N-甲基咪唑配体络合金属Cu(I)催化剂对水中2,4-二甲氧基溴苯还原脱溴

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合成了以N-甲基咪唑为配体,Cu为活性中心的络合金属多相催化剂Cu(I)-NHC-SBA-15。通过1H-NMR、13CNMR、有机元素分析和FTIR对各步合成反应产物结构经行了鉴定;用SEM、N2吸附脱附等方法对催化剂进行了表征;用ICP测定了催化剂Cu含量。对催化剂催化2,4-二甲氧基溴苯还原脱溴活性进行了测试。在反应时间为24 h,通过正交实验和单因素实验,考察了催化剂用量、反应温度、还原剂用量等因素对脱溴率的影响,并确定了最佳反应条件:催化剂用量为0.05 g、水合肼用量为2 m L、反应温度为80℃,脱溴效果较好,脱溴率达到98.5%。对催化剂重复使用进行了初步研究。对催化反应动力学进行了初步研究,结果表明,该多相催化反应是由表面反应速度控制,并符合一级动力学反应。对反应机理进行了初步探讨。 A complex metal heterogeneous catalyst Cu (I) -NHC-SBA-15 with N-methylimidazole as ligand and Cu as active center was synthesized. The structures of the reaction products were characterized by 1H-NMR, 13CNMR, organic elemental analysis and FTIR. The catalysts were characterized by means of SEM and N2 adsorption-desorption. The content of Cu in the catalyst was determined by ICP. The catalytic dechlorination activity of 2,4-dimethoxy-bromobenzene catalyzed by the catalyst was tested. The reaction time was 24 h, the effects of catalyst dosage, reaction temperature and the amount of reductant on the debromination rate were investigated by orthogonal experiments and single factor experiments. The optimum reaction conditions were determined as follows: the amount of catalyst was 0.05 g, The amount of hydrazine hydrate is 2 m L, the reaction temperature is 80 ℃, the debromination is better and the debromination rate reaches 98.5%. A preliminary study of catalyst re-use was carried out. The kinetics of catalytic reaction was studied preliminarily. The results show that the heterogeneous catalytic reaction is controlled by the surface reaction rate and accords with the first-order kinetic reaction. The reaction mechanism was discussed.
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