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In-situ mesoporous silica pillared clay synthesis and effect of titanium and iron incorporation to structural properties
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2020-05-22 , DOI: 10.1016/j.micromeso.2020.110342
B. Yeter Dincer , S. Balcı , F. Tomul

Standard Wyoming SWy-2 mineral as a clay source was modified by use of cetyltrimethylammonium bromide as surfactant before Silica Pillared Clays (SPCs) synthesis, while octylamine (OA) was chosen as an auxiliary surfactant. Using tetraethyl orthosilicate as a silica source by ranging silica/modified clay (Si/C+) molar ratio within 20–150, SPC supports were synthesized keeping OA/C+ molar ratio as 20. Hydrothermal syntheses of titanium and iron containing SPC catalysts were carried out with M/Si molar ratios in between 0.03 and 0.15. Structural characterization results explained well the proposed mechanism for formation of MCM-41 like silica pillars between clay layers. With an increase of (001) peak reflection yielding basal spacing values up to 6.9 nm, polycrystalline structure observed in XRD patterns was confirmed by TEM images in SPCs. TEM also showed silica phase formations between clay bundles. Structural properties at Si/C+ molar ratio as 50 were the best with a surface area of 1874 m2/g. Titanium loading resulted in some decreases in surface area values while structural properties of iron incorporated catalyst at low iron content were found to be closer to that of the support. The highest Lewis and Brønsted acidities were observed by low titanium and iron incorporation to high silica containing support, respectively. TGA results showed that calcination temperature of 550 °C was sufficient for stable structures formation. ICP analysis and TEM images indicated that titanium species settled locally nearly 100% loading success and presence of titanium increased iron loading success. XPS results showed presences of TiO2 and mostly Fe2O3 forms.



中文翻译:

原位介孔二氧化硅柱状粘土的合成及其结合钛和铁对结构性能的影响

在合成硅石柱状粘土(SPC)之前,通过使用十六烷基三甲基溴化铵作为表面活性剂对标准的怀俄明SWy-2矿物作为粘土源进行了改性,同时选择了辛胺(OA)作为辅助表面活性剂。使用原硅酸四乙酯作为二氧化硅源,通过使二氧化硅/改性粘土(Si / C +)的摩尔比在20-150之间可以合成SPC载体,同时保持OA / C +摩尔比为20。含钛和铁的SPC催化剂的水热合成,其M / Si摩尔比为0.03至0.15。结构表征结果很好地说明了提出的在粘土层之间形成MCM-41像二氧化硅柱的机理。随着(001)峰反射的增加,产生的基距值高达6.9 nm,通过SPC中的TEM图像证实了XRD图中观察到的多晶结构。TEM也显示出粘土束之间的二氧化硅相形成。Si / C +摩尔比为50时的结构性能最佳,表面积为1874 m 2/G。钛负载导致表面积值的一些降低,而发现低铁含量下掺铁催化剂的结构性能更接近载体。通过将低钛和低铁掺入到高二氧化硅含量的载体中,可以观察到最高的Lewis和Brønsted酸度。TGA结果表明550℃的煅烧温度足以形成稳定的结构。ICP分析和TEM图像表明,钛物种在当地的沉降成功率接近100%,钛的存在增加了铁的负载成功率。XPS结果表明存在TiO 2和大部分为Fe 2 O 3形式。

更新日期:2020-06-29
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