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	The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature
	Zhang, Zhenzhou1,2; Zhang, Qingde1; Jia, Lingyu1,2; Wang, Wenfeng1,2; Tian, Shao Peng1,2; Wang, Peng1,2; Xiao, He1,2; Han, Yizhuo1; Tsubaki, Noritatsu1,3; Tan, Yisheng1
刊名	Catalysis science & technology
	2016
卷号	6期号:15页码:6109-6117
ISSN号	2044-4753
DOI	10.1039/c6cy00460a
通讯作者	Zhang, qingde(qdzhang@sxicc.ac.cn) ; Tan, yisheng(tan@sxicc.ac.cn)
英文摘要	With increasing degrees of mo-sn interface contact, the molar ratio of methyl formate (mf) to methanol (meoh) and formaldehyde (fa) was found to linearly increase at the same time, which indicates that a high degree of moo3 and sno2 interface contact has a strong positive effect on the conversion of the methoxyl intermediate to mf in the dimethyl ether (dme) oxidation reaction. xrd and fourier transform exafs indicate that the structure of molybdenum oxide starts to change from moo3 clusters to oligomer moox domains with an increase in the degree of mo-sn interface contact, and the mo-o-sn structure begins to dominate at the contact interfaces when the degree of interface contact increases to 0.0256 and 0.0384 nm(2) sno2/mo atom. hrtem also confirms the presence of the moox domains on the surface of the catalyst possessing the smallest molybdenum oxide content, the signals of which were even undetected by xrd and raman. moreover, esr, xps and xafs suggest that mo5+ species exist in the mo-sn contact interfaces rather than on the surface of the catalysts. the evaluation results of moo3-sba-15 further verify the key role of mo5+ in the formation of mf. therefore, mo5+ is reasonably proposed to be the active center for the formation of mf in the dme oxidation reaction. based on the catalytic characterization results, the reaction pathway of dme oxidation to mf via methoxyl intermediates was proposed on the mo(v) sites. first, dme was absorbed and consequently dissociated to become an absorbed methoxy-mo(v) species with the assistance of acidic sites and lattice oxygen. then, the beta-h was eliminated, and an absorbed fa-mo(iv) species was formed. consequently, the absorbed methoxy-mo(v) species reacted with the neighboring absorbed fa-mo(iv) species, producing mf, and then, the mo(iv) species was regenerated to become an mo(v) species by the oxidation of o-2 so it could catalyze another reaction cycle. the deeper understanding of this investigation has substantial meaning for the preparation of a catalyst with a specific molybdenum oxide structure that can be applied for transforming the methoxyl intermediate to produce other high-value products through the dme oxidation reaction.
WOS关键词	SELECTIVE OXIDATION ; MOLYBDENUM OXIDE ; MILD CONDITIONS ; GAMMA-ALUMINA ; CATALYSTS ; METHANOL ; FORMALDEHYDE ; SURFACE ; ACID ; NANOPARTICLES
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000381431200035
内容类型	期刊论文
URI标识	http://www.corc.org.cn/handle/1471x/2376223
专题	中国科学院大学
通讯作者	Zhang, Qingde; Tan, Yisheng
作者单位	1.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Toyama Univ, Sch Engn, Dept Appl Chem, Gofuku 3190, Toyama 9308555, Japan
推荐引用方式 GB/T 7714	Zhang, Zhenzhou,Zhang, Qingde,Jia, Lingyu,et al. The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature[J]. Catalysis science & technology,2016,6(15):6109-6117.
APA	Zhang, Zhenzhou.,Zhang, Qingde.,Jia, Lingyu.,Wang, Wenfeng.,Tian, Shao Peng.,...&Tan, Yisheng.(2016).The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature.Catalysis science & technology,6(15),6109-6117.
MLA	Zhang, Zhenzhou,et al."The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature".Catalysis science & technology 6.15(2016):6109-6117.

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