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@ARTICLE{An:858791,
author = {An, Jinghua and Wang, Yehong and Lu, Jianmin and Zhang,
Jian and Zhang, Zhixin and Xu, Shutao and Liu, Xiaoyan and
Zhang, Tao and Gocyla, Martin and Heggen, Marc and
Dunin-Borkowski, Rafal and Fornasiero, Paolo and Wang, Feng},
title = {{A}cid-{P}romoter-{F}ree {E}thylene {M}ethoxycarbonylation
over {R}u-{C}lusters/{C}eria: {T}he {C}atalysis of
{I}nterfacial {L}ewis {A}cid–{B}ase {P}air},
journal = {Journal of the American Chemical Society},
volume = {140},
number = {11},
issn = {1520-5126},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2018-07631},
pages = {4172 - 4181},
year = {2018},
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.},
cin = {PGI-5},
ddc = {540},
cid = {I:(DE-Juel1)PGI-5-20110106},
pnm = {143 - Controlling Configuration-Based Phenomena (POF3-143)},
pid = {G:(DE-HGF)POF3-143},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:29482317},
UT = {WOS:000428356000049},
doi = {10.1021/jacs.8b01742},
url = {https://juser.fz-juelich.de/record/858791},
}