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用于优异催化氧化的超薄 Mn 基复合材料中的多界面耦合:界面耦合对结构缺陷的影响。

Multiple interface coupling in ultrathin Mn-based composites for superior catalytic oxidation: Implications of interface coupling on structural defects.

机构信息

Department of Inorganic Materials, School of Minerals Processing and Bioengineering, Central South University, Changsha 410083, China; Hunan Key Lab of Mineral Materials and Application, Central South University, Changsha 410083, China.

School of Civil and Environmental Engineering, Faculty of Engineering, Queensland University of Technology, Brisbane, Queensland 4001, Australia.

出版信息

J Colloid Interface Sci. 2023 Jul 15;642:380-392. doi: 10.1016/j.jcis.2023.03.150. Epub 2023 Mar 28.

Abstract

Manganese oxide has been recognized as one of the most promising gaseous heterogeneous catalysts due to its low cost, environmental friendliness, and high catalytic oxidation performance. The modulation of the interfacial coupling effect of manganese oxides by chemical means is considered a critical and effective way to improve the catalytic performance. Herein, a novel one-step synthetic strategy of highly-efficient ultrathin manganese-based catalysts is proposed through optimal regulation of metal/manganese oxide multi-interfacial coupling. Carbon monoxide (CO) and propane (CH) oxidation are employed as probe reactions to investigate the structure-catalytic mechanism - catalytic performance relationship. The ultrathin manganese (Mn)-based catalyst exhibits superior low-temperature catalytic activity with a 90% conversion of CO/CH realized at 106℃ and 350℃. Subsequently, the effect of "interfacial effect" on the intrinsic properties of manganese oxides is revealed. The ultrathin appearance of two-dimensional (2D) manganese dioxide (MnO) nanosheets changes the binding force in the vertical direction, thus resulting in an increase in the average manganese-oxygen (Mn-O) bond length and exposing more surface defects. Besides, the introduction of Copper (Cu) species into the catalyst further weakens the Mn-O bond and promotes the generation of oxygen vacancies, which subsequently enhances the oxygen migration rate. This study provides new insights into the optimal design of transition metal oxide interfacial assemblies for efficient catalytic reactions.

摘要

氧化锰因其成本低、环境友好和高催化氧化性能而被认为是最有前途的气态多相催化剂之一。通过化学手段调节氧化锰的界面耦合效应被认为是提高催化性能的关键和有效途径。本文通过优化金属/氧化锰多界面耦合,提出了一种高效超薄锰基催化剂的新型一步合成策略。以一氧化碳(CO)和丙烷(CH)氧化为探针反应,研究了结构-催化机理-催化性能的关系。超薄锰(Mn)基催化剂表现出优异的低温催化活性,在 106℃和 350℃时 CO/CH 的转化率达到 90%。随后,揭示了“界面效应”对氧化锰固有性质的影响。二维(2D)二氧化锰(MnO)纳米片的超薄外观改变了垂直方向的结合力,从而导致平均锰-氧(Mn-O)键长增加,并暴露出更多的表面缺陷。此外,将铜(Cu)物种引入催化剂中进一步削弱了 Mn-O 键,并促进了氧空位的产生,从而提高了氧迁移率。本研究为高效催化反应中过渡金属氧化物界面组装的优化设计提供了新的见解。

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