Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, PR China.
J Colloid Interface Sci. 2012 Apr 15;372(1):63-72. doi: 10.1016/j.jcis.2012.01.014. Epub 2012 Jan 24.
The dispersion and physicochemical behaviors of CuO-CoO binary metal oxides supported on γ-Al(2)O(3) were characterized by XRD, LRS, XPS, H(2)-TPR, and in situ FT-IR techniques. Their activities were evaluated by NO-CO model reaction. The results indicated that (a) for lower loadings, CuO and CoO were able to be highly dispersed on the surface of γ-Al(2)O(3) support; (b) the interaction between dispersed CuO and CoO upon γ-Al(2)O(3) was discussed in the view of incorporation model. According to this model and obtained results, the surface dispersed Cu-O-Co species were considered to exist on the surface of γ-Al(2)O(3); (c) CO or/and NO adsorption FT-IR results evidenced that the surface dispersed copper species could be reduced to lower valence by CO and the NO adsorption species converted with the increase in the temperature; (d) the surface dispersed Cu-O-Co species could be reduced to active Cu-□-Co species by CO among the mixture atmosphere. The formation of the surface synergetic oxygen vacancy (SSOV) was a crucial factor in the process of the NO-CO reaction. And a possible reaction pathway was tentatively proposed to discuss the NO-CO reaction based on all of these results.
用 XRD、LRS、XPS、H₂-TPR 和原位 FT-IR 技术对负载在 γ-Al₂O₃ 上的 CuO-CoO 二元金属氧化物的分散性和物理化学行为进行了表征。通过 NO-CO 模型反应评价了它们的活性。结果表明:(a)在较低的负载量下,CuO 和 CoO 能够高度分散在 γ-Al₂O₃ 载体的表面;(b)根据嵌入模型讨论了分散在 γ-Al₂O₃ 上的 CuO 和 CoO 之间的相互作用。根据该模型和得到的结果,认为表面分散的 Cu-O-Co 物种存在于 γ-Al₂O₃ 的表面;(c)CO 或/和 NO 吸附 FT-IR 结果表明,表面分散的铜物种可以被 CO 还原为较低的价态,而随着温度的升高,NO 吸附物种会发生转化;(d)在混合气氛中,CO 可以将表面分散的 Cu-O-Co 物种还原为活性的 Cu-□-Co 物种。表面协同氧空位(SSOV)的形成是 NO-CO 反应过程中的一个关键因素。基于这些结果,提出了一种可能的反应途径来讨论 NO-CO 反应。