Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid-Base Pair

Journal of the American Chemical Society
Jinghua AnFeng Wang

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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Citations

Mar 19, 2019·Angewandte Chemie·Zhifei HaoSihui Zhan
Jul 20, 2019·Chemical Communications : Chem Comm·Yu XinYanqin Wang
Dec 11, 2019·Chemical Communications : Chem Comm·Zhi-Qiao WangGuo-Cong Guo
Nov 1, 2018·Nanoscale Horizons : the Home for Rapid Reports of Exceptional Significance in Nanoscience and Nanotechnolgy·Li YuJiuhui Qu
Jul 26, 2021·Spectrochimica Acta. Part A, Molecular and Biomolecular Spectroscopy·Xiangchuan WuLina Wu
Dec 17, 2021·Chemistry, an Asian Journal·Wanjun GuoYanqin Wang

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