製備具磺酸官能基之中孔洞矽材應用於有機催化反應;Sulfonic Acid Functionalized Mesoporous Silica for the Catalytic Organic Reaction

Please use this identifier to cite or link to this item: http://ir.lib.ncu.edu.tw/handle/987654321/91975

Title:	製備具磺酸官能基之中孔洞矽材應用於有機催化反應;Sulfonic Acid Functionalized Mesoporous Silica for the Catalytic Organic Reaction
Authors:	范芳榕;Fan, Fang-Rong
Contributors:	化學學系
Keywords:	中孔洞材料;二氧化矽;異相觸媒;佩希曼縮合反應;酯化反應;光固化反應;Silica Mesoporous materials;Heterogeneous catalyst;Pechmann condensation;Esterification;Photopolymerization;SiO2
Date:	2023-07-19
Issue Date:	2024-09-19 14:44:32 (UTC+8)
Publisher:	國立中央大學
Abstract:	中孔洞矽材具有高比表面積、適當孔洞大小與熱穩定佳等等的優勢，因此本研究主要以中孔洞矽材做為底材，並修飾磺酸官能基，應用於酯化反應與佩希曼縮合反應 (Pechmann Condensation)中。本研究分成兩個部份。第一部份，本研究利用直接合成法，將磺酸官能基修飾在中孔洞矽材 SBA-15 上。透過調整磺酸官能基與 TEOS 的比例，可合成出一系列 S15SX (X = 5, 10, 20, 25, 30)的樣品。經過 SAXRD, BET, XPS, TGA 等儀器鑑定確認材料結構的正確性與穩定性後，應用於三羥甲基丙烷 (TMP)酯化反應，並分別探討不同結構中孔洞矽材、磺酸官能基比例、不同丙烯酸與三羥甲基丙烷比例、不同溶劑比例、不同催化劑量等變因帶給反應的差異性。最後得知 AA 與 TMP 的莫爾比 2:1、環己烷與甲苯的體積比為 2:1 時，加入 1.8g S15S10 並施以 25 c.c/min 的空氣流速，能達到 50 %TMPDA 產量。而且，回收測試實驗中，當 S15S10 進行五次回收實驗後，仍具有 13%的 TMPDA 產量。第二部份，本研究以擴孔的 SBA-16，LP-SBA-16 作為底材，並調整磺酸官能基比例合成一系列樣品:LP-S16SX (X= 5, 10, 20)，應用於佩希曼縮合反應中。研究中探討不同反應物比例、不同溫度、不同催化劑量、不同磺酸官能基比例以及不同結構的催化劑所帶來的影響。最後，當 Resorcinol 與 EAA 的莫爾比例為 1:1.5、反應時間 5 分鐘、溫度為 130 °C 時，可達到 TOF 值為 810 (h-1)的效果。在回收測試中，催化劑反應五次後仍具有 7%的產率。;In this study, we adapted silica mesoporous materials loading with sulfonic acid group as catalyst due to its high specific surface area, proper pore size and high thermal stability properties. During the first part, we synthesized S15SX (X = 5, 10, 20, 25, 30) with TEOS as the silicon source, MPTMS as the sulfonica acid group precursor and P123 as the soft template. Due to the BET results, S15S10 possess 555cm2/g high specific surface area and 1.01nm optimal pore size. Those properties seem to favor the performance in esterification. Therefore, we applied it into Fischer esterification to produce TMPDA and explored the best experimental condition. Finally, we found that adding 1.8g S15S10 and 25 c.c/min air flow in the solution when molar ratio of AA:TMP is 2:1 and volume ratio of cyclohexane:toluene is 2:1 could reach 50% TMPDA GC Percent. Moreover, S15S10 still could produce 13% TMPDA GC Percent after 5 times recycling test. In the second part, we employed LP-SBA-16 as the supporting materials and loaded with different amount of sulfonic acid group (LP-S16SX, X = 5, 10 ,20). Its high specific surface area, optimal pore size properties may be possibly favor the Pechmann condensation. Eventually, we found that LP-S16S5 exhibited high performance (810 (h-1)) in Pechmann condensation at 130 °C. Last but not least, LP- S16S5 still could get 7 % yield after 5 recycling tests.
Appears in Collections:	[Graduate Institute of Chemistry] Electronic Thesis & Dissertation

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