铁掺杂的介孔氧化硅复合物催化酮经贝克曼重排一步转化合成酰胺  

A one-step conversion of ketones to amides via Beckmann rearrangement catalyzed by iron-doped mesoporous silica complex

作　　者：陈婷婷[1] 洪欣悦 冯是燕 李雯 张祖磊[2] CHEN Ting-ting;HONG Xin-yue;FENG Shi-yan;LI Wen;ZHANG Zu-lei(Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology,College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,China;School of Biology and Chemical Engineering,Jiaxing University,Jiaxing 314001,China)

机构地区：[1]浙江省化工高效制造技术重点实验室,浙江大学化学工程与生物工程学院,浙江杭州310027 [2]嘉兴学院生物与化学工程学院,浙江嘉兴314001

出　　处：《高校化学工程学报》2020年第5期1196-1203,共8页Journal of Chemical Engineering of Chinese Universities

基　　金：浙江省科技厅分析测试项目(2018C37076)。

摘　　要：酰胺是一类常见的天然化合物和工业原料,广泛用于生产洗涤剂、润滑剂等产品,通过贝克曼(Beckmann)重排反应合成酰胺在工业上应用比较广泛,此过程使用的催化剂多为强酸,反应条件较为苛刻。为寻找更佳的催化体系,制备并表征了一种新型的铁掺杂介孔氧化硅催化剂,考察了该催化剂对二苯甲酮和盐酸羟胺经Beckmann重排在无溶剂条件下一步生成N-苯基苯甲酰胺的催化效果。实验结果表明2 mmol二苯甲酮用40 mg催化剂,在130℃下反应1 h,酰胺产率可达到95%。考察了该催化剂对不同底物的适用性,结果表明,该催化剂对邻甲基苯乙酮、对甲氧基苯乙酮等催化产率均达到80%以上。通过回收再生,该催化剂经6次循环后仍具有良好的催化活性。Amides are common natural compounds and industrial raw materials,which are widely used in the production of detergents,lubricants and other products.The production of amides from ketones via Beckmann rearrangement is an extensive method in industry.However,strong acids are generally used as catalysts in this process that results in harsh reaction conditions.In order to explore a better catalytic system,a new iron-doped mesoporous silica catalyst was prepared and characterized,and its catalytic effect for Beckmann rearrangement of diphenylketone and hydroxylamine hydrochloride to produce N-phenylbenzamide in one-step and solvent-free method was investigated.The results show that the yield of amide can reach 95%when 2 mmol benzophenone reacted for 1 h at 130℃in the presence of 40 mg catalyst.Subsequently,various ketones were employed as the substrates to explore the scope and limitation of this catalyst,and the results show that the yield of corresponding amides are both over 80%for o-methylacetophenone and p-methoxyacetophenone.Furthermore,the catalyst still had good catalytic performance after reused for six times.

关 键 词：BECKMANN重排 N-苯基苯甲酰胺 介孔复合催化剂 高效 循环再生 

分 类 号：TQ465.92[化学工程—制药化工]