts [J].
Kang, Lin ;
Han, Lupeng ;
He, Jiebing ;
Li, Hongrui ;
Yan, Tingting ;
Chen, Guorong ;
Zhang, Jianping ;
Shi, Liyi ;
Zhang, Dengsong .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2019, 53 (02) :938-945
[10]   Ce-Ti Amorphous Oxides for Selective Catalytic Reduction of NO with NH3: Confirmation of Ce-O-Ti Active Sites [J].
Li, Ping ;
Xin, Ying ;
Li, Qian ;
Wang, Zhongpeng ;
Zhang, Zhaoliang ;
Zheng, Lirong .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2012, 46 (17) :9600-9605