TY  - JOUR
AU  - An, Jinghua
AU  - Wang, Yehong
AU  - Lu, Jianmin
AU  - Zhang, Jian
AU  - Zhang, Zhixin
AU  - Xu, Shutao
AU  - Liu, Xiaoyan
AU  - Zhang, Tao
AU  - Gocyla, Martin
AU  - Heggen, Marc
AU  - Dunin-Borkowski, Rafal
AU  - Fornasiero, Paolo
AU  - Wang, Feng
TI  - Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair
JO  - Journal of the American Chemical Society
VL  - 140
IS  - 11
SN  - 1520-5126
CY  - Washington, DC
PB  - American Chemical Society
M1  - FZJ-2018-07631
SP  - 4172 - 4181
PY  - 2018
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - pmid:29482317
UR  - <Go to ISI:>//WOS:000428356000049
DO  - DOI:10.1021/jacs.8b01742
UR  - https://juser.fz-juelich.de/record/858791
ER  -