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掺杂介孔碳中限域的氧化铈纳米颗粒:一种制备亚胺合成催化剂的策略。

Cerium Oxide Nanoparticles Confined in Doped Mesoporous Carbons: A Strategy to Produce Catalysts for Imine Synthesis.

作者信息

Lima Oliveira Rafael, Ledwa Karolina A, Chernyayeva Olga, Praetz Sebastian, Schlesiger Christopher, Kepinski Leszek

机构信息

Institute of Low Temperature and Structure Research of the Polish Academy of Sciences, 50-422 Wroclaw, Poland.

Institute of Physical Chemistry of the Polish Academy of Sciences, 01-224 Warsaw, Poland.

出版信息

Inorg Chem. 2023 Aug 21;62(33):13554-13565. doi: 10.1021/acs.inorgchem.3c01985. Epub 2023 Aug 9.

Abstract

A group of (doped N or P) carbons were synthesized using soluble starch as a carbon precursor. Further, ceria nanoparticles (NPs) were confined into these (doped) carbon materials. The obtained solids were characterized by various techniques such as N physisorption, XRD, TEM, SEM, XPS, and XAS. These materials were used as catalysts for the oxidative coupling between benzyl alcohol and aniline as the model reaction. Ceria immobilized on mesoporous-doped carbon shows higher activity than the other materials, benchmark catalysts, and most of the previously reported catalysts. The control of the ceria NP size, the presence of Ce cations, and an increment in the disorder in the ceria NP structure caused by a support-ceria interaction could increase the number of oxygen vacancies and improve its catalytic performance. CN-meso/CeO was also used as the catalyst for a rich scope of substrates, such as substituted aromatic alcohols, linear alcohols, and different types of amines. The influence of various reaction parameters (substrate content, reaction temperature, and catalyst content) on the activity of this catalyst was also checked.

摘要

使用可溶性淀粉作为碳前驱体合成了一组(掺杂N或P的)碳材料。此外,将二氧化铈纳米颗粒(NPs)限制在这些(掺杂的)碳材料中。通过诸如N物理吸附、XRD、TEM、SEM、XPS和XAS等各种技术对所得固体进行了表征。这些材料用作苯甲醇和苯胺之间氧化偶联的模型反应的催化剂。负载在介孔掺杂碳上的二氧化铈显示出比其他材料、基准催化剂以及大多数先前报道的催化剂更高的活性。二氧化铈NP尺寸的控制、Ce阳离子的存在以及由载体 - 二氧化铈相互作用引起的二氧化铈NP结构无序度的增加可增加氧空位的数量并改善其催化性能。CN - meso/CeO还用作多种底物的催化剂,如取代的芳族醇、直链醇和不同类型的胺。还研究了各种反应参数(底物含量、反应温度和催化剂含量)对该催化剂活性的影响。

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