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作 者:曹红岩[1] 王健礼[1] 闫生辉[1] 刘志敏[1] 龚茂初[1] 陈耀强[1]
机构地区:[1]四川大学化学学院,教育部绿色化学与技术重点实验室,成都610064
出 处:《物理化学学报》2012年第8期1936-1942,共7页Acta Physico-Chimica Sinica
基 金:国家自然科学基金(20773090,20803049)资助项目~~
摘 要:考察了乙酸乙酯催化燃烧时,铈锆固溶体中掺杂M(M=Mn,Y)对催化剂MnOx/Ce0.50-zZr0.50-zM2zOy/Al2O3活性的影响.结果表明:Mn的掺杂明显增加了储氧材料的储氧量(OSC),Y的掺杂明显降低了催化剂的还原温度;Mn和Y的同时掺杂兼具Mn掺杂和Y掺杂的优点.催化剂MnOx/Ce0.40Zr0.40Mn0.10Y0.10Oy/Al2O3性能最佳,乙酸乙酯完全转化温度为513K,且T10%和T100%间隔的温度范围最窄,可适用于较大初始浓度变化范围和较高空速(GHSV)条件下的乙酸乙酯净化.H2程序升温还原(H2-TPR)和X射线衍射(XRD)测试显示,MnOx/Ce0.40Zr0.40Mn0.10Y0.10Oy/Al2O3具有较低的还原温度和较大的还原峰面积;Mn和Y进入铈锆固溶体的晶格,改善了其织构性能,促进了锰氧化物在载体表面的分散.The effect of doping M (M = Mn,Y) into ceria-zirconia solid solutions on the activity of MnOx/Ce0.50-zZr0.50-zM2zOy/Al2O3 for catalytic combustion of ethyl acetate has been investigated. It is found that doping of Mn increases greatly the oxygen storage capacity (OSC) of the oxygen-storage materials (OSMs); doping of Y decreases obviously the reduction temperature of catalysts; the doping of Mn and Y combines the advantages of doping of Mn and Y. MnOx/Ce0.40Zr0.40Mn0.10Y0.10Oy/ Al2O3 has the best catalytic performance. The complete conversion temperature of ethyl acetate over the catalyst is 513K and the temperature range between T10% and T100% is the smallest. This catalyst can be applied to abatement of ethyl acetate under conditions of wider range of inert concentration and higher gas hourly space velocity (GHSV). Results of H2-temperature-programmed reduction(H2-TPR)and X-ray diffraction (XRD) analyses show that MnOx/Ce0.40Zr0.40Mn0.10Y0.10Oy/Al2O3 has lower reduction temperature and larger peak area. Mn and Y enter the lattice of ceria-zirconia solid solutions, which improves the textural properties and greatly promotes the MnOx dispersion on the support surface.
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