The City College of New York and The Graduate School of CUNY, New York, NY 10031, USA.
J Hazard Mater. 2011 Dec 15;197:294-303. doi: 10.1016/j.jhazmat.2011.09.087. Epub 2011 Sep 29.
New silica-based composites were obtained using a slow precipitation of mixed oxide Ce(1-x)Zr(x)O(2) on the surface of mesoporous silica, SBA-15. The samples were tested as NO(2) adsorbents in dynamic conditions at room temperature. The surface of the initial and exhausted materials was characterized using N(2) sorption, XRD, TEM, potentiometric titration, and thermal analysis before and after exposure to NO(2). In comparison with unsupported Ce(1-x)Zr(x)O(2) mixed oxides, a significant increase in the NO(2) adsorption capacity was observed. This is due to the high dispersion of active oxide phase on the surface of SBA-15. A linear trend was found between the NO(2) adsorption capacity and the amount of Zr(OH)(4) added to the structure. Introduction of Zr(4+) cations to ceria contributes to an increase in the amount of Ce(3+), which is the active center for the NO(2) adsorption, and to an increase in the density of -OH groups. These groups are found to be involved in the retention of both NO(2) and NO on the surface. After exposure to NO(2), an acidification of the surface caused by the oxidation of the cerium as well as the formation of nitrite and nitrates took place. The structure of the composites appears not to be affected by reactive adsorption of NO(2).
采用混合氧化物 Ce(1-x)Zr(x)O(2)在介孔硅 SBA-15 表面的缓慢沉淀法制备了新型硅基复合材料。将这些样品作为 NO(2)吸附剂在室温下的动态条件下进行测试。在暴露于 NO(2)前后,使用 N(2)吸附、XRD、TEM、电位滴定和热分析对初始和耗尽材料的表面进行了表征。与未负载的 Ce(1-x)Zr(x)O(2)混合氧化物相比,观察到 NO(2)吸附容量有显著提高。这是由于活性氧化物相在 SBA-15 表面的高分散性所致。NO(2)吸附容量与添加到结构中的 Zr(OH)(4)量之间存在线性趋势。Zr(4+)阳离子引入到氧化铈中有助于增加 Ce(3+)的量,Ce(3+)是 NO(2)吸附的活性中心,并增加 -OH 基团的密度。这些基团被发现参与了表面上 NO(2)和 NO 的保留。暴露于 NO(2)后,铈的氧化以及亚硝酸盐和硝酸盐的形成导致表面酸化。复合材料的结构似乎不受 NO(2)的反应性吸附的影响。