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负载型铜/氧化锌催化剂中酒精诱导的强金属-载体相互作用。

Alcohol-Induced Strong Metal-Support Interactions in a Supported Copper/ZnO Catalyst.

机构信息

State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

出版信息

Angew Chem Int Ed Engl. 2023 May 15;62(21):e202301563. doi: 10.1002/anie.202301563. Epub 2023 Apr 18.

Abstract

Tuning the strong metal-support interaction (SMSI) in metal catalysts is a promising strategy to improve their catalytic performance. In this article, we systematically investigated the influences of different alcohol/water mixtures on the evolution of the interfacial structure of Cu/ZnO catalysts in the reduction stage. A series of in situ characterization and theoretical simulation studies were performed to elucidate the various mechanisms of alcohol induced SMSI. It was found that when methanol/water is added to H during the reduction pretreatment, more oxygen vacancies are formed on the ZnO support, which facilitates the dissociation of H O and the hydroxylation of ZnO species. Such promotion eventually favors the SMSI between Cu and ZnO and increases the catalytic activity for the methanol steam reforming reaction. In contrast, the addition of ethanol/water and 1-propanol/water during reduction leads to a physical blockage of the catalyst by alcohol molecules, poisoning the active Cu sites and limiting the migration of ZnO species.

摘要

调变金属催化剂中强的金属-载体相互作用(SMSI)是提高其催化性能的一种很有前途的策略。在本文中,我们系统地研究了不同醇/水混合物对 Cu/ZnO 催化剂在还原阶段界面结构演变的影响。进行了一系列的原位表征和理论模拟研究,以阐明醇诱导 SMSI 的各种机制。结果发现,当甲醇/水在还原预处理过程中加入 H 时,ZnO 载体上形成了更多的氧空位,这有利于 H O 的离解和 ZnO 物种的羟化。这种促进作用最终有利于 Cu 和 ZnO 之间的 SMSI,并提高甲醇蒸汽重整反应的催化活性。相比之下,在还原过程中加入乙醇/水和 1-丙醇/水会导致醇分子对催化剂的物理阻塞,使活性 Cu 位中毒,并限制 ZnO 物种的迁移。

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