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    請使用永久網址來引用或連結此文件: http://ir.lib.ncu.edu.tw/handle/987654321/73989


    題名: 三維結構具官能基之中孔洞材料製備含銀鎳合金奈米顆粒於催化之應用;Synthesis of Ag/Ni Alloy Nanoparticles Confined in Carboxylic Acid Functionalized Cubic SBA-1 Mesoporous Silica Nanoparticle as Efficient Catalysts for Reduction of 4-Nitrophenol and Degradation Reactions
    作者: 夏汝安;Hsia, Nu-An
    貢獻者: 化學學系
    關鍵詞: 中孔洞材料;銀鎳合金;4-硝基苯酚;染料降解;mesoporous material;Ag/Ni nanoparticle;4-nitrophenol;dye degradation
    日期: 2017-07-24
    上傳時間: 2017-10-27 12:57:43 (UTC+8)
    出版者: 國立中央大學
    摘要: 本論文主要分為兩部分,第一部分是利用陽離子型界面活性劑Hexadecyl pyridinium chloride (CPC) 及陰離子型高分子Poly(acrylic acid) (PAA) 為模板,在鹼性環境下合成具羧酸官能基之中孔材料SBA-1,簡稱為CS-1B-x,且x = [CES / (CES + TEOS) ],修飾官能基後,仍能保有SBA-1系列的Pm3n規則結構,接著將所合成CS-1B-x吸附金屬離子,可成功還原成銀奈米金屬顆粒以及銀鎳合金奈米顆粒在此中孔材料上。在形成金屬奈米粒子的過程中,能受到孔洞大小空間之限制以及羧酸官能基之影響,其尺寸約於3 – 10 nm之間。吸附奈米金屬後,CS-1B-x材料結構也無崩解的情形發生,可以發現銀奈米粒子最佳含浸量為0.3 mmol,而銀奈米顆粒的尺寸為3.2 nm。
    將此系列材料進一步應用於4-Nitrophenol之還原催化反應,並將催化數據帶入Pseudo-first order得出反應速率常數,可發現銀的奈米顆粒愈小,催化活性會有較好的表現;但當銀鎳比是6:4時其催化效果是最好的,其反應速率常數3.0 x 10-2 s-1,其催化反應在2-3分鐘便能結束。
    第二部分是將此含奈米金屬之中孔材料進行染料之催化降解反應,以Methyl orange以及Rhodamine B做為示範染料進行降解,可以發現Ag06Ni04-CS-1B-10對於Methyl orange的降解能力是最好的,反應速率常數為6.9 x 10-2 s-1;而Ag08Ni02-CS-1B-10對於Rhodamine B有最高的反應速率,其反應速率常數為2.7 x 10-2 s-1。結果顯示本實驗所製備之含奈米合金之中孔洞料對於染料降解也能有非常優異的催化活性。
    ;Silver nanoparticles (Ag NPs) with a particle size about 3 nm are successfully confined within the cage-type mesopores of cubic SBA-1 mesoporous silica nanoparticles (MSNs) functionalized with carboxylic acid (-COOH) groups (CS-1B-x). Under alkaline condition of pH 9, the –COOH groups deprotonate and become -COO- groups, and thus can effectively interact with the Ag+ ions and allow facile fabrication of Ag NPs. We also used Ag+ and Ni2+ to synthesis Ag/Ni alloy incorporated in CS-1B-10. The materials were characterized by powder X-ray diffraction (XRD), solid-state 13C and 29Si MAS NMR spectroscopy, nitrogen adsorption-desorption measurements, scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS).
    In the first project, the catalytic activity of these Ag NPs based SBA-1 materials were tested for reduction of 4-nitrophenol. As the catalyst for the reduction of 4-NP, the Ag-0.3-CS-1B-10 exhibit a very high catalytic activity with the activity parameter of 120 ( s-1 g-1 cat.), and Ag06Ni04-CS-1B-10 is 150 ( s-1 g-1 cat.).
    Then we further used Ag/Ni alloy incorporated in CS-1B-10 for dye degradation. The degradation of methyl orange and rhodamine b follows the pseudo first order kinetics. As the catalyst for the degradation of methyl orange, Ag06Ni04-CS-1B-10 exhibits a good catalytic activity with the activity parameter of 345.0 ( s-1 g-1 cat.), also processing rhodamine b degradation by using Ag08Ni02-CS-1B-10, the activity parameter is 135.0 ( s-1 g-1 cat.). This remarkable catalytic activity for the reduction of 4-nitrophenol and degradation of methyl orange/rhodamine b can be attributed to the ultra-small Ag/Ni NPs confined in cage-type mesopores of SBA-1 MSNs, which have the particle size around 500 nm.
    顯示於類別:[化學研究所] 博碩士論文

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