This title appears in the Scientific Report :
2018
Please use the identifier:
http://dx.doi.org/10.1021/jacs.8b01742 in citations.
Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair
Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair
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 c...
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Personal Name(s): | An, Jinghua |
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Wang, Yehong / Lu, Jianmin / Zhang, Jian / Zhang, Zhixin / Xu, Shutao / Liu, Xiaoyan / Zhang, Tao / Gocyla, Martin / Heggen, Marc / Dunin-Borkowski, Rafal / Fornasiero, Paolo / Wang, Feng (Corresponding author) | |
Contributing Institute: |
Mikrostrukturforschung; PGI-5 |
Published in: | Journal of the American Chemical Society, 140 (2018) 11, S. 4172 - 4181 |
Imprint: |
Washington, DC
American Chemical Society
2018
|
DOI: |
10.1021/jacs.8b01742 |
PubMed ID: |
29482317 |
Document Type: |
Journal Article |
Research Program: |
Controlling Configuration-Based Phenomena |
Publikationsportal JuSER |
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 (∼3500 h–1). The interfacial Lewis acid–base pair [Ru-O-Ce-Vö], which consists of acidic Ce-Vö (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 1H MAS NMR, pyridine-IR and DFT calculations reveals the hydrogen species derived from methanol contains Brönsted acidity. The EMC reaction mechanism under acid-promoter-free condition over Ru-clusters/ceria catalyst is discussed. |