Cu-Zn-Al基催化剂制备及催化等离子体转化甲烷制甲醇  

Preparation of Cu-Zn-Al-Based Catalysts and their Application in Methane Conversion to Methanol by Plasma

作　　者：徐锋 李凡 朱丽华 李创 XU Feng;LI Fan;ZHU Li-hua;LI Chuang(School of Safety Engineering,Heilongjiang University of Science and Technology,Harbin 150022,China)

机构地区：[1]黑龙江科技大学安全工程学院,黑龙江哈尔滨150022

出　　处：《高校化学工程学报》2018年第4期869-876,共8页Journal of Chemical Engineering of Chinese Universities

基　　金：国家自然科学基金(51374098;51504087)

摘　　要：为了探讨催化剂对低温等离子体转化甲烷制甲醇的影响,将Cu-Zn-Al基催化剂引入介质阻挡放电系统,进行了甲烷等离子体-催化制甲醇的研究,考察了催化剂填装方式、催化剂载体、催化剂助剂对甲醇生成的影响。结果表明,将催化剂负载在堇青石蜂窝陶瓷上(Cu-Zn-Al/HC)的填装方式可获得较好的催化效果;堇青石表面结构对甲醇的生成具有显著影响,将催化剂负载在经酸蚀处理的堇青石蜂窝陶瓷上(Cu-Zn-Al/HC-AE),可使单位能耗甲醇产量提高28%;在催化剂中添加助剂Ce利于甲醇的生成,应用Cu-Zn-Al-Ce/HC-AE催化剂时,单位能耗甲醇最大产量较单纯等离子体体系提高了183.7%。基于等离子体-催化甲烷反应结果和发射光谱原位诊断,推断等离子体与催化剂协同转化甲烷制甲醇反应中甲醇通过自由基反应和费托合成两条途径生成。In order to investigate catalyst effects on methane conversion to methanol by low-temperature plasma, dielectric barrier discharge plasma combined with Cu-Zn-Al-based catalysts was applied. Effects of catalyst filling mode, catalyst carrier and catalyst auxiliaries on methanol formation were investigated. The results show that the catalyst loaded on cordierite honeycomb ceramics（Cu-Zn-Al/HC） exhibits excellent catalytic activity. The surface structure of cordierite has a significant effect on methanol formation. A Cu-Zn-Al/HC-AE catalyst was prepared by loading the Cu-Zn-Al catalyst on cordierite honeycomb ceramics after acid etching, and methanol productivity was increased by 28% per unit energy consumption. Addition of Ce into catalysts can facilitate methanol formation, and the maximum methanol productivity is increased by 183.7% compared with pure plasma system. The results of plasma-catalyst reaction and emission spectrum in situ diagnosis indicate that methanol is formed through approaches of free radical reaction and Fischer-Tropsch synthesis.

关 键 词：CU-ZN-AL 低温等离子体 介质阻挡放电 甲烷 甲醇 催化剂 

分 类 号：TQ223.1[化学工程—有机化工] TD712[矿业工程—矿井通风与安全]