焙烧温度对CuO在γ-Al2O3载体上的分散和催化CO完全氧化性能的影响

doi:10.3724/SP.J.1077.2008.00454

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焙烧温度对CuO在γ-Al₂O₃载体上的分散和催化CO完全氧化性能的影响

王哲, 赵曦, 万海勤, 朱捷, 刘斌, 董林

南京大学化学化工学院, 介观化学教育部重点实验室, 南京 210093

收稿日期:2007-07-23 修回日期:2007-10-11 出版日期:2008-05-20 网络出版日期:2008-05-20

Influence of Calcination Temperature on the Dispersion Behavior and CO Oxidation Properties of CuO/γ-Al₂O₃ Catalyst

WANG Zhe, ZHAO Xi, WAN Hai-Qin, ZHU Jie, LIU Bin, DONG Lin

Key Laboratory of Mesoscopic Chemistry of MOE, Department of Chemistry, Nanjing University, Nanjing 210093, China

Received:2007-07-23 Revised:2007-10-11 Published:2008-05-20 Online:2008-05-20

摘要/Abstract

摘要： 采用浸渍法制备了经不同温度焙烧的CuO/γ-Al₂O₃催化剂, 并通过BET、XRD、UV-DRS、H₂-TPR以及CO完全氧化反应, 研究了不同焙烧温度对CuO/γ-Al₂O₃催化剂中CuO组分的分散、还原和催化性质的影响. 结果表明: 当焙烧温度为450℃时, CuO在γ-Al₂O₃上的分散容量约为0.56mmol/100m²; 当焙烧温度达到750℃时, Cu²⁺同时占据γ-Al₂O₃载体(110)面上的八面体和四面体空位. 对于450℃焙烧的低CuO含量的样品, 在H₂-TPR结果中只观察到处于八面体空位的CuO物种的还原, 而经750℃焙烧的样品则同时观察到处于八面体和四面体空位的CuO物种的还原, 且处于八面体空位的CuO的还原会促进处于四面体空位的CuO的还原. 处于八面体空位的CuO在CO完全氧化反应中的活性要高于处于四面体空位的CuO.

关键词: CuO/γ-Al₂O₃, CO完全氧化反应, 焙烧温度

Abstract:

CuO/γ-Al₂O₃ samples were prepared by impregnating γ-Al₂O₃with an aqueous solution containing requisite amount of Cu(NO₃)₂. BET, XRD, UV-DRS, H₂-TPR and CO oxidation were employed to characterize the dispersion, reduction behavior and catalytic properties of CuO/γ-Al₂O₃ catalyst calcinated at different temperatures. The results indicate that the dispersion capacity of CuO on the surface of γ-Al₂O₃ is about 0.56mmol/100m² when it is calcinated at 450℃; while for the samples calcinated at 750℃, Cu²⁺ would occupy both the octahedral and tetrahedral vacant sites on the (110) plane of γ-Al₂O₃. For samples with low CuO loading amount, only the reduction peak of Cu²⁺ in octahedral coordination environment is observed in xxCu/Al-450 samples; while for xx Cu/Al-750 samples, the reduction peaks of Cu²⁺ in octahedral and tetrahedral coordination environment can be observed and the reduction of Cu²⁺ in octahedral coordination environment would promote the reduction of Cu²⁺ in tetrahedral coordination environment. The CO oxidation results indicate that the activity of dispersed CuO species in octahedral coordination environment is higher than that in tetrahedral coordination environment.

Key words: CuO/γ-Al₂O₃, CO oxidation, calcination temperature

中图分类号:

O643

王哲,赵曦,万海勤,朱捷,刘斌,董林. 焙烧温度对CuO在γ-Al₂O₃载体上的分散和催化CO完全氧化性能的影响[J]. 无机材料学报, DOI: 10.3724/SP.J.1077.2008.00454.

WANG Zhe,ZHAO Xi,WAN Hai-Qin,ZHU Jie,LIU Bin,DONG Lin. Influence of Calcination Temperature on the Dispersion Behavior and CO Oxidation Properties of CuO/γ-Al₂O₃ Catalyst[J]. Journal of Inorganic Materials, DOI: 10.3724/SP.J.1077.2008.00454.

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焙烧温度对CuO在γ-Al₂O₃载体上的分散和催化CO完全氧化性能的影响

Influence of Calcination Temperature on the Dispersion Behavior and CO Oxidation Properties of CuO/γ-Al₂O₃ Catalyst

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