Ce0.50Zr0.50O2中掺杂M(M = Mn,Y)对乙酸乙酯燃烧催化剂MnOx/Ce0.50-zZr0.50-zM2zOy/Al2O3性能的影响

doi:10.3866/PKU.WHXB201205173

物理化学学报 >> 2012, Vol. 28 >> Issue (08): 1936-1942.doi: 10.3866/PKU.WHXB201205173

Ce_0.50Zr_0.50O₂中掺杂M(M = Mn,Y)对乙酸乙酯燃烧催化剂MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/Al₂O₃性能的影响

曹红岩, 王健礼, 闫生辉, 刘志敏, 龚茂初, 陈耀强

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

收稿日期:2012-04-27 修回日期:2012-05-16 发布日期:2012-07-10
通讯作者: 陈耀强 E-mail:nic7501@scu.edu.cn
基金资助:
国家自然科学基金(2077309、20803049)资助项目

Effect of Doping M (M = Mn, Y) into Ce_0.50Zr_0.50O₂ on the Properties of MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/Al₂O₃ for Catalytic Combustion of Ethyl Acetate

CAO Hong-Yan, WANG Jian-Li, YAN Sheng-Hui, LIU Zhi-Min, GONG Mao-Chu, CHEN Yao-Qiang

Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China

Received:2012-04-27 Revised:2012-05-16 Published:2012-07-10
Contact: CHEN Yao-Qiang E-mail:nic7501@scu.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20773090, 20803049).

摘要/Abstract

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MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/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MnO_x/Ce_0.40Zr_0.40Mn_0.10Y_0.10O_y/Al₂O₃ 性能最佳,完全转化温度为513K,且T_10% 和 T_100%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,MnO_x/Ce_0.40Zr_0.40Mn_0.10Y_0.10O_y/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。

关键词: VOCs, 催化燃烧, 乙酸乙酯, MnO_x, 铈锆固溶体, 掺杂

Abstract:

The effect of doping M (M = Mn,Y) into ceria-zirconia solid solutions on the activity of MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/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. MnO_x/Ce_0.40Zr_0.40Mn_0.10Y_0.10O_y/ Al₂O₃ has the best catalytic performance. The complete conversion temperature of ethyl acetate over the catalyst is 513K and the temperature range between T_10% and T_100% 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 MnO_x/Ce_0.40Zr_0.40Mn_0.10Y_0.10O_y/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 MnO_x dispersion on the support surface.

Key words: Volatile organic compounds, Catalytic combustion, Ethyl acetate, MnO_x, Ceria-Zirconia Solid solutions, Doping

MSC2000:

O643

曹红岩, 王健礼, 闫生辉, 刘志敏, 龚茂初, 陈耀强. Ce_0.50Zr_0.50O₂中掺杂M(M = Mn,Y)对乙酸乙酯燃烧催化剂MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/Al₂O₃性能的影响[J]. 物理化学学报, 2012, 28(08): 1936-1942.

CAO Hong-Yan, WANG Jian-Li, YAN Sheng-Hui, LIU Zhi-Min, GONG Mao-Chu, CHEN Yao-Qiang. Effect of Doping M (M = Mn, Y) into Ce_0.50Zr_0.50O₂ on the Properties of MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/Al₂O₃ for Catalytic Combustion of Ethyl Acetate[J]. Acta Phys. -Chim. Sin., 2012, 28(08): 1936-1942.

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Ce_0.50Zr_0.50O₂中掺杂M(M = Mn,Y)对乙酸乙酯燃烧催化剂MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/Al₂O₃性能的影响

Effect of Doping M (M = Mn, Y) into Ce_0.50Zr_0.50O₂ on the Properties of MnO_x/Ce_0.50-zZr_0.50-zM_2zO_y/Al₂O₃ for Catalytic Combustion of Ethyl Acetate

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