首页> 外文期刊>Chemistry of Materials: A Publication of the American Chemistry Society >Engineering Lewis Acidity in Zeolite Catalysts by Electrochemical Release of Heteroatoms during Synthesis
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Engineering Lewis Acidity in Zeolite Catalysts by Electrochemical Release of Heteroatoms during Synthesis

机译:通过合成过程中杂原子的电化学释放来设计沸石催化剂中的路易斯酸度

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摘要

The creation of heteroatom nodes in zeolite frameworks is a challenging but rewarding pathway to superior materials for numerous catalytic applications. Here,we present a novel method for precise control over heteroatom incorporation by in situ anodic release of a desired metal during hydrothermal zeolite synthesis. The generic character of the technique and the applicability of the new synthesis reactor are shown across 3 zeolite structures crystallized and 4 electrode metals in two pH zones and by offering access to a new mixed-metal zeolite. The timed and voltage-controlled metal release offers a minimized interference between the metal precursor state and critical events in the zeolite's crystallization. A mechanistic study for Sn-MFI revealed the key importance of controlled release: while keeping its concentration lower than in batch,a lot more Sn can be incorporated into the framework. The method grants access to 10X increased framework Lewis acid site densities (vs batch controls) for the most relevant stannosilicates. As a proof,the electro-made materials demonstrate higher productivity than their classic counterparts in lactate catalysis. This innovative approach effectively expands the synthesis space of zeolites.
机译:在沸石框架中创建杂原子节点是一条具有挑战性但回报丰厚的途径,可获得用于众多催化应用的优质材料。在这里,我们提出了一种在水热沸石合成过程中通过原位阳极释放所需金属来精确控制杂原子掺入的新方法。该技术的通用特性和新合成反应器的适用性显示在两个 pH 区内的 3 种沸石结构结晶和 4 种电极金属上,并提供对新型混合金属沸石的访问。定时和电压控制的金属释放使金属前驱体状态与沸石结晶中的关键事件之间的干扰最小化。一项针对Sn-MFI的机理研究揭示了控释的关键重要性:在保持其浓度低于批次的同时,可以将更多的Sn纳入框架中。该方法允许获得最相关的锡硅酸盐的 10 倍的框架路易斯酸位点密度(与批次对照相比)。作为证明,电制材料在乳酸催化方面表现出比经典材料更高的生产率。这种创新方法有效地扩展了沸石的合成空间。

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