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Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair
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Abstract 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.
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Metadata
- Authors
- An, J., Wang, Y., Lu, J., Zhang, J., Zhang, Z., Xu, S., Liu, X., Zhang, T., Gocyla, M., Heggen, M., Dunin-Borkowski, R. E., Fornasiero, P., & Wang, F.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-02-26
- Volume
- 140
- Issue
- 11
- Pages
- 4172-4181
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2794256365
- Cited by
- 258
- References
- 67
- FWCI
- 7.95
- Type
- journal article
- Language
- en
- Open access
- green
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