Acidity of mesoporous MoOx/ZrO2 and WOx/ZrO2 materials: A combined solid-state NMR and theoretical calculation study

CORC > 武汉物理与数学研究所 > 中国科学院武汉物理与数学研究所 > 2011年以前论文发表（包括2011年）

	Acidity of mesoporous MoOx/ZrO2 and WOx/ZrO2 materials: A combined solid-state NMR and theoretical calculation study
	Xu, J ; Zheng, AM ; Yang, J ; Su, YC ; Wang, JQ ; Zeng, DL ; Zhang, MJ ; Ye, CH ; Deng, F
刊名	JOURNAL OF PHYSICAL CHEMISTRY B
	2006-06-08
卷号	110 期号:22 页码:10662-10671
英文摘要	The acidity of mesoporous MoOx/ZrO2 and WOx/ZrO2 materials was studied in detail by multinuclear solid-state NMR techniques as well as DFT quantum chemical calculations. The H-1 MAS NMR experiments clearly revealed the presence of two different types of strong Brlnsted acid sites on both MoOx/ZrO2 and WOx/ZrO2 mesoporous materials, which were able to prontonate adsorbed pyrine-d(5) (resulting in H-1 NMR signals at chemical shifts in the range 16-19 ppm) as well as adsorbed trimethylphosphine ( giving rise to P-31 NMR signal at ca. 0 ppm). The C-13 NMR of adsorbed 2-C-13-acetone indicated that the average Brlnsted acid strength of the two mesoporous materials was stronger than that of zeolite HZSM-5 but still weaker than that of 100% H2SO4, which was in good agreement with theoretical predictions. The quantum chemical calculations revealed the detailed structures of the two distinct types of Brlnsted acid sites formed on the mesoporous MoOx/ZrO2 and WOx/ZrO2. The existence of both monomer and oligomer Mo ( or W) species containing a Mo-OH-Zr ( or W-OH-Zr) bridging OH group was confirmed with the former having an acid strength close to zeolite HZSM-5, with the latter having an acid strength similar to sulfated zirconia. On the basis of our NMR experimental and theoretical calculation results, a possible mechanism was proposed for the formation of acid sites on these mesoporous materials.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Physical
研究领域[WOS]	Chemistry
关键词[WOS]	PROBE MOLECULE TRIMETHYLPHOSPHINE ; TUNGSTATED ZIRCONIA CATALYST ; DENSITY-FUNCTIONAL THEORY ; DOUBLE-RESONANCE NMR ; C-13 CHEMICAL-SHIFT ; IN-SITU NMR ; MAGNETIC-RESONANCE ; RAMAN-SPECTROSCOPY ; SULFATED ZIRCONIA ; ALUMINUM-CHLORIDE
收录类别	SCI
语种	英语
WOS记录号	WOS:000237954000012
公开日期	2015-07-28
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/4785]
专题	武汉物理与数学研究所_2011年以前论文发表（包括2011年）
作者单位	1.Wuhan Univ Sci & Technol, Dept Chem, Wuhan 430081, Peoples R China 2.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China
推荐引用方式 GB/T 7714	Xu, J,Zheng, AM,Yang, J,et al. Acidity of mesoporous MoOx/ZrO2 and WOx/ZrO2 materials: A combined solid-state NMR and theoretical calculation study[J]. JOURNAL OF PHYSICAL CHEMISTRY B,2006,110(22):10662-10671.
APA	Xu, J.,Zheng, AM.,Yang, J.,Su, YC.,Wang, JQ.,...&Deng, F.(2006).Acidity of mesoporous MoOx/ZrO2 and WOx/ZrO2 materials: A combined solid-state NMR and theoretical calculation study.JOURNAL OF PHYSICAL CHEMISTRY B,110(22),10662-10671.
MLA	Xu, J,et al."Acidity of mesoporous MoOx/ZrO2 and WOx/ZrO2 materials: A combined solid-state NMR and theoretical calculation study".JOURNAL OF PHYSICAL CHEMISTRY B 110.22(2006):10662-10671.