碳球为模板水热合成Mg-Co复合氧化物及其催化分解N_2O（英文）  

Catalytic decomposition of N_2O over Mg-Co composite oxides hydrothermally prepared by using carbon sphere as template

作　　者：郑丽[1] 李和健 徐秀峰[1] ZHENG Li;LI He-jian;XU Xiu-feng(School of Chemistry and Chemical Engineering , Institute of Applied Catalysis, Yantai University, Yantai 264005, Chin)

机构地区：[1]烟台大学化学化工学院应用催化研究所,山东烟台264005

出　　处：《燃料化学学报》2018年第5期569-577,共9页Journal of Fuel Chemistry and Technology

基　　金：supported by the Shandong Provincial Natural Science Foundation(ZR2017MB020);Graduate Innovation Foundation of Yantai University(GIFYTU)

摘　　要：用自制的碳球为模板剂,尿素为沉淀剂,120℃水热合成尖晶石型Mg-Co复合氧化物(MgCo_2O_4),在其表面浸渍K_2CO_3溶液制得K改性催化剂,用于催化分解N2O。用X射线衍射(XRD)、N2物理吸附-脱附、扫描电镜(SEM)、H2程序升温还原(H2-TPR)、O2程序升温脱附(O2-TPD)、X射线光电子能谱(XPS)等技术对催化剂进行结构表征,考察了钴镁离子/碳球的质量比、尿素/钴镁离子的物质的量比等制备参数对催化剂活性的影响。结果表明,钴镁离子/碳球的质量比为0.192、尿素/钴镁离子的物质的量比为2,制得的MgCo_2O_4催化剂活性较高。K改性MgCo_2O_4催化剂在400℃有氧无水、有氧有水条件下连续反应50 h,N2O转化率分别保持在91%和62%,稳定性较好。MgCo2O4 composite oxides with spinel structure were hydrothermally prepared at 120 ℃ by using carbon sphere as template and urea as precipitant. K2CO3 solution was impregnated on MgCo2O4 and the K-modified catalyst was obtained. These catalysts were applied in catalytic decomposition of N2O and characterized by X-ray diffraction（ XRD）,nitrogen physisorption,scanning electron microscopy（ SEM）,temperature-programmed reduction of hydrogen（ H2-TPR）,temperature-programmed desorption of oxygen（ O2-TPD）,and X-ray photoelectron spectroscopy（ XPS）. Effect of catalysts preparation parameters such as mass ratio of cobalt and magnesium to carbon sphere,molar ratio of urea to metallic cations,on their catalytic activity was investigated. It is shown that the catalyst prepared with mass ratio 0.192 of cobalt and magnesium to carbon sphere,molar ratio 2 of urea to cobalt and magnesium cations,exhibits higher catalytic activity than others. Furthermore,91% and 62% conversions of N2O could be reached over 0.02 K/MgCo2O4 catalyst at 400 ℃ after continuous running for 50 h under the atmosphere of oxygen-alone and oxygen-steam together,respectively,revealing that K-modified MgCo2O4 catalyst is stable under both reaction atmospheres.

关 键 词：N2O催化分解 Mg-Co复合氧化物 K改性催化剂 催化活性 

分 类 号：O643.3[理学—物理化学]