Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations

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	Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations
	Xu, Jun 1; Zheng, Anmin 1; Wang, Xiumei 1; Qi, Guodong 1; Su, Jihu 2,3; Du, Jiangfeng 2,3; Gan, Zhehong 4; Wu, Jianfeng 5; Wang, Wei 5; Deng, Feng 1
刊名	CHEMICAL SCIENCE
	2012
卷号	3 期号:10 页码:2932-2940
英文摘要	Room temperature activation of methane over a Zn modified H-ZSM-5 zeolite catalyst was investigated by solid-state NMR spectroscopy in combination with other spectroscopic methods and DFT theoretical calculations. We found for the first time that the activation of methane resulted in the preferential formation of surface methoxy intermediates at room temperature, which mediated the formation of methanol and its further conversion to hydrocarbons. Experimental and theoretical calculation results demonstrated that an oxygen-containing dizinc cluster center in an open shell was responsible for homolytic cleavage of the C-H bond of methane at room temperature, leading to the formation of methyl radicals. The zeolite matrix readily trapped the methyl radicals by forming the surface methoxy intermediates for further selective conversion. In parallel to the homolytic cleavage pathway, heterolytic dissociation of methane was also observed on isolated Zn2+ ions at room temperature, which gives rise to zinc methyl species.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Multidisciplinary
研究领域[WOS]	Chemistry
关键词[WOS]	SURFACE METHOXY GROUPS ; IN-SITU ; ZSM-5 ZEOLITE ; DISSOCIATIVE ADSORPTION ; PROPANE AROMATIZATION ; LIGHT PARAFFINS ; ACTIVE-SITE ; MFI ZEOLITE ; HY ZEOLITE ; OXIDATION
收录类别	SCI
语种	英语
WOS记录号	WOS:000308094100004
公开日期	2015-07-14
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/1667]
专题	武汉物理与数学研究所_磁共振应用研究部
作者单位	1.Chinese Acad Sci, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Inst Phys & Math, Wuhan 430071, Peoples R China 2.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China 3.Univ Sci & Technol China, Dept Modern Phys, Hefei 230026, Peoples R China 4.Natl High Magnet Field Lab, Tallahassee, FL 32310 USA 5.Lanzhou Univ, Coll Chem Chem Engn, State Key Lab Appl Organ Chem, Lanzhou 730000, Peoples R China
推荐引用方式 GB/T 7714	Xu, Jun,Zheng, Anmin,Wang, Xiumei,et al. Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations[J]. CHEMICAL SCIENCE,2012,3(10):2932-2940.
APA	Xu, Jun.,Zheng, Anmin.,Wang, Xiumei.,Qi, Guodong.,Su, Jihu.,...&Deng, Feng.(2012).Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations.CHEMICAL SCIENCE,3(10),2932-2940.
MLA	Xu, Jun,et al."Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations".CHEMICAL SCIENCE 3.10(2012):2932-2940.