Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx

doi:10.1039/c8cy02033g

	Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx
	Xiao, Feng-Shou 3; Zhao, Zhenchao 1; Yu, Rui 1; Shi, Chuan 1; Gies, Hermann 2; De Vos, Dirk 4; Yokoi, Toshiyuki 5; Bao, Xinhe 6; Kolb, Ute 7; McGuire, Robert 8
刊名	CATALYSIS SCIENCE & TECHNOLOGY
	2019-01-07
卷号	9 期号:1 页码:241-251
ISSN号	2044-4753
DOI	10.1039/c8cy02033g
通讯作者	Mueller, Ulrich(ulrich.mueller@basf.com) ; Zhang, Weiping(wpzhang@dlut.edu.cn)
英文摘要	The relatively low hydrothermal stability of Al-rich Cu-SSZ-13 catalysts hinders their practical application in ammonia selective catalytic reduction (NH3-SCR) reaction. Rare-earth ions were introduced into the Al-rich SSZ-13 zeolite using an organotemplate-free synthesis prior to the exchange of Cu2+ ions. Among the rare-earth ions tested (Ce, La, Sm, Y, Yb), Y shows significant enhancement of the hydrothermal stability and NH3-SCR activities after severe hydrothermal aging at 800 degrees C for 16 h when compared with Cu-SSZ-13 without Y. Cu-Y-SSZ-13 catalysts with various amounts of Y were prepared, and it is found that with increasing Y content, the low temperature NO conversions can be improved even after hydrothermal aging. SEM-EDX analysis together with two-dimensional multiple quantum magic-angle-spinning nuclear magnetic resonance (Na-23 MQ MAS NMR) confirms that the Y ions are successfully incorporated into the ion-exchange sites of the SSZ-13 zeolite. Results from Al-27 MAS, Si-29 MAS NMR, temperature-programmed desorption of ammonia (NH3-TPD) and quantitative H-1 MAS NMR indicate that Y can stabilize the framework Al and also preserve the BrOnsted acid sites in the Al-rich SSZ-13 zeolite. The hydrogen temperature programmed reduction (H-2-TPR), ultraviolet-visible-near infrared spectroscopy (UV-vis-NIR) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of nitric oxide (NO) or NH3 adsorption demonstrate that introduction of Y ions causes Cu2+ ions to preferentially occupy the 6-MR, which has high hydrothermal stability. However, too much of Y may lead to activity loss at both low and high temperatures. The optimized Al-rich Cu-Y-SSZ-13 with 2.8 wt% of copper (Cu) and 1.3 wt% of Y displays almost the same deNO(x) activities as the conventional organotemplated high silica Cu-SSZ-13 catalyst in a wide reaction temperature window of 150-650 degrees C after severe hydrothermal treatment. Rare-earth ions could be an effective additive for Cu-SSZ-13 catalysts to further improve their hydrothermal stability for practical applications.
资助项目	National Natural Science Foundation of China[2187020455] ; National Natural Science Foundation of China[21603022] ; Fundamental Research Funds for the Central Universities in China[DUT16RC(3)002] ; Fundamental Research Funds for the Central Universities in China[DUT17TD04] ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics[N-16-08] ; Program for Liaoning Innovative Research Team in University[LT2016001] ; INCOE (International Network of Centers of Excellence) project
WOS关键词	SELECTIVE CATALYTIC-REDUCTION ; SOLID-STATE NMR ; MAS NMR ; CU/SSZ-13 ; NH3 ; SITES ; FRAMEWORK ; COMPLEX ; ALUMINA ; CATION
WOS研究方向	Chemistry
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000454918600021
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities in China ; Fundamental Research Funds for the Central Universities in China ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Program for Liaoning Innovative Research Team in University ; Program for Liaoning Innovative Research Team in University ; INCOE (International Network of Centers of Excellence) project ; INCOE (International Network of Centers of Excellence) project ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities in China ; Fundamental Research Funds for the Central Universities in China ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Program for Liaoning Innovative Research Team in University ; Program for Liaoning Innovative Research Team in University ; INCOE (International Network of Centers of Excellence) project ; INCOE (International Network of Centers of Excellence) project ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities in China ; Fundamental Research Funds for the Central Universities in China ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Program for Liaoning Innovative Research Team in University ; Program for Liaoning Innovative Research Team in University ; INCOE (International Network of Centers of Excellence) project ; INCOE (International Network of Centers of Excellence) project ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities in China ; Fundamental Research Funds for the Central Universities in China ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Open Project Funds of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics ; Program for Liaoning Innovative Research Team in University ; Program for Liaoning Innovative Research Team in University ; INCOE (International Network of Centers of Excellence) project ; INCOE (International Network of Centers of Excellence) project
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/166360]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Mueller, Ulrich; Zhang, Weiping
作者单位	1.Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China 2.Ruhr Univ Bochum, Inst Geol Mineral & Geophys, Bochum, Germany 3.Zhejiang Univ, Dept Chem, Hangzhou 310028, Zhejiang, Peoples R China 4.Katholieke Univ Leuven, Ctr Surface Chem & Catalysis, Leuven, Belgium 5.Tokyo Inst Technol, Chem Resources Lab, Yokohama, Kanagawa, Japan 6.Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 7.Johannes Gutenberg Univ Mainz, Inst Phys Chem, D-55128 Mainz, Germany 8.BASF SE, Proc Res & Chem Engn, D-67056 Ludwigshafen, Germany
推荐引用方式 GB/T 7714	Xiao, Feng-Shou,Zhao, Zhenchao,Yu, Rui,et al. Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx[J]. CATALYSIS SCIENCE & TECHNOLOGY,2019,9(1):241-251.
APA	Xiao, Feng-Shou.,Zhao, Zhenchao.,Yu, Rui.,Shi, Chuan.,Gies, Hermann.,...&Zhang, Weiping.(2019).Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx.CATALYSIS SCIENCE & TECHNOLOGY,9(1),241-251.
MLA	Xiao, Feng-Shou,et al."Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx".CATALYSIS SCIENCE & TECHNOLOGY 9.1(2019):241-251.