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Fast room temperature lability of aluminosilicate zeolites

机译:硅铝酸盐沸石在室温下的快速固化

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摘要

Aluminosilicate zeolites are traditionally used in high-temperature applications at low water vapour pressures where the zeolite framework is generally considered to be stable and static. Increasingly, zeolites are being considered for applications under milder aqueous conditions. However, it has not yet been established how neutral liquid water at mild conditions affects the stability of the zeolite framework. Here, we show that covalent bonds in the zeolite chabazite (CHA) are labile when in contact with neutral liquid water, which leads to partial but fully reversible hydrolysis without framework degradation. We present ab initio calculations that predict novel, energetically viable reaction mechanisms by which Al-O and Si-O bonds rapidly and reversibly break at 300 K. By means of solid-state NMR, we confirm this prediction, demonstrating that isotopic substitution of 17O in the zeolitic framework occurs at room temperature in less than one hour of contact with enriched water.
机译:硅铝酸盐沸石传统上用于低水蒸气压的高温应用中,其中通常认为沸石骨架是稳定和静态的。越来越多地考虑将沸石用于温和的水性条件下。然而,尚未确定在温和条件下中性液态水如何影响沸石骨架的稳定性。在这里,我们显示了沸石菱沸石(CHA)中的共价键在与中性液态水接触时不稳定,这会导致部分但完全可逆的水解而没有骨架降解。我们提供了从头算的方法来预测新颖的,在能量上可行的反应机理,通过该机理,Al-O和Si-O键在300 K处快速且可逆地断裂。通过固态NMR,我们证实了这一预测,证明了<沸石骨架中的sup> 17 O在室温下与浓缩水接触不到一小时就会发生。

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