硫化CoMo/Al2O3催化剂上H2同时催化还原SO2和NO(Ⅰ)——催化剂的制备、表征及性能
Simultaneous Reduction of SO2 and NO by H2 over Sulfided CoMo/Al2O3 Catalyst(Ⅰ): Preparation, Characterization and Properties
作者单位
朱 鹏 上海应用技术学院上海 200235 
李雪辉 华南理工大学化学与化工学院广州 510640 
王芙蓉 华南理工大学化学与化工学院广州 510640 
王乐夫 华南理工大学化学与化工学院广州 510640 
摘要: 用浸渍法制备了CoMo/Al2O3催化剂,并对其进行了XRD、低温氮吸附-脱附和TPR表征。结果表明,随着Co负载量的增加,催化剂表面活性物种增加,但同时催化剂的比表面积和孔容逐渐减小;硫化后的催化剂比未经硫化处理的催化剂表面具有更多更易还原的活性物种。将所制得的催化剂硫化后用于NO分解和H2还原NO反应,NO均完全转化,但催化剂最终会因为晶格硫的大量流失而活性下降。在H2还原NO反应体系中,H2的存在使得催化剂晶格硫的流失速率极大变缓,催化剂活性下降较慢;在H2同时还原SO2和NO体系中,由于晶格硫能够得到外界源源不断的补充,因此,SO2和NO能同时在催化剂表面实现稳定的还原,反应温度、空速、进料气中H2的配比、催化剂中Co负载量以及硫化预处理方式对催化剂的活性有显著影响。活性测试结果表明,在500 ℃,空速12 000 h-1n(H2)/n(SO2+NO)=2时,5%Co10%Mo/Al2O3上SO2和NO转化率均为100%,单质硫产率达96.6 %。
关键词:     氧化铝  氢气  催化还原  二氧化硫  一氧化氮  废气处理
基金项目: 
Abstract: CoMo/Al2O3 catalysts were prepared by impregnation and characteized of XRD, low temperature nitrogen adsorption-desorption and TPR. The results showed that the active species on the surface of catalyst increased with the increasing of Co loadings, but at the same time, the specific surface area and pore volume decreased. There were more active species which could be reduced more easily on the surface of sulfided catalyst than that of the catalyst without sulfidation. The conversion of NO was 100% on sulfided catalyst for the reactions of both NO decomposition and reduction by H2, but the activity of the catalyst decreased ultimately because of the serious loss of lattice sulfur. While in the reaction of NO reduction by H2, the presence of H2 made the loss rate of lattice sulfur greatly slow down, and the catalytic activity decreased more slowly. In the reaction of simultaneous reduction of SO2 and NO by H2, steady conversion of SO2 and NO realized for continuous supply of lattice sulfur. The activity of the catalyst was influenced dramatically by reaction temperature, space velocity, H2 ratio, Co loading and sufiding method. When space velocity was 12 000 h-1 and n(H2)/n(SO2+NO)=2, at 500 ℃, the conversion of both SO2 and NO could reach 100 %, and the yield of sulfur was 96.6%.
Keywords: cobalt  molybdenum  alumina  hydrogen  catalytic reduction  sulfur dioxide  nitric oxide  waste gas treatment
 
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朱 鹏,李雪辉,王芙蓉,王乐夫.硫化CoMo/Al2O3催化剂上H2同时催化还原SO2和NO(Ⅰ)——催化剂的制备、表征及性能[J].无机化学学报,2008,24(11):1837-1845.
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