Catalytic activity of immobilized Ru nanoparticles in a porous metal-organic framework using supercritical fluid

Abstract

A Zr-based metal-organic framework (Zr-MOF) with both micropores and mesopores was prepared by the reaction of 1,4-benzenedicarboxylic acid (H 2 BDC) and ZrOCl 2 ·8H 2 O with the aid of a citric acid (CA) chelating agent and a cetyltrimethylammonium bromide (CTAB) surfactant. This was followed by formation of a Ru@Zr-MOF catalyst from RuCl 3 ·3H 2 O in a supercritical CO 2 -methanol solution. The catalyst was characterized by Fourier transform infrared spectroscopy, power X-ray diffraction, transmission electron microscopy, thermo-gravimetric analysis, N 2 adsorption-desorption, X-ray photoelectron spectroscopy, and inductively coupled plasma-atomic emission spectroscopy. Ru particles with an average diameter of 2.3 nm were uniformly supported in the Zr-MOF. The catalytic performance of Ru@Zr-MOF for the hydrogenation of benzene and its derivatives was investigated and was found to be active and stable. 以柠檬酸为螯合剂, 十六烷基三甲基溴化胺为表面活性剂, 通过 ZrOCl 2 ·8H 2 O 与对苯二甲酸 (H 2 BDC) 反应制备了同时具有微孔和介孔结构的 Zr 基金属有机骨架材料 (Zr-MOF), 并在超临界 CO 2 -甲醇流体中将 Ru 负载于 Zr-MOF 上, 制备了 Ru@Zr-MOF 催化剂, 采用傅里叶变换红外光谱、X 射线粉末衍射、透射电子显微镜、热重分析、N 2 吸附-脱附、X 射线光电子能谱和电感耦合等离子体发射光谱对催化剂进行了表征, 研究了该催化剂在苯及其同系物加氢反应中的催化性能. 结果表明, Ru 纳米金属颗粒均匀地分散在 Zr-MOF 载体上, 平均粒径约为 2.3 nm, 在苯及其同系物的加氢反应中表现出很高的催化活性和稳定性. Ru nanoparticles are immobilized in a Zr-based metal-organic framework (MOF) having both micropores and mesopores. The Ru@Zr-MOF catalyst for the hydrogenation of benzene and its derivatives is very active and stable.