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新型对苯二酚-氧化铝复合材料稳定无客体包合物结构:在气体处理中的应用

Novel Hydroquinone-Alumina Composites Stabilizing a Guest-Free Clathrate Structure: Applications in Gas Processing.

作者信息

Coupan Romuald, Moonen Peter, Dicharry Christophe, Plantier Frédéric, Diaz Joseph, Péré Eve, Khoukh Abdel, Guerton Fabrice, Sénéchal Pascale, Charvillat Cédric, De Solan Marie-Line, Torré Jean-Philippe

机构信息

E2S UPPA, CNRS, Total, LFCR, Université de Pau et des Pays de l'Adour, Pau 64012, France.

Total Research & Technology Feluy, Zone Industrielle Feluy C, Seneffe 7181, Belgium.

出版信息

ACS Appl Mater Interfaces. 2020 Jul 29;12(30):34137-34147. doi: 10.1021/acsami.0c06187. Epub 2020 Jul 21.

DOI:10.1021/acsami.0c06187
PMID:32634302
Abstract

Organic clathrates formed by hydroquinone (HQ) and gases such as CO and CH are solid supramolecular host-guest compounds in which the gaseous guest molecules are encaged in a host framework of HQ molecules. Not only are these inclusion compounds fascinating scientific curiosities but they can also be used in practical applications such as gas separation. However, the development and future use of clathrate-based processes will largely depend on the effectiveness of the reactive materials used. These materials should enable fast and selective enclathration and have a large gas storage capacity. This article discusses the properties and performance of a new composite material able to form gas clathrates with hydroquinone (HQ) deposited on alumina particles. Apart from the general characterization of the HQ-alumina composite, one of the most remarkable observations is the unexpected formation of a guest-free clathrate structure with long-term stability (>2 years) inside the composite. Interestingly enough, in addition to a slight improvement in the enclathration kinetics of pure CO compared to powdered HQ, preferential capture of CO molecules is observed when the HQ-alumina composite is exposed to an equimolar CO/CH gas mixture. In terms of gas capture selectivity toward CO, the performance of this new composite exceeds that of pure HQ and HQ-silica composites developed in a previous study, opening up new opportunities for the design and use of these novel materials for gas separation.

摘要

由对苯二酚(HQ)与一氧化碳(CO)、甲烷(CH)等气体形成的有机包合物是固体超分子主客体化合物,其中气态客体分子被包裹在HQ分子的主体框架中。这些包合物不仅是引人入胜的科学奇物,还可用于气体分离等实际应用。然而,基于包合物的工艺的发展及未来应用在很大程度上取决于所用反应材料的有效性。这些材料应能实现快速且选择性的包合作用,并具有较大的气体储存容量。本文讨论了一种新型复合材料的性质和性能,该材料能够与沉积在氧化铝颗粒上的对苯二酚(HQ)形成气体包合物。除了对HQ-氧化铝复合材料进行一般性表征外,最显著的观察结果之一是在复合材料内部意外形成了具有长期稳定性(>2年)的无客体包合物结构。有趣的是,与粉末状HQ相比,纯CO的包合动力学略有改善,而且当HQ-氧化铝复合材料暴露于等摩尔的CO/CH气体混合物时,会观察到对CO分子的优先捕获。就对CO的气体捕获选择性而言,这种新型复合材料的性能超过了先前研究中开发的纯HQ和HQ-二氧化硅复合材料,为设计和使用这些用于气体分离的新型材料开辟了新机会。

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