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通过烯烃复分解反应和负载型铂将共价有机框架连接起来作为硅氢化反应的高效催化剂。

Tying Covalent Organic Frameworks through Alkene Metathesis and Supported Platinum as Efficient Catalysts for Hydrosilylation.

作者信息

Gu Defa, Li Guangwen, Liu Yushan, Liu Yuzhou

机构信息

School of Chemistry, Beihang University, Bejing 100191, China.

Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China.

出版信息

Nanomaterials (Basel). 2022 Jan 31;12(3):499. doi: 10.3390/nano12030499.

Abstract

Recently there has been a great interest in covalent organic frameworks due to their fascinating properties. Current approaches to improve their hydrolytic stability mainly rely on the transformation of the dynamic bonds into strong and irreversible bonds, but these approaches also reduce the versatility of the frameworks. Herein, we would like to demonstrate a solution to this dilemma by forming hierarchical bonds through olefin metathesis to produce highly stable COFs. Our approach allows unprecedented opportunities for post-modification of the inner space through the dynamic imine bonds while maintaining the integrity of the framework. Specifically, we demonstrate an amorphous-to-crystalline transformation. In addition, the porosity can be enhanced by up to 70% after full removal of the amine subunits. Overall, our work provides a new direction for the generation of highly stable while still versatile COFs. Meanwhile, platinum(II) complexes can be supported on BHU-2 (Pt@BHU-2) or BHU-2-Oxidate(Pt@BHU-2-Oxidate) as efficient catalysts for hydrosilylation.

摘要

近年来,共价有机框架因其迷人的特性而备受关注。目前提高其水解稳定性的方法主要依赖于将动态键转化为强不可逆键,但这些方法也降低了框架的多功能性。在此,我们想通过烯烃复分解形成分级键来制备高度稳定的共价有机框架,以此展示解决这一困境的方法。我们的方法为通过动态亚胺键对内部空间进行后修饰提供了前所未有的机会,同时保持框架的完整性。具体而言,我们展示了一种从无定形到结晶的转变。此外,在完全去除胺亚基后,孔隙率可提高多达70%。总体而言,我们的工作为生成高度稳定且仍具多功能性的共价有机框架提供了新方向。同时,铂(II)配合物可以负载在BHU-2(Pt@BHU-2)或BHU-2-氧化物(Pt@BHU-2-氧化物)上,作为硅氢化反应的高效催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a875/8915182/dcdaa627b997/nanomaterials-12-00499-sch001.jpg

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