新穎含銅多層次沸石的製備與其丙烯選擇性氧化反應的催化研究

Novel Copper-Containing Hierarchical Zeolites: Preparation and Catalytic Study on Selective Oxidation of Propylene

張格愷(Ko-Kai Chang)

指導教授 ： 楊家銘

國立清華大學/理學院/化學系所/碩士(2019年)

摘要

多層次孔洞沸石由於有高比表面積且含有中孔洞，因此在催化過程中氣體反應物更容易接觸材料中的活性位點，再加上物質傳遞效率的提升，使得多層次孔洞沸石的催化效率比一般沸石塊材高。要在不摻雜鋁的沸石中放入金屬最常見的方法為含浸法，但是含浸法並不能控制金屬在材料中的分布位置以及分散性，本論文成功設計出具螯合官能基之結構導向試劑，C6H13-N+(CH3)2-(CH2)6-N+(CH3)2-(CH2)6-NH-(CH2)2-NH-(CH2)6-N+(CH3)2-(CH2)6-N+(CH3)2-C6H13(4Br-), 簡寫為 N2-En-N2，利用此結構導向試劑能夠合成出具有金屬螯合能力且奈米層板以十字交錯方式進行自我支撐的多層次孔洞 silicalite-1，利用位在層狀結構間的金屬螯合官能基可以與銅離子形成穩定的錯合物，進而得到負載高分散銅的多層次孔洞沸石催化劑，並將其應用於丙烯的選擇性氧化反應，且在180 ℃ 下有高丙烯醛選擇性。

關鍵字

多層次沸石 ； 丙烯選擇性氧化 ； 結構導向試劑

並列摘要

Hierarchical silicalite-1 zeolites with high surface areas, high pore volume ratios, high accessibilities, and ready mass transport properties have better catalytic performance than bulk silicalite-1. However, the most common strategy to prepare metal-containing silicalite-1 is impregnation which could not easily control the position and dispersity of metal. Here, we successfully synthesize a new type triblock structure-directing agent (SDA) with metal chelating group in the middle. The triblock SDA is C6H13-N+(CH3)2-(CH2)6-N+(CH3)2-(CH2)6-NH-(CH2)2-NH-(CH2)6-N+(CH3)2-(CH2)6-N+(CH3)2-C6H13(4Br-), abbreviated to N2-En-N2. By using this new type SDA, we could synthesize hierarchical silicalite-1 comprising highly-branched, self-pillared, orthogonally-stacked and metal chelating agent at the same time. The highly disperse copper complexes which are between two MFI nanosheets could be prepared by aid of chelating part. We applied this catalyst to selective oxidation of propylene catalytic reaction, and high acrolein selectivity at 180℃ could be obtained.

並列關鍵字

Hierarchical zeolites ； Structure-directing agent ； Selective oxidation of propylene

參考文獻

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