A Polymer-Oriented Synthesis Of Triazinyl Functionalized Mesoporous Organic Polymer Encapsulating Uitrafine Metal Clusters for Alkynes Semi-Hydrogenation.

IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Rui Zhang, Shaohang Zheng, Luoqi Wang, Qingsong Li, Lichao Wang, Ling Zhang, Zhen-An Qiao
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Abstract

Preparation of highly dispersed ultrafine metal clusters (MCs)- based catalysts with good stability and preeminent catalytic performance is a challenging problem for heterogeneous catalysis. Herein, we design and controllably synthesize a triazinyl functionalized mesoporous organic polymer (TRI-MOP) through a polymer-oriented synthesis strategy using polyethyleneimine (PEI) as pore-forming agent. The obtained TRI-MOP material possesses abundant worm-like mesopores, rich triazinyl groups, and high stability. Ultrafine Pd clusters with a small size (≈0.76 nm) are successfully anchored in the mesoporous channel of TRI-MOP by a simple impregnation-reduction approach. The as-prepared Pd@TRI-MOP catalyst exhibits excellent catalytic activity (96%) and selectivity (97%) in the semi-hydrogenation of phenylacetylene under very mild reaction conditions. The exceptional performance of Pd@TRI-MOP catalyst is attributed to the small size effect of Pd clusters, the electron coupling effect between the supports and the Pd and enriched meso-scaled pores. Therefore, this work provides a new platform for designing and preparing stable functional porous organic polymer materials to confine size-controlled MCs with superior catalytic performance for diversified potential catalysis applications.

三嗪基功能化介孔有机聚合物包封氨基金属团簇用于炔半加氢的聚合物定向合成。
制备具有良好稳定性和优异催化性能的高分散超细金属团簇催化剂是多相催化领域的难题。本文以聚乙烯亚胺(PEI)为成孔剂,采用聚合物定向合成策略,设计并可控合成了三嗪基功能化介孔有机聚合物(TRI-MOP)。所得的TRI-MOP材料具有丰富的蠕虫状介孔、丰富的三嗪基和高的稳定性。通过简单的浸渍还原方法,成功地将小尺寸(≈0.76 nm)的超细Pd团簇固定在TRI-MOP的介孔通道中。制备的Pd@TRI-MOP催化剂在非常温和的反应条件下,对苯乙炔的半加氢反应具有优异的催化活性(96%)和选择性(97%)。Pd@TRI-MOP催化剂的优异性能主要归功于钯簇的小尺寸效应、载体与钯之间的电子耦合效应以及富集的介孔。因此,这项工作为设计和制备稳定的功能多孔有机高分子材料提供了一个新的平台,以限制具有优异催化性能的尺寸控制MCs,以实现多种潜在的催化应用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Chemistry - A European Journal
Chemistry - A European Journal 化学-化学综合
CiteScore
7.90
自引率
4.70%
发文量
1808
审稿时长
1.8 months
期刊介绍: Chemistry—A European Journal is a truly international journal with top quality contributions (2018 ISI Impact Factor: 5.16). It publishes a wide range of outstanding Reviews, Minireviews, Concepts, Full Papers, and Communications from all areas of chemistry and related fields. Based in Europe Chemistry—A European Journal provides an excellent platform for increasing the visibility of European chemistry as well as for featuring the best research from authors from around the world. All manuscripts are peer-reviewed, and electronic processing ensures accurate reproduction of text and data, plus short publication times. The Concepts section provides nonspecialist readers with a useful conceptual guide to unfamiliar areas and experts with new angles on familiar problems. Chemistry—A European Journal is published on behalf of ChemPubSoc Europe, a group of 16 national chemical societies from within Europe, and supported by the Asian Chemical Editorial Societies. The ChemPubSoc Europe family comprises: Angewandte Chemie, Chemistry—A European Journal, European Journal of Organic Chemistry, European Journal of Inorganic Chemistry, ChemPhysChem, ChemBioChem, ChemMedChem, ChemCatChem, ChemSusChem, ChemPlusChem, ChemElectroChem, and ChemistryOpen.
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