El-Bahy Zeinhom M, Mohamed Mohamed M, Zidan Farouk I, Thabet Mohamed S
Chemistry Department, Faculty of Science, Al-Azhar University, Nasr City, Cairo, Egypt.
J Hazard Mater. 2008 May 1;153(1-2):364-71. doi: 10.1016/j.jhazmat.2007.08.060. Epub 2007 Aug 28.
Co-ZSM-5 catalysts with different Co-loadings (2-30wt.%) were prepared by incipient wetness impregnation method. The prepared solid catalysts were characterized by X-ray diffraction, FTIR, in situ FTIR of pyridine adsorption and surface area measurements. The XRD data presented disintegration in the zeolitic crystalline structure accompanied by an increase in particle size of the prepared solids. New phases, Co(3)O(4) and Co(2)SiO(4), were detected with increasing the Co-loading, which indicate the strong interaction of cobalt ions with the ZSM-5 zeolite. FTIR study proved the presence of Co ions in stabilized sites inside the ZSM-5 framework. The in situ FTIR of adsorbed pyridine determined the type and relative strength of acidity on the surface of the prepared solids. The acidity switched from B-acid sites to L-acid sites with impregnation of cobalt ions in ZSM-5 zeolite. The acidity decreased with increasing Co-loading, which might be due to the destruction of zeolite framework and presence of new phases such as cobalt silicate and cobalt oxide on the surface. The surface texture characteristics changed with the promotion of ZSM-5 by cobalt ions, since a decrease of surface area, mean pore radius and pore volume was observed. The assessment of the catalytic activity was performed by the use of the photo-degradation of acid green (AG) dye as a probe reaction in presence of H(2)O(2) as an oxidant. The pH value controlled the degradation rate since a gradual increase of AG degradation rate was observed with increasing pH value and the optimum H(2)O(2) concentration was 61.6 mmol/l. It was found that, the AG degradation rate increased until an optimum value of Co-loading (ca. 10 wt.%), beyond which a monotonic decrease of reaction rate was recognized. The experimental data pointed to the importance of both the cobalt moieties and the zeolite framework structure in the AG degradation reaction.
采用初湿浸渍法制备了不同钴负载量(2-30wt.%)的Co-ZSM-5催化剂。通过X射线衍射、傅里叶变换红外光谱、吡啶吸附原位傅里叶变换红外光谱和表面积测量对制备的固体催化剂进行了表征。XRD数据显示,所制备固体的沸石晶体结构发生分解,同时粒径增大。随着钴负载量的增加,检测到新相Co(3)O(4)和Co(2)SiO(4),这表明钴离子与ZSM-5沸石存在强相互作用。傅里叶变换红外光谱研究证明ZSM-5骨架内稳定位点存在钴离子。吸附吡啶的原位傅里叶变换红外光谱确定了所制备固体表面酸性的类型和相对强度。随着钴离子浸渍到ZSM-5沸石中,酸性从B酸位点转变为L酸位点。酸性随钴负载量的增加而降低,这可能是由于沸石骨架的破坏以及表面存在新相如硅酸钴和氧化钴。由于观察到表面积、平均孔径和孔体积减小,钴离子对ZSM-5的促进作用使表面织构特征发生了变化。以酸性绿(AG)染料的光降解为探针反应,在以H(2)O(2)为氧化剂的条件下评估催化活性。pH值控制降解速率,因为随着pH值的增加,AG降解速率逐渐增加,最佳H(2)O(2)浓度为61.6 mmol/l。发现AG降解速率一直增加到钴负载量的最佳值(约10 wt.%),超过该值后反应速率单调下降。实验数据表明钴部分和沸石骨架结构在AG降解反应中都很重要。