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Rare-earth ion exchanged cu-ssz-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in nh3-scr of nox

文献类型:期刊论文

作者Zhao, Zhenchao1; Yu, Rui1; Shi, Chuan1; Gies, Hermann2; Xiao, Feng-Shou3; De Vos, Dirk4; Yokoi, Toshiyuki5; Bao, Xinhe6; Kolb, Ute7; McGuire, Robert8
刊名Catalysis science & technology
出版日期2019-01-07
卷号9期号:1页码:241-251
ISSN号2044-4753
DOI10.1039/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.
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
WOS类目Chemistry, Physical
语种英语
WOS记录号WOS:000454918600021
出版者ROYAL SOC CHEMISTRY
URI标识http://www.irgrid.ac.cn/handle/1471x/2372943
专题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
Zhao, Zhenchao,Yu, Rui,Shi, Chuan,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 Zhao, Zhenchao.,Yu, Rui.,Shi, Chuan.,Gies, Hermann.,Xiao, Feng-Shou.,...&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 Zhao, Zhenchao,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.

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来源:大连化学物理研究所

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