具羧酸官能基三維結構中孔洞材料製備含釕金屬及銅鎳金屬奈米顆粒之催化應用

Please use this identifier to cite or link to this item: http://ir.lib.ncu.edu.tw/handle/987654321/80393

Title:	具羧酸官能基三維結構中孔洞材料製備含釕金屬及銅鎳金屬奈米顆粒之催化應用
Authors:	夏國書;Hsia, Kuo-Shu
Contributors:	化學學系
Keywords:	中孔洞材料;金屬奈米顆粒;有機汙染物降解;產氫
Date:	2019-07-23
Issue Date:	2019-09-03 14:28:20 (UTC+8)
Publisher:	國立中央大學
Abstract:	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.
Appears in Collections:	[Graduate Institute of Chemistry] Electronic Thesis & Dissertation

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