製備酸性官能基中孔洞矽材與鈀鐵奈米雙金屬中孔洞/石墨烯碳複合材應用在有機催化反應;Sulfonic/Carboxylic Acid Functionalized Mesoporous Silica and Palladium Nanoparticles Embedded in the Carbon Composite for the Catalytic Organic Reaction

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題名:	製備酸性官能基中孔洞矽材與鈀鐵奈米雙金屬中孔洞/石墨烯碳複合材應用在有機催化反應;Sulfonic/Carboxylic Acid Functionalized Mesoporous Silica and Palladium Nanoparticles Embedded in the Carbon Composite for the Catalytic Organic Reaction
作者:	許宏誠;Hsu, Hung-Cheng
貢獻者:	化學學系
關鍵詞:	中孔洞矽材;中孔洞碳材;還原氧化石墨烯;異相催化劑;有機催化反應;Mesoporous carbon materials;Mesoporous silica materials;Reduced graphene oxide;Heterogeneous catalysts;Organic reaction
日期:	2022-07-27
上傳時間:	2022-10-04 10:59:25 (UTC+8)
出版者:	國立中央大學
摘要:	本研究分為兩大部分。在第一部分研究中，利用直接合成法，將具有磺酸官能基與羧酸官能基團修飾在中孔洞矽材表面，合成出O-K6SXCY系列之酸性催化劑。此系列催化劑具有高比表面積、孔洞一致性和富有酸性位點之官能基，期望能夠應用在催化1, 6-己二醇為丙烯酸酯。本部分將製備好的O-K6SXCY經過一系列的儀器鑑定後，確認催化劑的結構與穩定性後，進行己二醇酯化反應，分別探討了反應時間、酸性雙官能基催化劑比例、不同丙烯酸當量、不同聚合抑制劑量、不同催化劑量以及不同溫度對轉化率與產率之影響。經過一系列的實驗優化，最後以O-K6S20作為本部分的最佳催化劑，其HDDA在20小時的產率為72.8%，HDA在10小時的產率為50.4%。在此部分研究中，O-K6S20展現了其應用性與高催化活性。第二部分研究中，主要是利用奈米雙金屬還原在中孔洞碳材 (CMK-9) 與還原氧化石墨烯 (rGO) 之碳複合材料上，利用化學還原法可有效地將PdNPs還原在碳複合材中，並藉由CMK-9具有高比表面積及rGO具有快速電子傳輸效率，能夠快速將電子提供給PdNPs，增加PdNPs的電子密度，進而提升催化活性。本部分將合成出來的Pd(x)/Y%Fe3O4@rGOC9系列經過儀器鑑定後，應用在鈴木偶聯反應中，並分別探討了不同比例的碳複合材 (rGOC9)、不同Fe3O4含浸量、不同PdNPs含浸量、不同催化材料、不同溶劑、不同鹼、不同芳基鹵化物、不同芳基硼酸和不同溫度對催化反應之影響。經過一系列的實驗優化，Pd(0.75)/10%Fe3O4@rGOC9展現了優異的催化活性，其轉化率與產率分別達99.0%與94.8%，周轉頻率 (TOF) 高達7920.0 h-1。 ;This thesis consists of two parts, In the first part, we successfully synthesized the sulfonic acid and carboxylic acid functionalized mesoporous silicas (O-K6SXCY series) by direct synthesis using TEOS as silicon source, MPTMS or CES as functional group precursor, P123 as a soft template and hydrogen peroxide as an oxidant in an acidic environment. Among all the as-prepared catalysts, O-K6S20 has the best catalytic activity. According to the BET result, The synthesized O-K6S20 was confirmed about 679 m2/g. It has high surface area, good pore volume and high acid sites. It can increase the rate of acrylic acid and hexanediol to produce acrylate with 50.4% HDA yield and 72.8% HDDA yield at 90℃. In the second part, the aim of this work is to synthesize bimetallic PdFe nanoparticles within the pores of mesoporous carbon (CMK-9) and reduced graphene oxide (rGO) composite support, and use them as the catalysts for the Suzuki-Miyaura cross-coupling reaction between iodobenzene and phenylboronic acid. The metal nanoparticles are immobilized within the support by double agent chemical reduction method which uses NaBH4 and NH3BH3 as the reducing agents. Due to high surface area of CMK-9 and fast electron efficiency of rGO, PdFe nanoparticles are dispersed homogenously within the rGOC9 composite support. The metal (Pd:Fe) contents are varied to explore its effect on the performance of the catalyst which showed that Pd(0.75)/10%Fe3O4@rGO C9 exhibited excellent catalytic activity with 97% conversion and turnover frequency up to 7760 h-1. The utilization of Fe3O4 as one of the components has not only reduced the production cost of the catalyst but also allowed its efficient recovery and reuse.
顯示於類別:	[化學研究所] 博碩士論文

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