Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair

doi:10.1021/jacs.8b01742

	Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair
	Zhang, Tao 1; An, Jinghua 1,2; Wang, Yehong 1; Lu, Jianmin 1; Zhang, Jian 1; Zhang, Zhixin 1; Xu, Shutao 1; Liu, Xiaoyan 1; Gocyla, Martin 3,4; Heggen, Marc 3,4
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2018-03-21
卷号	140 期号:11 页码:4172-4181
ISSN号	0002-7863
DOI	10.1021/jacs.8b01742
文献子类	Article
英文摘要	The interface of metal-oxide plays pivotal roles in catalytic reactions, but its catalytic function is still not clear. In this study, we report the high activity of nanostructured Ru/ceria (Ru-clusters/ceria) in the ethylene methoxycarbonylation (EMC) reaction in the absence of acid promoter. The catalyst offers 92% yield of MP with TOF of 8666 h(-1), which is about 2.5 times of homogeneous Pd catalyst (similar to 3500 h(-1)). The interfacial Lewis acid base pair [Ru-O-Ce-Vo], which consists of acidic Ce-Vo (oxygen vacancy) site and basic interfacial oxygen of Ru-O-Ce linkage, acts as active site for the dissociation of methanol and the subsequent transfer of hydrogen to the activated ethylene, which is the key step in acid-promoter-free EMC reaction. The combination of H-1 MAS NMR, pyridine-IR and DFT calculations reveals the hydrogen species derived from methanol contains Bronsted acidity. The EMC reaction mechanism under acid-promoter-free condition over Ru-clusters/ceria catalyst is discussed.
WOS关键词	METAL-SUPPORT INTERACTIONS ; FINDING SADDLE-POINTS ; SOLID-STATE NMR ; CO OXIDATION ; CERIA CATALYSTS ; INFRARED-SPECTROSCOPY ; METHANOL SYNTHESIS ; IN-SITU ; PALLADIUM(II) COMPLEXES ; HETEROGENEOUS CATALYSIS
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000428356000049
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/168972]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Wang, Feng
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany 4.Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany 5.Univ Trieste, INSTM, Ctr Excellence Nanostruct Mat CENMAT, Dept Chem & Pharmaceut Sci, Via L Giorgieri 1, I-34127 Trieste, Italy
推荐引用方式 GB/T 7714	Zhang, Tao,An, Jinghua,Wang, Yehong,et al. Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2018,140(11):4172-4181.
APA	Zhang, Tao.,An, Jinghua.,Wang, Yehong.,Lu, Jianmin.,Zhang, Jian.,...&Wang, Feng.(2018).Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,140(11),4172-4181.
MLA	Zhang, Tao,et al."Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 140.11(2018):4172-4181.