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具有动态脉动运动的催化活性多孔组件,用于高效交换产物和试剂。

Catalytically-active porous assembly with dynamic pulsating motion for efficient exchange of products and reagents.

作者信息

Wu Shanshan, Huang Liping, Hou Yu, Liu Xin, Kim Jehan, Liang Yongri, Zhao Jiong, Zhang Liwei, Ji Hongbing, Lee Myongsoo, Huang Zhegang

机构信息

Fine Chemical Industry Research Institute and PCFM Lab, School of Chemistry, Sun Yat-sen University, Guangzhou, 510275, PR China.

State Key Laboratory for Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, PR China.

出版信息

Commun Chem. 2020 Jan 24;3(1):11. doi: 10.1038/s42004-020-0259-4.

Abstract

Despite recent advances in the use of porous materials as efficient heterogeneous catalysts which operate through effectively trapping reagents in a well-defined space, continuously uptaking reagents to substitute products in the cavity for efficient product turnover still remains challenging. Here, a porous catalyst is endowed with 'breathing' characteristics by thermal stimulus, which can enable the efficient exchange of reagents and products through reversible stacking from inflated aromatic hexamers to contracted trimeric macrocycles. The contracted super-hydrophobic tubular interior with pyridine environment exhibits catalytic activity towards a nucleophilic aromatic substitution reaction by promoting interactions between concentrated reagents and active sites. Subsequent expansion facilitates the exchange of products and reagents, which ensures the next reaction. The strategy of mesoporous modification with inflatable transition may provide a new insight for construction of dynamic catalysts.

摘要

尽管在使用多孔材料作为高效多相催化剂方面取得了最新进展,这类催化剂通过在明确界定的空间中有效捕获试剂来发挥作用,但要持续摄取试剂以在腔内替换产物从而实现高效的产物周转仍然具有挑战性。在此,一种多孔催化剂通过热刺激具备了“呼吸”特性,这能够通过从膨胀的芳香六聚体到收缩的三聚大环的可逆堆叠实现试剂和产物的高效交换。具有吡啶环境的收缩超疏水管状内部通过促进浓缩试剂与活性位点之间的相互作用,对亲核芳香取代反应表现出催化活性。随后的膨胀促进了产物和试剂的交换,从而确保下一次反应。具有可膨胀转变的介孔修饰策略可能为构建动态催化剂提供新的思路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9d46/9814577/86efd080cfd6/42004_2020_259_Fig1_HTML.jpg

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