微波辅助异丁烯选择氧化催化剂的合成及构效关系  

Synthesis and structure-activity mechanism of tert-butanol selective oxidation catalysts by a microwave-assisted method

作　　者：袁巧 张文忠 阎梁 谷甜甜 王磊 任万忠 田晖 Yuan Qiao;Zhang Wenzhong;Yan Liang;Gu Tiantian;Wang Lei;Ren Wanzhong;Tian Hui(College of Chemistry and Chemical Engineering,Yantai University,Yantai 264000,Shandong,China;Weifang Xingxing United Chemical Co.,Ltd.,Weifang 261000,Shandong,China;Shandong Key Laboratory of Chemical Engineering and Process,Yantai 264000,Shandong,China)

机构地区：[1]烟台大学化学化工学院,山东烟台264000 [2]潍坊星兴联合化工有限公司,山东潍坊261000 [3]山东省化学工程与过程重点实验室,山东烟台264000

出　　处：《工业催化》2023年第11期42-49,共8页Industrial Catalysis

基　　金：山东省重大科技创新工程项目(2021ZDSYS24);烟台市科技创新发展计划(2020XDRH100)。

摘　　要：采用微波水热法制备了Mo-Bi系催化剂,并用于催化异丁烯(IB)选择氧化制备甲基丙烯醛(MAL)反应。通过X射线粉末衍射(XRD)、拉曼光谱(Raman)、扫描电子显微镜(SEM)、程序升温还原(H_(2)-TPR)等对催化剂进行表征,结果表明,制备的催化剂中含有Co_(6)Fe_(4)Mo_(12)Bi_(1.5)O x、CoMoO_(4)、MoO_(3)以及FeMoO_(4)等晶相。通过改变微波水热制备时间和温度探究其对催化剂性能的影响,结果表明,制备时间对催化剂颗粒形貌及组分影响较大,随着时间的延长,催化剂颗粒团聚加剧,由纳米颗粒到微米棒状颗粒转化,同时生成更多的Co_(6)Fe_(4)Mo_(12)Bi_(1.5)O x活性相。此外,微波水热制备温度为160℃对活性相形成最为有利,在此温度下,制备时间为90 min和120 min的催化剂表现出了良好的催化性能,异丁烯转化率和甲基丙烯醛选择性都在90%以上。A series of Mo-Bi catalysts were prepared by a microwave-assisted hydrothermal method for the oxidation reaction of isobutene(IB)to methacrolein(MAL).The catalysts were characterized by XRD,Raman,SEM and H_(2)-TPR methods to determine Co_(6)Fe_(4)Mo_(12)Bi_(1.5)Ox,CoMoO_(4),MoO_(3)and FeMoO_(4)crystalline phases.The researches focus on the effects of preparation time and temperature on catalysis performance.Results showed that the catalyst particle morphology and composition were greatly affected by the preparation time.With the extension of preparation time,the agglomeration of catalyst particles was intensified,and the nanoparticles were transformed into micron rod-like particles,and more Co_(6)Fe_(4)Mo_(12)Bi_(1.5)O x was generated at the same time.In addition,the preparation temperature of 160℃was the most favorable for the formation of active phase.At the temperature,the catalysts prepared for 90 min and 120 min showed good catalytic performance,and the conversion of IB and the selectivity of MAL were both more than 90%.

关 键 词：催化剂工程 微波水热法 Co_(6)Fe_(4)Mo_(12)Bi_(1.5)Ox Mo-Bi系催化剂 构效关系 

分 类 号：O643.36[理学—物理化学] TQ426.6[理学—化学]