具磺酸官能基中孔洞矽材與製備奈米鈀金屬於中孔洞碳氮材在有機催化反應之應用

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題名:	具磺酸官能基中孔洞矽材與製備奈米鈀金屬於中孔洞碳氮材在有機催化反應之應用
作者:	陳科廷;Chen, Ke-Ting
貢獻者:	化學學系
關鍵詞:	奈米鈀金屬;中孔洞矽材;中孔洞碳氮材;果醣水解反應;六價鉻還原;palladium nanoparticles;mesoporous silicas;mesoporous N-doped carbon material;fructose hydrolysis;reduction of Cr(VI)
日期:	2021-08-27
上傳時間:	2021-12-07 11:29:34 (UTC+8)
出版者:	國立中央大學
摘要:	本研究主要探討方向分為兩大部分。第一部分是利用TEOS及MPTMS為共同矽源，P123作為軟模板，在酸性環境下以雙氧水作為氧化劑，並以直接合成法的方式合成出具有磺酸官能基之中孔洞矽材K6SX及S15SX。由於K6SX及S15SX具有高比表面積以及良好的孔洞體積，並且經官能基修飾後，表面會富含磺酸官能基，藉此期望在果醣水解產出5-羥甲基糠醛(HMF)反應上會擁有良好的表現。本實驗將製成的K6SX以及S15SX應用在催化果醣水解反應上，分別探討二維結構以及三維結構、不同溫度以及不同催化劑量對催化活性之影響。經過一系列的探討，K6S20作為催化劑去進行果醣水解反應，其HMF產率可達87.42%( Ratio(Mfructose/Mcata) = 9)。在這項研究中， K6S20展示了其應用於催化果醣水解產HMF是一具高催化活性的催化劑。而在第二部分研究中，透過三維結構之中孔洞碳材CMK-9及中孔洞碳氮材N-CMK-9作為載體，並利用化學還原劑使金屬還原速率上升，將奈米鈀金屬還原在N-CMK9及CMK-9中。CMK-9及N-CMK-9具有高比表面積以及良好的孔洞體積，此外N-CMK-9還具有缺陷的CN位點，更能使離子鈀金屬快速且平均分散在孔道之中，進而提高催化活性。本實驗將製成的Pd(X)@C9以及Pd(X)@NC9應用在催化六價鉻還原反應當中，分別探討不同載體以及不同含浸金屬量對催化活性之影響。在催化六價鉻還原反應的研究中，Pd(2)@NC9展現出很高的催化活性，其TOF值可達1.78 min-1。在這項研究中，Pd(2)@NC9展示其用於六價鉻還原催化反應中是具有高前景的催化劑。 ;This thesis consists of two parts. In the first part, the sulfonic acid functionalized mesoporous silicas (K6SX and S15SX) have been successfully synthesized by one-pot synthesis using tetraethoxysilane (TEOS) and mercaptopropyltrimethoxysilane (MPTMS) as silicon source, P123 as a soft template and hydrogen peroxide as an oxidant in an acidic environment. According to the BET result, the surface area of K6S20 and S15S20 was confirmed about 682.6 m2/g and 452.5 m2/g. Because of the high surface area, good pore volume, and rich in sulfonic acid functional groups, K6S20 and S15S20 might have a good performance in the reaction of fructose hydrolysis to produce 5-hydroxymethylfurfural (HMF). Among all the as-prepared catalysts, K6S20 exhibited the highest HMF yield of 87.42 % at 135oC with 20 mg catalyst, 3 ml DMSO and 1 mmol fructose. In the second part, palladium nanoparticles embedded in mesoporous N-doped carbon material (N-CMK-9), which was synthesized by nanocasting, through the double agent chemical reduction method as a catalytic catalyst. N-doped carbon material N-CMK-9 has a high surface area, good pore volume, defective CN sites and nitrogen gaps, so palladium nanoparticles could be uniformly dispersing in the materials to improve the catalytic activity. According to the TEM images, the particle size of the palladium nanoparticles was confirmed about 2-6 nm and 2-5 nm. The Pd(X)@C9 and Pd(X)@NC9 exhibited high catalytic activity for the reduction of environmentally harmful Cr(VI) to Cr (III). Among all the as-prepared catalysts, Pd(2)@NC9 exhibited the highest turnover frequency of 1.72 min-1.
顯示於類別:	[化學研究所] 博碩士論文

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