National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization, School of Chemical Engineering and Technology , Hebei University of Technology , Tianjin 300130 , China.
ACS Appl Mater Interfaces. 2019 Sep 18;11(37):33978-33986. doi: 10.1021/acsami.9b11578. Epub 2019 Sep 5.
Constructing three-dimensional (3D) hierarchical materials with spatial compartmentalization of multiple catalytic functionalities effectively facilitates the chemical processes' intensification, especially for bulky-molecule-involved cascade reaction. Herein, a facile and novel core-shell colloidal crystal templating strategy was developed to synthesize highly ordered arrays of integrated yolk-shelled nanoreactor consisting of monolithically interconnected ZIF-8 shell and sulfonated polystyrene yolks decorated with rhodium nanoparticles. The obtained nanoreactor achieves efficient catalytic one-pot cascade Knoevenagel condensation-hydrogenation reactions for larger molecules, by taking advantage of the superior mass diffusion properties of the hierarchical macro/microporous metal-organic framework (MOF) skeleton, robust monolith nature, and spatially separated functionalities. This work offers an important strategy for preparing MOF-based composites with a hierarchical framework, accelerating various applications of MOFs, such as electrochemical applications, photothermal conversion, and heterogeneous catalysis.
构建具有多种催化功能空间分隔的三维（3D）分层材料，有效地促进了化学过程的强化，特别是对于涉及大体积分子的级联反应。在此，本文开发了一种简便新颖的核壳胶体晶体模板策略，用于合成由单连通 ZIF-8 壳和磺化聚苯乙烯蛋黄组成的高度有序的整体蛋黄壳纳米反应器，其中负载有纳米铑颗粒。所得到的纳米反应器通过利用分级的大/微孔金属有机骨架（MOF）骨架、坚固的整体性质和空间分离功能的优越质量扩散特性，实现了对大体积分子的高效一锅法级联 Knoevenagel 缩合-氢化反应的催化。这项工作为制备具有分级框架的基于 MOF 的复合材料提供了一种重要策略，加速了 MOFs 在电化学应用、光热转换和多相催化等方面的各种应用。
