本篇論文分成兩個部分，第一部分為在鹼性環境下合成具有羧酸官能 基 中孔洞材料 SBA-1，簡稱 CS-1B-x，其中 x = [CES/(CES+TEOS)]。將合成好的材料 CS-1B-x含浸釕金屬離子前驅液，利用化學還原法將釕金屬離子還原成釕金屬奈米顆粒，形成金屬奈米顆粒的過程中，受到材料孔洞大小及官能基的影響，其金屬顆粒大小約在 2-4 nm間。再將含浸釕金屬奈米顆粒的材料應用於硼烷氨水解製氫反應中，在 Ru(1)-CS-1B-10時，達到最佳的催化活性，其 TOF值為 202.4 H2 mol/metal mol min、 活化能為 24.13 kJ/mol。 第二部分 為將 CS-1B-x含浸銅及鎳金屬離子前驅液，利用熱還原法將 金屬離子還原成金屬奈米顆粒。過程中，在鹼性環境下 (pH = 9) 吸附金屬離子，此時材料上的羧酸官能基 (COOH) 會 去離子化 形成負離子 ( 能夠有效吸附金屬離子進入材料中。將合成好的材料應用於 4-Nitrophenol之催化還原反應，將得到的數據帶入 Pseudo-first order得出反應速率常數 ，得知在銅及鎳的比例為 8 2時，達到最佳的催化活性，其反應速率 k值高達 205.3 s-1g-1。;I have two part in my study. In the first part, ruthenium Nanoparticles (Ru NPs) are successfully confined within the cage-type mesopores of cubic mesoporous silica nanoparticles (MSNs) SBA-1 (sample denoted as Ru(y)-CS-1B-x) functionalized with carboxylic acid (-COOH) groups. The Ru NPs were forms inside the pores of SBA-1 by using chemical reduction with aqueous solution of NaBH4 and NH3BH3. The synthesized Ru(y)-CS-1B-x materials were characterized by nitrogen adsorption-desorption isotherms, powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), solid-state 13C and 29Si MAS NMR spectroscopy. According to the TEM images, it can be known that particle size of Ru NPs is about 2-4 nm. The Ru(1)-CS-1B-10 catalyst exhibits high catalytic activity in the catalytic hydrogen generation through hydrolysis of NH3BH3. The turnover frequency of 202.4 H2 mol/metal mol min and activation energy of 24.13 kJ/mol. The remarkable activity for hydrolysis of NH3BH3 can be attributed to the ultra-small Ru NPs confined in mesoporous of SBA-1 MSNs. In the second part, the copper/nickel alloy incorporated in CS-1B-x (CuyNi10-y-CS-1B-x), Under alkaline condition (pH=9), the –COOH groups on the surface deprotonate and become –COO- group, with efficiently interact with Cu2+/Ni2+ cations and allow facile fabrication of Cu-Ni NPs. The CuyNi10-y-CS-1B-x were used for reduction of 4-nitrophenol, and the Cu8Ni2-CS-1B-10 shows high catalytic activity with the activity parameter of 205.3 (s-1gcat.-1). The synergistic effect between Cu and Ni plays an important role for reduction of 4-nitrophenol.
