發(fā)布時間：2018-04-29 08:11

  本文選題：Anderson型雜多酸 + 烯烴環(huán)氧化　； 參考：《上海應(yīng)用技術(shù)大學(xué)》2017年碩士論文

【摘要】：在最前沿和最新的文獻(xiàn)中,催化術(shù)語通常與“綠色化學(xué)”和“可持續(xù)性”等概念密切相關(guān),因?yàn)榇呋墙档驮S多化學(xué)工業(yè)過程的能耗和環(huán)境負(fù)擔(dān)最有效的方案。選擇性催化氧化反應(yīng)在當(dāng)前化工行業(yè)中特別重要。許多關(guān)鍵的化學(xué)品和中間體如醇,環(huán)氧化物,醛,酮和有機(jī)酸都是通過選擇性催化氧化作用產(chǎn)生的。多金屬氧酸鹽具備很好氧化還原性質(zhì),持久的對抗氧化劑和環(huán)境兼容性。本論文是對Anderson型雜多酸烷氧化合物催化氧化性能的應(yīng)用進(jìn)行探究。(1)使用雙邊氨基共價修飾的Mn-Anderson型多金屬氧酸鹽作為催化劑,H2O2為氧化劑,無需自由基引發(fā)劑,對苯乙烯進(jìn)行催化氧化,能夠精確可控進(jìn)行專一選擇性生成環(huán)氧化合物或順式—二羥基化合物。通過單因子變量的方法優(yōu)化反應(yīng)。經(jīng)研究發(fā)現(xiàn),當(dāng)反應(yīng)溫度為50℃時,用CH3CN作為溶劑,對環(huán)氧化合物具有專一選擇性,其中選擇性≥99%,收率≥90%。當(dāng)反應(yīng)溫度為70℃時,用CH3CN/H20作為溶劑,對二羥基化合物具有專一選擇性,其選擇性及收率均≥99%。并成功地將各種烯烴轉(zhuǎn)化成相應(yīng)的環(huán)氧化物和順式二醇,具有優(yōu)異的選擇性和收率。(2)在水中使用單邊氨基修飾的Fe-Anderson型多酸[FeMo6018(OH)3{(OCH2)3CNH2}](FeⅢMo6-NH2)作為催化劑,1 atm 氧分子作為氧化劑,催化氧化苯甲醛生成苯甲酸,其中收率和選擇性均≥90%。許多種醛類已成功轉(zhuǎn)化為相應(yīng)的羧酸且具有優(yōu)良的產(chǎn)率。所需反應(yīng)條件溫和,可在FeⅢMo6-NH2催化劑極低使用量進(jìn)行,底物甚至可以擴(kuò)大量到克級,其收率和選擇性收率和選擇性均≥90%。其操作的簡單性、所需條件溫和、催化劑綠色環(huán)保以及可以回收循環(huán)使用。使其在工業(yè)規(guī)模上使用的潛力。
[Abstract]:In the cutting-edge and most recent literature, catalytic terminology is often closely related to concepts such as "green chemistry" and "sustainability", as catalysis is the most effective way to reduce the energy consumption and environmental burden of many chemical industrial processes. Selective catalytic oxidation is particularly important in the chemical industry. Many key chemicals and intermediates such as alcohols epoxides aldehydes ketones and organic acids are produced by selective catalytic oxidation. Polyoxometalates have good redox properties, persistent antioxidant and environmental compatibility. In this paper, the application of Anderson type heteropolyacid alkoxy compounds in catalytic oxidation was investigated. The Mn-Anderson type polyoxometalates modified by bilateral amino groups were used as catalyst H _ 2O _ 2 as oxidant without free radical initiator. The catalytic oxidation of styrene can produce epoxy compounds or cis-dihydroxyl compounds. The response was optimized by the method of single factor variable. It was found that when the reaction temperature was 50 鈩，

本文編號：1819115