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Chemical modification of metal oxide carrier's surfaces with a silane coupling agent and an application of the method to catalyst preparation

机译:硅烷偶联剂对金属氧化物载体表面的化学改性及其在催化剂制备中的应用

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Several metal oxides were modified with γ-anilinopropyltrimethoxysilane (AnPS). Variations in the physicochemical properties with the modification were investigated in detail. The adsorptivity of 12-tungstophosphate anion (PW12) was shown to be greatly improved in the carriers such as SiO_2, TiO_2, and Al_2O_3, which are porous and have a high surface area, but it was not increased in SnO_2 and MgO, which have a small surface area and a high isoelectric point. With TiO_2-carrier, quantitative studies on the adsorptivity were carried out further, and the interaction modes of PW12 on the AnPS-modified surfaces were discussed based on FT-IR and XPS analyses. The isotherm attained quite steeply to a monomolecular layer of PW12. The FT-IR bands ascribed to the anilino group deformed considerably and the N1s-peak in XPS shifted along with the PW12-adsorption. From the findings it was strongly suggested that PW12 was effectively fixed through an acid-base interaction on the AnPS-TiO_2. Catalytic activity of PW12 fixed on AnPS-TiO_2 for 2-propanol dehydration as a test reaction were examined; in the pretreatment at 300 ℃ the activity was limited to a low level but after the treatment at 450 ℃ it increased in proportion to the PW12-loading on the AnPS-TiO_2 surfaces. Thus, it was inferred that PW12 was quite regularly dispersed over the modified surface. In conclusion, it is suggested that the modification technique is applicable to the preparation of a metal oxide-supported heteropolyacid catalyst.
机译:几种金属氧化物用γ-苯胺基丙基三甲氧基硅烷(AnPS)改性。对该修饰物理化性质的变化进行了详细研究。结果表明,在多孔且具有高表面积的SiO_2,TiO_2和Al_2O_3等载流子中,12钨磷酸盐阴离子(PW12)的吸附性得到了极大的改善,但在SnO_2和MgO中却没有增加小表面积和高等电点。以TiO_2为载体,对吸附性进行了定量研究,并通过FT-IR和XPS分析讨论了PW12在AnPS改性表面上的相互作用方式。等温线非常陡峭地达到了PW12的单分子层。归因于苯胺基基团的FT-IR谱带发生了很大的变形,并且XPS中的N1s峰随着PW12的吸附而移动。根据这些发现,强烈暗示PW12通过酸碱相互作用有效地固定在AnPS-TiO_2上。测试了固定在AnPS-TiO_2上的PW12对2-丙醇脱水的催化活性,作为测试反应。在300℃的预处理中,活性被限制在较低的水平,但在450℃的处理后,活性与AnPS-TiO_2表面上PW12的负载成正比。因此,推断出PW12非常规则地分散在改性表面上。总之,建议该改性技术可用于制备金属氧化物负载的杂多酸催化剂。

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