铁改性石墨相氮化碳催化苯酚羟基化反应合成二酚  

Hydroxylation of Phenol to Produce Dihydroxybenzene Catalyzed by Iron Modified Graphitic Carbon Nitride

作　　者：张力嫱 高陆玺 吕雪川[1] 焦玉娟[1] 高肖汉[1] 曹月坤[1] ZHANG Liqiang;GAO Luxi;L Xuechuan;JIAO Yujuan;GAO Xiaohan;CAO Yuekun(School of Chemistry and Material Science,College of Chemistry,Chemical Engineering and Environmental Engineering,Liaoning Shihua University,Fushun 113001,China)

机构地区：[1]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

出　　处：《石油学报（石油加工）》2020年第2期403-409,共7页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：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N 2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-C3N 4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。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-C3N4 were 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.

关 键 词：苯酚羟基化 过氧化氢 绿色化学 石墨相氮化碳(g-C 3N 4) Fe/g-C 3N 4 

分 类 号：O625.3[理学—有机化学]