%0 Journal Article
%A An, Jinghua
%A Wang, Yehong
%A Lu, Jianmin
%A Zhang, Jian
%A Zhang, Zhixin
%A Xu, Shutao
%A Liu, Xiaoyan
%A Zhang, Tao
%A Gocyla, Martin
%A Heggen, Marc
%A Dunin-Borkowski, Rafal
%A Fornasiero, Paolo
%A Wang, Feng
%T Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair
%J Journal of the American Chemical Society
%V 140
%N 11
%@ 1520-5126
%C Washington, DC
%I American Chemical Society
%M FZJ-2018-07631
%P 4172 - 4181
%D 2018
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%$ pmid:29482317
%U <Go to ISI:>//WOS:000428356000049
%R 10.1021/jacs.8b01742
%U https://juser.fz-juelich.de/record/858791