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Fe-MOF-74的溶剂热合成及其在苯酚羟基化反应中的催化性能

Solvothermal synthesis of Fe-MOF-74 and its catalytic properties in phenol hydroxylation.

作者信息

Bhattacharjee Samiran, Choi Jung-Sik, Yang Seung-Tae, Choi Sang Beom, Kim Jaheon, Ahn Wha-Seung

机构信息

Department of Chemical Engineering, Inha University, Incheon 402-751, Korea.

出版信息

J Nanosci Nanotechnol. 2010 Jan;10(1):135-41. doi: 10.1166/jnn.2010.1493.

Abstract

A Fe-containing metal-organic framework, Fe-MOF-74, was solvothermally synthesized using FeCl2.4H2O and 2,5-di-hydroxy-1,4-benzenedicarboxylic acid. Characterization was conducted by XRD, BET surface area measurement, FT-IR spectroscopy, TGA, and elemental analysis, which confirmed successful preparation of Fe-MOF-74 having an identical framework structure to that reported for MOF-74. Fe-MOF-74 was found to be an effective heterogeneous catalyst for the hydroxylation of phenol using H2O2 as an oxidant; 60% phenol conversion was achieved at 20 degrees C in water with 68 and 32% selectivity to catechol and hydroquinone, respectively. The effect of temperature, phenol/H2O2 mole ratio, catalyst quantity, and solvent on catalytic performance was discussed, and a reaction mechanism is proposed based upon the experimental results.

摘要

采用FeCl₂·4H₂O和2,5 - 二羟基 - 1,4 - 苯二甲酸通过溶剂热法合成了一种含铁金属有机框架材料Fe - MOF - 74。通过X射线衍射(XRD)、比表面积测定(BET)、傅里叶变换红外光谱(FT - IR)、热重分析(TGA)和元素分析进行表征,证实成功制备了具有与报道的MOF - 74相同框架结构的Fe - MOF - 74。发现Fe - MOF - 74是以H₂O₂为氧化剂催化苯酚羟基化反应的有效多相催化剂;在20℃的水中,苯酚转化率达到60%,对邻苯二酚和对苯二酚的选择性分别为68%和32%。讨论了温度、苯酚/H₂O₂摩尔比、催化剂用量和溶剂对催化性能的影响,并根据实验结果提出了反应机理。

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