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Semipermeable Organic–Inorganic Hybrid Microreactors for Highly Efficient and Size-Selective Asymmetric Catalysis
ACS Catalysis ( IF 12.9 ) Pub Date : 2017-09-06 00:00:00 , DOI: 10.1021/acscatal.7b01659
Xiaoming Zhang 1 , Lingyan Jing 1 , Lijuan Wei 1 , Fengwei Zhang 2 , Hengquan Yang 1
Affiliation  

A highly efficient and size-selective organic–inorganic hybrid microreactor was fabricated successfully by assembling the semipermeable microporous silica hollow nanospheres at the interface of organic polymers containing an asymmetric transfer hydrogenation catalyst. The small micropores in the silica shells (1.0–1.5 nm) of the microreactors provide short mass-transfer channels for small molecules but prevent the diffusion of large reactants through the shell. At the same time, the combination of the outer microporous silica and inner polymers endows the microreactor with hydrophobic@hydrophilic property, which helps its dispersion in water as well as the adsorption of reactant molecules from water, yielding an ideal microenvironment for water medium catalysis reactions. Such microreactors could efficiently catalyze the aqueous asymmetric transfer hydrogenation (ATH) of small-sized ketones with catalytic activity comparable to the homogeneous Rh-VBSDPEN catalyst (TOF 625 vs 724 h–1). Meanwhile, the microreactors also showed size selectivity toward large-sized reactants. Our studies provide an approach for the construction of artificial bioinspired microreactors with size-selective properties and favorable catalysis microenvironments.

中文翻译:

半透性有机-无机杂化微反应器,用于高效和尺寸选择性的不对称催化

通过在含有不对称转移加氢催化剂的有机聚合物的界面上组装半透性微孔二氧化硅空心纳米球,成功地制造了一种高效且尺寸选择性的有机-无机杂化微反应器。微反应器的二氧化硅壳(1.0-1.5 nm)中的小微孔为小分子提供了短的传质通道,但阻止了大反应物通过壳扩散。同时,外部微孔二氧化硅和内部聚合物的结合使微反应器具有疏水亲水性,这有助于其在水中的分散以及从水中吸附反应物分子,从而为水介质催化反应提供了理想的微环境。 。–1)。同时,微反应器还显示出对大型反应物的尺寸选择性。我们的研究为构建具有尺寸选择特性和良好催化微环境的人工生物启发式微反应器提供了一种方法。
更新日期:2017-09-07
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