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SBA-15表面改性及其对介孔La0.8Sr0.2CoO3钙钛矿型催化剂结构和性能的影响
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关 键 词:SBA-15  表面改性  模板法  介孔La0.8Sr0.2CoO3  低温CO氧化  
收稿时间:2016-12-22

Surface Modification of SBA-15 and Its Effect on the Structure and Properties of Mesoporous La0.8Sr0.2CoO3
Xue-Hui HUANG,Xiao-Hui SHANG,Peng-Ju NIU. Surface Modification of SBA-15 and Its Effect on the Structure and Properties of Mesoporous La0.8Sr0.2CoO3[J]. Acta Physico-Chimica Sinica, 2017, 33(7): 1462-1473. DOI: 10.3866/PKU.WHXB201704103
Authors:Xue-Hui HUANG  Xiao-Hui SHANG  Peng-Ju NIU
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Abstract:Mesoporous SBA-15 with mesopore diameter up to 10.1 nm was prepared by a hydrothermal method, and was further functionalized to obtain different surface properties. Thus-prepared SBA-15 was employed as a template to synthesize rhombohedrally crystallized mesoporous La0.8Sr0.2CoO3 perovskite via a nanocasting method. The surface properties of the SBA-15 were adjusted by treatment with concentrated hydrochloric acid, trimethylchlorosilane (TMCS), and 3-aminopropyltriethoxysilane (APTES). A series of characterization techniques verified that all the synthesized templates possessed ordered two-dimensional hexagonal mesoporous structure, and the surface was successfully modified with methyl and amino groups. The mesoporous perovskite structure was formed in the samples and the surface properties of SBA-15 significantly influenced the structure and properties of La0.8Sr0.2CoO3 perovskite oxides. Wide-angle X-ray diffraction patterns suggested that the modified silica templates were conducive to the formation of pure perovskite frameworks with good crystallinity. The catalysts also possessed mesoporous structure, as confirmed by small-angle XRD patterns, high-resolution transmission electron microscopy images, and nitrogen adsorption analysis. Moreover, the La0.8Sr0.2CoO3 materials synthesized using surface-functionalized templates exhibited relatively higher catalytic activity and stability in CO oxidation. Complete CO conversion could be achieved at 140℃ using the thus-prepared La0.8Sr0.2CoO3 materials, and no significant loss in catalytic activity was observed after 100 h of on-stream reaction experiments. X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, and O2 temperature-programmed desorption experiments revealed that the existence of Co4+, Sr enrichment in the perovskite structure, and high content of adsorbed oxygen species play a critical role in the enhanced catalytic activity of the catalysts. We also proposed the possible reasons for the effect of surface properties of the silica templates on the structure and properties of the La0.8Sr0.2CoO3 nanomaterials.
Keywords:SBA-15  Surface modification  Template  Mesoporous La0.8Sr0.2CoO3  Low-temperature CO oxidation  
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