无溶剂条件下Co-NC选择性氧化乙苯制备苯乙酮  

Co-NC selective oxidation of ethylbenzene into acetophenone under solvent-free conditions

作　　者：王彦召 苗馨戈 王艳涛 杨维冉 WANG Yanzhao;MIAO Xinge;WANG Yantao;YANG Weiran(Key Laboratory of Poyang Lake Environment and Resources Utilization,Ministry of Education,Nanchang University,Nanchang 330047,China;School of Resources,Environmental and Chemical Engineering,Nanchang University,Nanchang 330031,China)

机构地区：[1]南昌大学鄱阳湖环境与资源利用教育部重点实验室,江西南昌330047 [2]南昌大学资源环境与化工学院,江西南昌330031

出　　处：《南昌大学学报（工科版）》2021年第3期210-216,275,共8页Journal of Nanchang University(Engineering & Technology)

基　　金：江西省博士后择优资助项目(2020KY40)。

摘　　要：通过调节合成溶剂和温度,制备了4种钴基沸石咪唑酯骨架结构化合物——ZIF-67,并在不同温度下碳化得到了一系列Co-NC催化剂。在无溶剂条件下考察了催化剂选择性氧化乙苯制备苯乙酮的催化活性,持续供氧条件下苯乙酮生产效率达143.7 mmol·g^(-1)·h^(-1)。通过HRTEM、XRD和XPS表征探讨了催化剂活性与其结构的关系。研究表明低温碳化的Co-NC催化剂金属纳米颗粒更小且均匀,吡啶氮含量更高,这可能是其催化乙苯氧化活性更高的原因。Four kinds of metal organic frameworks ZIF-67 were prepared by adjusting the synthetic solvent and temperature,and a series of Co-NC catalysts were obtained through carbonization of the ZIF-67 at different temperature.The catalytic activity of these catalysts for the selective oxidation of ethylbenzene to acetophenone was tested under solvent-free conditions,the productivity of acetophenone achieved 143.7 mmol·g^(-1)·h^(-1)under continuous oxygen supply conditions.The relationship of the catalysts activity and their structure was discussed based on HRTEM,XRD and XPS characterization,which suggested that Co-NC catalysts obtained by lower temperature carbonization possessed smaller and uniform metal nanoparticles,and higher pyridinic N content,which probably attribute to its higher catalytic activity for ethylbenzene oxidation.

关 键 词：ZIF-67 Co催化剂 乙苯氧化 苯乙酮 无溶剂反应 

分 类 号：O622[理学—有机化学]