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Studies of the Active Sites for Methane Dehydroaromatization Using Ultrahigh-Field Solid-State Mo-95 NMR Spectroscopy
Hu, Jian Zhi1; Kwak, Ja Hun1; Wang, Yong1; Peden, Charles H. F.1; Zheng, Heng2,3; Ma, Ding; Bao, Xinhe2
刊名JOURNAL OF PHYSICAL CHEMISTRY C
2009-02-19
DOI10.1021/jp8107914
113期:7页:2936-2942
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
类目[WOS]Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
研究领域[WOS]Chemistry ; Science & Technology - Other Topics ; Materials Science
关键词[WOS]BRONSTED ACID SITES ; ANGLE-SPINNING NMR ; MAS NMR ; HYDRODESULFURIZATION CATALYSTS ; DEHYDRO-AROMATIZATION ; ZEOLITE CATALYSTS ; MO ; NAPHTHALENE ; QUADRUPOLE ; CONVERSION
英文摘要In this contribution, we show that the spin-lattice relaxation time, T-1, corresponding to zeolite exchanged molybdenum species in Mo/HZSM-5 catalysts is about 2 orders of magnitude shorter than the corresponding T, for small MoO3 crystallites. Such a difference is utilized to differentiate the exchanged Mo species from MoO3 agglomerates in Mo/H7-SM-5 catalysts and to readily estimate their relative fractions present in catalysts with varying Mo loading. A good linear correlation between the amount of zeolite exchanged species and the aromatics formation rate during catalytic methane dehydroaromatization is obtained. This result significantly strengthens our prior conclusion that the exchanged Mo species are the active centers for this reaction on Mo/HZSM-5 catalysts (J. Am. Chem. Soc. 2008, 130, 3722-3723). Of more general interest for Mo-exchanged zeolites, the results may provide useful data for analyzing the binding of exchanged Mo species in zeolite cages. In particular, the NMR data suggest a possible saturation loading for the exchanged Mo species at a Mo/Al ratio of approximately 0.5 for the ZSM-5 zeolite used in this study (Si/Al = 25). Furthermore, for polycrystalline MoO3 powder samples, the parameters related to the electric field gradient (EFG) tensor, the chemical shift anisotropy (CSA), and the three Euler angles required to align the CSA principal axis system with the quadrupolar principal axis system are determined by analyzing both the magic angle spinning (MAS) and. static Mo-95 spectra. The new results obtained from this study on MoO3 powders should help to clarify some of the contradictions in prior literature reports of studies of Mo-containing solids by Mo-95 NMR.
语种英语
WOS记录号WOS:000263299600040
引用统计
被引频次:19[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/141247
专题中国科学院大连化学物理研究所
作者单位1.Pacific NW Natl Lab, Inst Interfacial Catalysis, Richland, WA 99352 USA
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.SW Res & Design Inst Chem Ind Chengdu, Chengdu, Peoples R China
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Hu, Jian Zhi,Kwak, Ja Hun,Wang, Yong,et al. Studies of the Active Sites for Methane Dehydroaromatization Using Ultrahigh-Field Solid-State Mo-95 NMR Spectroscopy[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2009,113(7):2936-2942.
APA Hu, Jian Zhi.,Kwak, Ja Hun.,Wang, Yong.,Peden, Charles H. F..,Zheng, Heng.,...&Bao, Xinhe.(2009).Studies of the Active Sites for Methane Dehydroaromatization Using Ultrahigh-Field Solid-State Mo-95 NMR Spectroscopy.JOURNAL OF PHYSICAL CHEMISTRY C,113(7),2936-2942.
MLA Hu, Jian Zhi,et al."Studies of the Active Sites for Methane Dehydroaromatization Using Ultrahigh-Field Solid-State Mo-95 NMR Spectroscopy".JOURNAL OF PHYSICAL CHEMISTRY C 113.7(2009):2936-2942.
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