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MnO-Au 纳米花中活性相和载体优化的结合:对绿色氧化反应表现出高活性。

Combining active phase and support optimization in MnO-Au nanoflowers: Enabling high activities towards green oxidations.

机构信息

Departamento de Química Fundamental, Instituto de Química, Universidade de São Paulo, Av. Prof. Lineu Prestes, 748, 05508-000 São Paulo, SP, Brazil.

Departamento de Engenharia Química, Universidade Federal de São Carlos, 13565-905 São Carlos, SP, Brazil.

出版信息

J Colloid Interface Sci. 2018 Nov 15;530:282-291. doi: 10.1016/j.jcis.2018.06.089. Epub 2018 Jun 28.

Abstract

Among the several classes of chemical reactions, the green oxidation of organic compounds has emerged as an important topic in nanocatalysis. Nonetheless, examples of truly green oxidations remain scarce due to the low activity and selectivity of reported catalysts. In this paper, we present an approach based on the optimization of both the support material and the active phase to achieve superior catalytic performances towards green oxidations. Specifically, our catalysts consisted of ultrasmall Au NPs deposited onto MnO nanoflowers. They displayed hierarchical morphology, large specific surface areas, ultrasmall and uniform Au NPs sizes, no agglomeration, strong metal-support interactions, oxygen vacancies, and Au species at their surface. These features led to improved performances towards the green oxidations of CO, benzene, toluene, o-xylene, glucose, and fructose relative to the pristine MnO nanoflowers, commercial MnO decorated with Au NPs, and other reported catalysts. We believe that the catalytic activities, stabilities, and mild/green reaction conditions described herein for both gas and liquid phase oxidations due to the optimization of both the support and active phase may inspire the development of novel catalytic systems for a wealth of sustainable transformations.

摘要

在几类化学反应中,有机化合物的绿色氧化已成为纳米催化中的一个重要课题。然而,由于报道的催化剂活性和选择性较低,真正的绿色氧化实例仍然很少。在本文中,我们提出了一种基于优化载体材料和活性相的方法,以实现绿色氧化的优异催化性能。具体来说,我们的催化剂由沉积在 MnO 纳米花上的超小 Au NPs 组成。它们具有分级形貌、大比表面积、超小且均匀的 Au NPs 尺寸、无团聚、强的金属-载体相互作用、氧空位和表面上的 Au 物种。这些特性导致它们在 CO、苯、甲苯、对二甲苯、葡萄糖和果糖的绿色氧化方面的性能优于原始 MnO 纳米花、用 Au NPs 修饰的商业 MnO 和其他报道的催化剂。我们相信,由于优化了载体和活性相,本文中描述的气-液两相氧化反应的催化活性、稳定性和温和/绿色反应条件可能会激发新型催化体系的发展,从而实现丰富的可持续转化。

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