不同Cu负载量Cu-ZSM-5催化剂上正丁胺的选择催化氧化性能  

SELECTIVE CATALYTIC OXIDATION PERFORMANCE OF N-BUTYLAMINE OVER Cu-ZSM-5 CATALYSTS WITH DIFFERENT COPPER LOADINGS

作　　者：邢欣 李娜 程杰 XING Xin;LI Na;CHENG Jie(College of Environmental Science and Engineering,Taiyuan University of Science and Technology,Taiyuan 030024,China;National Engineering Laboratory for VOCs Pollution Control Material&Technology,Research Center for Environmental Material and Pollution Control Technology,University of Chinese Academy of Sciences,Beijing 101408,China)

机构地区：[1]太原科技大学环境科学与工程学院,太原030024 [2]中国科学院大学环境材料与污染控制技术研究中心挥发性有机物污染控制材料与技术国家工程实验室,北京101408

出　　处：《环境工程》2022年第3期51-58,共8页Environmental Engineering

基　　金：太原科技大学博士科研启动基金(20202053);北京市科技计划课题(Z181100000118003);中央高校基本科研业务费专项资金。

摘　　要：采用等体积浸渍法制备不同Cu负载量(1%、2%、5%和10%)的系列Cu-ZSM-5催化剂,并考察了Cu负载量对催化剂的正丁胺催化氧化性能的影响。通过XRD、N_(2)吸脱附、EPR、H_(2)-TPR、NH_(3)-TPD表征方法对催化剂的晶相结构和物化性质进行表征并研究构效关系。结果表明:Cu负载量为10%的催化剂催化活性最高,在300℃下实现了正丁胺的完全转化;而Cu负载量为5%的催化剂N_(2)选择性最佳,低温时N_(2)选择性明显高于其他催化剂。表征结果表明,催化剂的氧化还原性能主要影响正丁胺的转化率,Cu负载量影响催化材料的氧化还原性能,Cu负载量高的催化剂氧化还原性能优异。高N_(2)选择性主要归属于催化剂孤立态Cu^(2+)物种和弱酸性位,催化剂的弱酸性位有利于正丁胺的吸附活化和深度氧化。A series of Cu-ZSM-5 catalysts with different Cu loadings(1%,2%,5% and 10%) were synthesized by equal volume impregnation method,and the effect of Cu loading on n-butylamine catalytic oxidation was investigated.The crystal structure and physicochemical properties of the catalysts were characterized by XRD,N_(2) adsorption desorption,EPR,H_(2)-TPR and NH_(3)-TPD,and the structure-activity relationship was studied.The catalyst with Cu loading of 10% had the highest catalytic activity,and the complete conversion of n-butylamine was achieved at 300 ℃.The catalyst with 5% Cu loading had the best N_(2) selectivity,and the N_(2) selectivity at low temperature was significantly higher than that of the other catalysts.The characterization results showed that the redox performance of the catalyst mainly affected the n-butylamine conversion,the different Cu loading affected the redox performance of the catalyst materials,and the catalyst with higher Cu loading had excellent redox performance.The high N_(2) selectivity could be attributed to the isolated Cu^(2+) species and the weak acid sites of the catalyst,which was conducive to the adsorption activation and deep oxidation of n-butylamine to form N_(2).

关 键 词：正丁胺 选择催化氧化 Cu-ZSM-5催化剂 铜物种 酸性 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]