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作 者:许响生[1] 陈傲昂[1] 周莉[1] 李小青[1] 顾辉子[1] 严新焕[1]
机构地区:[1]浙江工业大学绿色化学合成技术国家重点实验室培育基地,浙江杭州310014
出 处:《催化学报》2013年第2期391-396,共6页
基 金:国家自然科学基金(21076197;20676124);浙江省自然科学基金项目(Y4090440);浙江省钱江人才项目(2010R10038)~~
摘 要:采用浸渍法制备Ru/C催化剂,并用于原位液相催化邻氯硝基苯(o-CNB)加氢合成邻氯苯胺(o-CAN)反应中.考察了浸渍顺序、助剂、还原温度、载体和助剂含量等因素对催化剂稳定性的影响.采用透射电子显微镜、X射线光电子能谱、傅里叶红外光谱和N2吸附-脱附等手段表征催化剂.结果表明,以15%Fe为助剂,活性炭为载体,制备得到的0.5%Ru-Fe/C催化剂经过523K氢气还原后o-CNB的转化率为99.7%,o-CAN的选择性达到98.7%,反应140h未出现明显失活.催化剂表面吸附CO导致中毒是失活的主要原因,同时对催化剂再生方法进行了探究.Ru-based crystalline catalysts were prepared by the impregnation method using different supports and promoters and were applied in the in-situ liquid phase catalytic hydrogenation of ortho-chloronitrobenzene (o-CNB) to ortho-chloroaniline (o-CAN). The effects of different preparation factors (including impregnation sequence, promoters, reduction temperature, supporters and promoter content) on the catalyst stability were investigated. The Ru-Fe/C catalyst was systematically characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and N2adsorption-desorption with regard to physical-chemical properties such as particle size and distribution, electronic state, adsorption species, and surface parameters. The results indicated that the 0.5%Ru-15%Fe/C catalyst hashigher hydrogenation activity with 99.7% o-CNB conversion and 98.7% o-CAN selectivity.The catalyst can berun for 140 h without obvious deactivation. Based on the results of characterization, the poisonous CO adsorption on catalyst surface was the main reason for deactivation, and the catalyst regeneration was studied.
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