双金属Co/Zn沸石咪唑酯骨架材料ZIF-67负载的铜纳米颗粒:一种用于还原合成染料和硝基芳烃的优异催化剂。

Bimetallic Co/Zn zeolitic imidazolate framework ZIF-67 supported Cu nanoparticles: An excellent catalyst for reduction of synthetic dyes and nitroarenes.

作者信息

Budi Canggih Setya, Deka Juti Rani, Hsu Wan-Chi, Saikia Diganta, Chen Ke-Ting, Kao Hsien-Ming, Yang Yung-Chin

机构信息

Department of Chemistry, National Central University, Chung-Li 32054, Taiwan, ROC.

Institute of Materials Science and Engineering, National Taipei University of Technology, Taipei 106, Taiwan, ROC.

出版信息

J Hazard Mater. 2021 Apr 5;407:124392. doi: 10.1016/j.jhazmat.2020.124392. Epub 2020 Oct 29.

Abstract

In this study, a sub-class of microporous crystalline metal organic frameworks (MOFs) with zeolite-like configurations, i.e., zeolitic imidazolate frameworks of single node ZIF-67 and binary nodes ZIF-Co/Zn are used as the supports to develop Cu nanoparticles based nanocatalysts. Their catalytic activities are comparatively evaluated where Cu(x)@ZIF-Co/Zn exhibits better performances than Cu(x)@ZIF-67 in the reduction of synthetic dyes and nitroarenes. For instance, the Cu(0.25)@ZIF-Co/Zn catalyst shows an excellent reaction rate of 2.088 × 10 s and an outstanding activity of 104.4 sg for the reduction of methyl orange. The same catalyst also performs an exceptional catalytic activity in the hydrogenation of p-nitrophenol to p-aminophenol with the activity of 216.5 sg. A synergistic role of unique electronic properties rising from the direct contact of Cu NPs with the bimetallic nodes ZIF-Co/Zn, higher surface area of support, appropriate Cu loading and maintainable microporous frameworks with higher thermal and hydrolytic stability collectively enhances the catalytic activity of Cu(x)@ZIF-Co/Zn. Moreover, this catalyst shows excellent stability and recyclability, which can retain high conversion after reuse for 10 cycles.

摘要

在本研究中,一类具有类沸石构型的微孔晶体金属有机框架材料(MOFs),即单节点ZIF-67和双节点ZIF-Co/Zn的沸石咪唑酯框架材料,被用作载体来制备基于铜纳米颗粒的纳米催化剂。对它们的催化活性进行了比较评估,结果表明在还原合成染料和硝基芳烃方面,Cu(x)@ZIF-Co/Zn比Cu(x)@ZIF-67表现出更好的性能。例如,Cu(0.25)@ZIF-Co/Zn催化剂在还原甲基橙时显示出2.088×10 s的优异反应速率和104.4 sg的出色活性。同样的催化剂在对硝基苯酚加氢制对氨基苯酚的反应中也表现出卓越的催化活性,活性为216.5 sg。铜纳米颗粒与双金属节点ZIF-Co/Zn直接接触产生的独特电子性质、载体的高比表面积、适当的铜负载量以及具有更高热稳定性和水解稳定性的可维持微孔框架的协同作用,共同提高了Cu(x)@ZIF-Co/Zn的催化活性。此外,该催化剂表现出优异的稳定性和可回收性,重复使用10次后仍能保持高转化率。

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