Journal Article

FZJ-2018-07631

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair

An, J. ; Wang, Y. ; Lu, J. ; Zhang, J. ; Zhang, Z. ; Xu, S. ; Liu, X. ; Zhang, T. ; Gocyla, M. ; Heggen, M.FZJ* ; Dunin-Borkowski, R.FZJ* ; Fornasiero, P. ; Wang, F. (Corresponding author)

2018
American Chemical Society Washington, DC

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Please use a persistent id in citations: doi:10.1021/jacs.8b01742

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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Contributing Institute(s):

1. Mikrostrukturforschung (PGI-5)

Research Program(s):

1. 143 - Controlling Configuration-Based Phenomena (POF3-143) (POF3-143)

Appears in the scientific report 2018

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Database coverage:
; BIOSIS Previews ; Clarivate Analytics Master Journal List ; Current Contents - Life Sciences ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; IF >= 10 ; JCR ; NCBI Molecular Biology Database ; Nationallizenz ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Web of Science Core Collection

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