臺灣大學: 化學研究所鄭淑芬李珍燕Lee, Jan-YenJan-YenLee2013-04-112018-07-102013-04-112018-07-102012http://ntur.lib.ntu.edu.tw//handle/246246/257451SBA-15的介孔洞材料比起其他介孔材料M41S引起更大的注意力,主要是SBA-15材料具有較大的孔洞半徑和較高的熱穩定性。 這些介孔材料若應用在吸附和催化上,為了有更好的分子擴散和質傳效果,考慮SBA-15材料的形態是很重要的。根據Zhao等人原始文獻報導,其SBA-15具有六角排列的孔洞;以及數微米長度的纖維狀孔道。同一團隊,稍後藉著加入KCl 或NaCl 合成出棒狀型態 (1- 2微米) 的 SBA-15材料。 最近,具有短通道 (次微米) 的SBA-15已被合成出。此類短通道的材料,對於較大的染料分子吸附和酵素的固定化有很好的效能。 純的二氧化矽骨架的介孔材料沒有甚麼活性,但是將有機官能基導入通道內,可形成功能化介孔材料而改善介孔材料性能。有兩種常用的修飾法1.共聚合法 2. 後嫁接法, 共聚合法因為步驟少方法簡便,且可使官能基均勻分散於孔道內;不會堵塞洞口。 本論文是利用中性交聯共聚物P123為模板試劑,共聚合法合成一系列功能化的SBA-15材料,並用於吸附水中的污染物的研究。 第一部分,合成不同型態的胺基官能基SBA-15材料 ( NH2-SBA-15)和扁平狀SBA-15修飾不同官能基,如:甲基 (Me-), 苯基 (Ph- ), 胺基 (-(CH)3NH2)材料,用於吸附兩種酸性染料 (acid red Moo, acid orange AO12), 研究吸附量或吸附速率如何受吸附的狀態影響,例如:吸附劑種類,官能基含量, 溶液PH值,溫度等, 進一步計算出其熱力和動力學數據。 因為很多的工廠排放出廢棄液,內含很多重金屬離子而危害人類的健康,所以這方面的議題愈來愈重要。故論文第二部分是:合成一系列修飾 胺基- (NH2-), 硫醇基 (SH-), 和Schiff鹼性基的SBA-15材料用於吸附水中的Cu2+ 和Pb2+兩離子。同樣的,探討其吸附性質,並試圖用硬軟酸鹼理論 (HSAB theory) 說明實驗的結果。The SBA-15 material has attracted great attention in compared with other mesoporous silica such as M41S, due to its relatively large pore diameter (5-8 nm) and better hydrothermal stability. For better molecular diffusion and mass transfer inside the pores during the applications in adsorption and catalysis, the morphology of SBA-15 is important. According to the original paper reported by Zhao et al., SBA-15 materials have fiber-like morphology and channeling pores in the micrometers length, parallel to the long axis of the fibers. The same group later synthesized SBA-15 materals with a rod-like morphology and average pore length of ca. 1-2 μm by adding salts such as KCl and NaCl. Recently, SBA-15 mesoporous silica with very short mesopore channels in the sub-micrometer scale have been synthesized. These short channeled SBA-15 materials offer great advantages in faster speed and larger capacity for adsorption of bulky molecules as well as in enzymes immobilization. To expand the applications in adsorption and catalysis, the functionalization of mesoporous silica with organic groups is important because of the inert nature of the silica surface. Two methods are commonly adapted to prepare organic functionalized SBA-15 materials: one-pot co-condensation or post-grafting method. The co-condensation method is often preferred over the post-grafting pathway because it minimizes processing steps and provides more uniform distribution of organic functionalities without blocking the entrance of the mesopores. This thesis focused on the preparations and adsorptive applications of functionalized mesoporous silica materials using co-polymer P123 as the pore-directing agent in acid condition. In the first part, the amino-functionalized SBA-15 (NH2-SBA-15) materials with different morphologies and the platelet SBA-15 with tailoring different agents are synthesized and used as adsorbents in adsorption of two different anionic dyes (acid red 73 and acid orange 12) in aqueous solutions. The adsorption behaviors of dyes are studied at different experimental conditions including morphologies of adsorbents, pH of solution, the effect of organic functional groups and the content of amino-functional groups on SBA-15 framework. The kinetic parameters are further calculated on amino-functionalized fibrous materials. Many industries such as textiles, mining, painting, electroplating, plumbing, Fertilizer, and battery manufacturing are charge their wastewater with various heavy metals such as Pb (II) and Cu (II) into the environment causing serious pollution problems and threatening people’s health. Therefore, removal of these heavy metals from industrial wastewater has been causing more and more attentions. In the second part, amino, thiol and other Schiff base-type groups were incorporated onto the SBA-15 network. Schiff base ligands are known as efficient chelating agent for many metals, easily prepared by condensation between aldehydes and amines. These functionalized SBA-15 materials were used as an adsorbent to investigate the behaviors in removing Cu2+ and Pb2+ from aqueous solutions. The hard and soft acids and bases (HSAB) theory was used to explain the experimental result.140 bytestext/htmlen-US平板狀SBA-15;SBA-15型態;官能基化SBA-15;酸性染料吸附;銅鉛離子吸附platelet-SBA-15;morphology of SBA-15;organic-functionalized-SBA-15;adsorption of acid dye;adsorption of copper and lead ions[SDGs]SDG2[SDGs]SDG11功能化之SBA-15介孔材料在吸附水中汙染物的應用研究Studies of Applying Functionalized Mesoporous SBA-15 in Adsorption of Pollutants in Waterthesishttp://ntur.lib.ntu.edu.tw/bitstream/246246/257451/1/index.html