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

被引：210

作者：

An, Jinghua ^{[1
,2
]}

Wang, Yehong ^{[1
]}

Lu, Jianmin ^{[1
]}

Zhang, Jian ^{[1
]}

Zhang, Zhixin ^{[1
]}

Xu, Shutao ^{[1
]}

Liu, Xiaoyan ^{[1
]}

Zhang, Tao ^{[1
]}

Gocyla, Martin ^{[3
,4
]}

Heggen, Marc ^{[3
,4
]}

Dunin-Borkowsk, Rafal E. ^{[3
,4
]}

Fornasiero, Paolo ^{[5
]}

Wang, Feng ^{[1
]}

机构：

[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

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2018年 / 140卷 / 11期

基金：

中国国家自然科学基金;

关键词：

METAL-SUPPORT INTERACTIONS; FINDING SADDLE-POINTS; SOLID-STATE NMR; CO OXIDATION; METHANOL SYNTHESIS; IN-SITU; PALLADIUM(II) COMPLEXES; SURFACE-CHEMISTRY; CERIA CATALYSTS; HYDROGENATION;

D O I：

10.1021/jacs.8b01742

中图分类号：

O6 [化学];

学科分类号：

0703 ;

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.

引用

页码：4172 / 4181

页数：10

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