Dougherty Troy A, Baker Richard T
EaStChem, School of Chemistry, University of St Andrews, St Andrews, Fife KY16 9ST, UK.
Nanomaterials (Basel). 2024 Apr 9;14(8):651. doi: 10.3390/nano14080651.
Four ceria-based mesoporous oxide materials were prepared using a new vacuum impregnation (VI) templating method developed by the authors, namely, vacuum-assisted nanocasting (VAN). Two hard templates (SBA-15 and KIT-6) were employed, and products with compositions CeO and CeGdO (CGO) were made with each. The desired fluorite phase and composition were confirmed by powder XRD and EDS. The product structures were characterised by XRD, TEM, gas physisorption and SAXS. All products contained ordered mesoporous material in high yields. The specific surface areas (SSAs) and pore volumes of the products were determined to be high and the pore size and pore spacings related well to the templates from which the materials were synthesised. The TEM studies confirmed that the samples had a 3D pore structure, with this being the negative of the original template. The target materials were not only produced in high yields, but also displayed a porous single-crystal morphology with non-linear lattice planes. The highest SSA values and pore volumes were reported for materials impregnated using the KIT-6 template and with the CGO composition. The results suggest that VAN is an excellent and reproducible method for producing ordered mesoporous cerias and has considerable potential for wider application. All the mesoporous products showed dramatically increased reducibility in TPR experiments compared with a high-SSA nanoparticulate ceria reference. This is very promising for their potential applications in oxidation catalysts and in fuel cell components.
作者采用一种新开发的真空浸渍(VI)模板法,即真空辅助纳米铸造(VAN),制备了四种基于二氧化铈的介孔氧化物材料。使用了两种硬模板(SBA - 15和KIT - 6),分别制备了组成为CeO和CeGdO(CGO)的产物。通过粉末XRD和EDS确认了所需的萤石相和组成。通过XRD、TEM、气体物理吸附和SAXS对产物结构进行了表征。所有产物都以高产率包含有序介孔材料。产物的比表面积(SSA)和孔体积测定结果较高,且孔径和孔间距与合成材料所用的模板有良好的对应关系。TEM研究证实样品具有三维孔结构,这是原始模板的负像。目标材料不仅高产率制备,而且呈现出具有非线性晶格平面的多孔单晶形态。使用KIT - 6模板且具有CGO组成的材料报道了最高的SSA值和孔体积。结果表明VAN是一种制备有序介孔二氧化铈的优秀且可重复的方法,具有广泛应用的巨大潜力。与高SSA纳米颗粒二氧化铈参比物相比,所有介孔产物在TPR实验中均表现出显著提高的还原度。这对于它们在氧化催化剂和燃料电池组件中的潜在应用非常有前景。