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Oxygen Vacancy in CeO 2 Facilitate the Catalytic Activity of Pd/CeO 2 for CO Direct Esterification to Dimethyl Oxalate
Catalysis Letters ( IF 2.8 ) Pub Date : 2021-05-15 , DOI: 10.1007/s10562-021-03650-4
Chao Hu , Kai-Qiang Jing , Xiao-Qi Lin , Jing Sun , Zhong-Ning Xu , Guo-Cong Guo

CO direct esterification to dimethyl oxalate (DMO) has important industrial application value. Pd-based heterogeneous catalysts have been often utilized for this reaction. However, the effects of defect structures causing by the different morphologies of the support on the catalytic performance has not been investigated sufficiently. In this work, three different morphologies of CeO2 support (denoted as rod, cube, and octahedron) loading Pd were synthesized, and further investigated their catalytic activities for CO direct esterification to DMO. The Pd/CeO2-rod catalyst exhibited the best CO conversion compared with Pd/CeO2-cube and Pd/CeO2-octa. The results of Raman and XPS show that CeO2-rod has the highest oxygen vacancy concentration than those of CeO2-cube and CeO2-octa. In addition, it was found that partial interfacial electrons transfer from Pd to CeO2 support at the interface from the result of XPS. More intriguingly, the result of in situ DRIRS of CO exhibits that the partial interfacial electrons transfer from CeO2 to Pd, resulting from oxygen vacancies serve as a charge compensator to promote partial electrons transfer. The enriched electron of Pd would promote the adsorption and activation of CO, thus enhancing the catalytic activity. This work will provide a general understanding of the support effect to catalytic performance, which induced by the oxygen vacancies.

Graphical Abstract



中文翻译:

CeO 2中的氧空位促进了Pd / CeO 2对CO直接酯化为草酸二甲酯的催化活性

CO直接酯化为草酸二甲酯(DMO)具有重要的工业应用价值。基于Pd的非均相催化剂通常被用于该反应。然而,尚未充分研究由载体的不同形态引起的缺陷结构对催化性能的影响。在这项工作中,合成了三种不同形态的CeO 2载体(表示为棒,立方和八面体)负载Pd,并进一步研究了它们对CO直接酯化为DMO的催化活性。与Pd / CeO 2-立方体和Pd / CeO 2-辛基相比,Pd / CeO 2-棒催化剂表现出最好的CO转化率。拉曼和XPS的结果表明CeO 2棒的空位浓度比CeO 2-立方体和CeO 2 -octa最高。另外,从XPS的结果发现,部分界面电子在界面处从Pd转移到CeO 2载体上。更有趣的是,CO的原位DRIRS结果表明,由于氧空位而导致的部分界面电子从CeO 2转移到Pd上,作为电荷补偿剂,促进了部分电子的转移。Pd的富集电子将促进CO的吸附和活化,从而增强催化活性。这项工作将提供对由氧空位引起的催化性能的支持作用的一般理解。

图形概要

更新日期:2021-05-15
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