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Development and Elucidation of Superior Turnover Rates and Selectivity of Supported Molecular Catalysts
ChemCatChem ( IF 4.5 ) Pub Date : 2018-02-06 , DOI: 10.1002/cctc.201701546
Rong Ye 1, 2 , Wen‐Chi Liu 1, 2 , Hui‐Ling Han 1, 3 , Gabor A. Somorjai 1, 2, 3
Affiliation  

Supported molecular catalysts consist of nanomaterials immobilized on a solid support. Important factors that control catalyst properties (reactivity, product selectivity, and stability) include the structure and compositions of both nanomaterials and supports. This review focuses on recent studies of supported molecular catalysts with controlled activity and selectivity in our group. We will first introduce the development of previously unexplored supported molecular catalysts. We will demonstrate the controllable selectivity of catalysts based on acidified mesoporous silica, metal‐organic frameworks (MOFs), hydrogen‐activated tungsten oxides, and noble metal doped MnxOy/Na2WO4 catalyst supported on mesoporous silica. We will then discuss advanced characterization techniques under reaction conditions, which offer mechanistic explanations of activity and selectivity of supported molecular catalysts. The applications of chemical transient kinetics (CTK) analysis, ambient pressure X‐ray photoelectron spectroscopy (APXPS), and sum‐frequency generation vibrational spectroscopy (SFG‐VS) are discussed. Next, we will describe new insights into catalysis at the nanoparticle‐support interfaces, which are catalytic environments unique to supported molecular catalysts. Examples include reactions at oxide‐metal interfaces and alcohol oxidation reactions at solid–gas and solid–liquid interfaces. Lastly, we will discuss heterogenized homogeneous catalysts and heterogenized enzyme catalysts as future directions of supported molecular catalysts.

中文翻译:

出色的周转率和负载型分子催化剂的选择性的开发与阐明

负载型分子催化剂由固定在固体载体上的纳米材料组成。控制催化剂性能(反应性,产物选择性和稳定性)的重要因素包括纳米材料和载体的结构和组成。这篇综述的重点是在我们小组中对具有受控活性和选择性的负载型分子催化剂的最新研究。我们将首先介绍以前未开发的负载型分子催化剂的开发。我们将展示基于酸化介孔二氧化硅,金属有机骨架(MOF),氢活化氧化钨和掺杂贵金属的Mn x O y / Na 2 WO 4的催化剂的可控选择性。催化剂负载在介孔二氧化硅上。然后,我们将讨论反应条件下的高级表征技术,该技术对负载型分子催化剂的活性和选择性进行了机械解释。讨论了化学瞬态动力学(CTK)分析,环境压力X射线光电子能谱(APXPS)和和频产生振动光谱(SFG-VS)的应用。接下来,我们将描述对纳米颗粒-载体界面催化的新见解,这是负载型分子催化剂特有的催化环境。例子包括在氧化物-金属界面的反应以及在固-气和固-液界面的醇氧化反应。最后,
更新日期:2018-02-06
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