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铁改性石墨相氮化碳催化苯酚羟基化反应合成二酚
引用本文:张力嫱,高陆玺,吕雪川,焦玉娟,高肖汉,曹月坤.铁改性石墨相氮化碳催化苯酚羟基化反应合成二酚[J].石油学报(石油加工),2020,36(2):403-409.
作者姓名:张力嫱  高陆玺  吕雪川  焦玉娟  高肖汉  曹月坤
作者单位:辽宁石油化工大学 化学化工与环境学部 化学与材料学院, 辽宁 抚顺 113001
基金项目:基金项目: 国家自然科学基金项目(21003069,21103078)资助
摘    要:石墨相氮化碳(g-C3N4)以其独特的电子结构和化学特性引起了广泛关注。以双氰胺和硝酸铁为原料,制备了Fe改性的石墨相氮化碳(Fe/ g-C3N4),采用红外光谱、XRD和N2吸附-脱附等分析手段对g-C3N4和 Fe/g-C3N4 进行了表征,并用以催化苯酚羟基化反应合成二酚,研究了Fe/ g-C3N4催化性能的影响因素。结果表明,Fe/ g-C3N4材料具有良好的介孔结构,Fe的引入改变了g-C3N4层状结构的层间距。当苯酚/H2O2摩尔比为2/1、铁负载量为0.7%(质量分数)、反应温度为50 ℃、反应时间为6 h时,苯酚的转化率达到39.7%,邻苯二酚和对苯二酚的总选择性为85.8%。重复实验结果证实该催化剂可以重复使用。

关 键 词:苯酚羟基化  过氧化氢  绿色化学  石墨相氮化碳(g-C3N4)  Fe/g-C3N4  
收稿时间:2018-12-17

Hydroxylation of Phenol to Produce Dihydroxybenzene Catalyzed by Iron Modified Graphitic Carbon Nitride
ZHANG Liqiang,GAO Luxi,LV Xuechuan,JIAO Yujuan,GAO Xiaohan,CAO Yuekun.Hydroxylation of Phenol to Produce Dihydroxybenzene Catalyzed by Iron Modified Graphitic Carbon Nitride[J].Acta Petrolei Sinica (Petroleum Processing Section),2020,36(2):403-409.
Authors:ZHANG Liqiang  GAO Luxi  LV Xuechuan  JIAO Yujuan  GAO Xiaohan  CAO Yuekun
Affiliation:School of Chemistry and Material Science, College of Chemistry, Chemical Engineering and Environmental Engineering,Liaoning Shihua University, Fushun 113001, China
Abstract:Graphitic carbon nitride (g-C3N4), possessing unique electronic and chemical properties, has attracted extensive attention from researchers. By using ferric nitrate and dicyandiamide as precursors, a series of Fe modified graphitic carbon nitride (Fe/ g-C3N4) were prepared and used for catalyzing the hydroxylation of phenol to dihydroxybenzene. Fe/ g-C3N4 and g-C3N4 were characterized by FT-IR spectra, XRD and N2 absorption-desorption isotherms. Effects of reaction conditions on the catalytic performance of Fe/ g-C3N4were studied. Results show that Fe/ g-C3N4 has uniform mesoporous structure and the layer spacing of g-C3N4 is changed after the introduction of Fe. Under optimized conditions, 39.7% phenol conversion and 85.8% catechol and hydroquinone selectivity are obtained, with Fe mass fraction of 0.7%, molar ratio of phenol to H2O2 of 2/1, reaction temperature of 50 ℃, and reaction time of 6 h. The reusability of the Fe/ g-C3N4 catalyst is very good by the recycling test.
Keywords:hydroxylation of phenol  hydrogen peroxide  green chemistry  graphitic carbon nitride (g-C3N4)  Fe/ g-C3N4  
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