氨基化多孔材料的制备及其吸附催化性能
发布时间:2018-05-21 17:23
本文选题:氨基功能化 + 多孔材料 ; 参考:《齐鲁工业大学》2015年硕士论文
【摘要】:氨基功能化的多孔材料在吸附、催化、分离等应用中表现出远优于未改性的多孔材料,使其应用价值得以提高,并且在一些新领域被广泛的应用。因此开发具有氨基功能的多孔材料备受关注。本论文将SBA-15和活性炭进行表面改性,制备出具有氨基基团的SBA-15和活性炭。同时,利用红外光谱、X射线衍射、热重、氮气吸脱附和环境扫描电子显微镜等测试方法对改性材料进行了表征。以正硅酸乙酯作为硅源,通过水热法合成出SBA-15。使用浓盐酸对SBA-15进行活化,活化后SBA-15表面的羟基相对含量增多。采用3-氨基丙基三乙氧基硅烷对活化过的SBA-15进行嫁接修饰,制备出具有氨基有机基团的SBA-15介孔材料。测试结果表明,氨基有机基团被成功的链接到SBA-15的表面,并保持了SBA-15原有的优良的结构性能,氨基功能化后氨基有机基团占总重比达到14%。二氧化碳程序升温脱附测试表明,氨基功能化的SBA-15具有氨基基团的优良性能,对二氧化碳的吸附强度是未修饰过的SBA-15的4倍。将活性炭在强氧化剂的溶液中进行氧化处理,制备出具有众多可修饰的含氧官能团的氧化活性炭。之后对氧化过的活性炭依次使用二氯亚砜和乙二胺处理,制备出氨基功能化的活性炭。测试结果表明,氨基有机基团被成功的嫁接到了活性炭的表面,氨基功能化的活性炭保持了活性炭原有的优良的结构性能,并且仍然具有良好的高热稳定性,氨基基团分解温度在430℃以上。采用浸渍还原法制备了氨基功能化的活性炭负载钯粒子的催化剂。通过X射线衍射测试表明,钯粒子完好的负载到其表面。建立了氨基功能化的活性炭作为固体载体的贵金属钯催化剂催化还原模型。以硝基苯作为催化还原对象,硼氢化钠为还原剂,测试结果表明,在8分钟内,99%硝基苯转换为苯胺。测试了催化剂重复使用性,实验结果表明,此催化剂在5个循环周期中的使用都可以使硝基苯的转化率达到99%。此外,对氨基功能化的活性炭吸附钯离子的性能进行研究,结果表明,固体载体的高吸附量能有利于提高催化剂的催化效率。
[Abstract]:Amino-functionalized porous materials are much better than unmodified porous materials in adsorption, catalysis, separation and so on, and have been widely used in some new fields. Therefore, the development of porous materials with amino function has attracted much attention. In this paper, the surface modification of SBA-15 and activated carbon was carried out to prepare SBA-15 and activated carbon with amino groups. At the same time, the modified materials were characterized by infrared X-ray diffraction, thermogravimetry, nitrogen adsorption and desorption, and environmental scanning electron microscopy. SBA-15 was synthesized by hydrothermal method using ethyl orthosilicate as silicon source. SBA-15 was activated by concentrated hydrochloric acid, and the relative content of hydroxyl groups on the surface of SBA-15 increased after activation. SBA-15 mesoporous materials with amino organic groups were prepared by grafting the activated SBA-15 with 3-aminopropyl triethoxy silane. The results showed that the amino organic group was successfully linked to the surface of SBA-15 and maintained the original excellent structure and performance of SBA-15. The ratio of amino organic group to total weight reached 14% after amino functionalization. The temperature programmed desorption test of carbon dioxide showed that the amino functionalized SBA-15 had excellent properties of amino group and the adsorption intensity of carbon dioxide was 4 times as much as that of unmodified SBA-15. The activated carbon was oxidized in the solution of strong oxidant, and the oxidized activated carbon with many modified oxygen functional groups was prepared. The oxidized activated carbon was then treated with dichloro sulfoxide and ethylenediamine in order to prepare amino functionalized activated carbon. The results showed that the amino organic group was successfully grafted to the surface of the activated carbon, and the amino functionalized activated carbon maintained the original excellent structural properties of the activated carbon and still had good thermal stability. The decomposition temperature of amino group is over 430 鈩,
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