本文關(guān)鍵詞： 蒙脫石 合成與表征 固體堿 Knoevenagel縮合反應(yīng)　出處：《南昌航空大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

【摘要】：蒙脫石是一種層狀結(jié)構(gòu)的鋁硅酸鹽粘土礦物,具有良好的電負(fù)性、離子交換性、分散懸浮性、吸附性和吸水性等特點,在催化領(lǐng)域得到廣泛的應(yīng)用。本文利用蒙脫石為原料,研發(fā)幾種在Knoevenagel縮合反應(yīng)中的固體堿催化劑,對催化劑的合成條件、結(jié)構(gòu)關(guān)系和催化性能進(jìn)行了系統(tǒng)的研究。既實現(xiàn)了該反應(yīng)體系中的多相化,也實現(xiàn)了清潔工藝和生產(chǎn),同時減少了環(huán)境污染。主要包括以下內(nèi)容:(1)查閱大量文獻(xiàn),對固體堿催化劑材料和改性蒙脫石材料進(jìn)行了綜述,介紹了催化Knoevenagel縮合反應(yīng)機(jī)理和改性蒙脫石的合成方法。(2)以蒙脫石、苯胺和FeCl3.6H2O為原料,合成蒙脫石/聚苯胺復(fù)合固體堿與磁性蒙脫石/聚苯胺復(fù)合固體堿,采用紅外光譜、紫外可見漫反射光譜、XRD等對其結(jié)構(gòu)進(jìn)行了表征,利用熔點儀對催化反應(yīng)后的產(chǎn)物熔點進(jìn)行測定。利用蒙脫石/聚苯胺復(fù)合固體堿作為催化劑,通過催化Knoevenagel縮合反應(yīng)的正交實驗,從中找出最佳實驗條件,并且對反應(yīng)溫度,催化劑用量,反應(yīng)時間分別進(jìn)行了研究實驗。合成的2種催化劑在Knoevenagel縮合反應(yīng)的重復(fù)實驗中能夠重復(fù)利用3次。(3)以蒙脫石和硝酸鋰為原料,合成12種蒙脫石/硝酸鋰復(fù)合固體堿,通過紅外光譜、XRD、氮氣等溫吸附-脫附等對其結(jié)構(gòu)進(jìn)行了表征,通過熔點儀對催化Knoevenagel縮合反應(yīng)后的產(chǎn)物熔點進(jìn)行測定。利用400℃煅燒的蒙脫石/(0.2g)硝酸鋰復(fù)合固體堿作為催化劑,通過催化Knoevenagel縮合反應(yīng)的正交實驗,從中找出最佳實驗條件。對部分合成的蒙脫石/硝酸鋰復(fù)合固體堿進(jìn)行催化Knoevenagel縮合反應(yīng)實驗,其中400℃煅燒的蒙脫石/(0.2g)硝酸鋰復(fù)合固體堿的催化效果最好,反應(yīng)產(chǎn)物的收率為96.3%。利用合成的400℃煅燒的蒙脫石/(0.2g)硝酸鋰復(fù)合固體堿催化劑對Knoevenagel縮合反應(yīng)進(jìn)行重復(fù)實驗中,這種催化劑都可以重復(fù)利用3次。(4)以蒙脫石和氫氧化鈉為原料,合成3種蒙脫石/NaOH復(fù)合固體堿,通過紅外光譜、XRD、氮氣等溫吸附-脫附等對其結(jié)構(gòu)進(jìn)行了表征,通過熔點儀對催化Knoevenagel縮合反應(yīng)后的產(chǎn)物熔點進(jìn)行測定。當(dāng)苯甲醛和丙二腈的物質(zhì)的量比為10 mmol:10 mmol、反應(yīng)時間1 h、反應(yīng)溫度60℃、催化劑用量0.1 g的條件下,利用合成的3種蒙脫石/NaOH復(fù)合固體堿作為催化劑,通過催化Knoevenagel縮合反應(yīng)實驗,其中550℃煅燒的蒙脫石/NaOH/CTAB固體堿的催化效果最好,反應(yīng)產(chǎn)物的收率為88.2%。利用其中合成的2種催化劑對Knoevenagel縮合反應(yīng)進(jìn)行重復(fù)實驗中,這2種催化劑都可以重復(fù)利用3次。(5)以蒙脫石、硫酸和3-氨丙基三甲氧基硅烷為原料,合成3種H-蒙脫石-NH2復(fù)合固體堿,通過紅外光譜、XRD、熱重分析等對其結(jié)構(gòu)進(jìn)行了表征,通過熔點儀對催化Knoevenagel縮合反應(yīng)后的產(chǎn)物熔點進(jìn)行測定。當(dāng)苯甲醛和丙二腈的物質(zhì)的量比為10 mmol:10 mmol、反應(yīng)時間1 h、反應(yīng)溫度60℃、催化劑用量0.1 g的條件下,利用合成的3種H-蒙脫石-NH2復(fù)合固體堿作為催化劑,通過催化Knoevenagel縮合反應(yīng)實驗,其中(酸化2h)H-蒙脫石-NH2復(fù)合固體堿的催化效果最好,反應(yīng)產(chǎn)物的收率為90.1%。利用其中合成的3種催化劑對Knoevenagel縮合反應(yīng)進(jìn)行重復(fù)實驗中,這3種催化劑都可以重復(fù)利用3次。
[Abstract]:Aluminum silicate clay mineral montmorillonite is a layered structure, with good electronegativity, ion exchange, dispersed suspension, adsorption and absorption, has been widely used in the field of catalysis. Using montmorillonite as raw materials, in the development of several Knoevenagel and solid alkali catalyst reaction in the synthesis conditions the catalyst, catalytic performance and structure relationship were studied. The reaction system is realized in multi phase, also achieved a clean production process and at the same time, to reduce the environmental pollution. Mainly includes the following contents: (1) the literature review of solid base catalyst materials and modified montmorillonite materials the review introduces the synthesis method of Knoevenagel catalyzed condensation reaction mechanism and modified montmorillonite. (2) with montmorillonite, aniline and FeCl3.6H2O as raw materials, synthesis of montmorillonite / polyaniline composite with magnetic solid base The montmorillonite / PANI composite solid base, using infrared spectroscopy, UV Vis diffuse reflectance spectra and structure were characterized by XRD, the melting point after the catalytic reaction product was determined by melting point apparatus. Using montmorillonite as catalyst / polyaniline composite solid base, through the orthogonal experiment of catalytic Knoevenagel reaction, to find out the best experimental conditions from in the catalyst and the reaction temperature, dosage, reaction time were studied. Experiments can be repeatedly used 3 times repeated tests of 2 kinds of catalyst in Knoevenagel condensation reaction. (3) using montmorillonite and lithium nitrate as raw materials, synthesis of 12 kinds of lithium nitrate / montmorillonite composite solid base, through the infrared spectrum, XRD and nitrogen adsorption desorption were used to characterize its structure, the melting point of Knoevenagel catalytic condensation reaction after the products were determined by melting point apparatus using 400 calcined montmorillonite. Stone (0.2g) / lithium nitrate composite solid alkali as catalyst, through orthogonal experiment of catalytic Knoevenagel reaction, to find out the best experimental conditions from. On the part of the synthesis of lithium nitrate / montmorillonite composite solid alkali catalyst for Knoevenagel condensation reaction, including 400 calcined / montmorillonite (0.2g) had the best catalytic effect of lithium nitrate composite solid alkali reaction, the yield of the product was synthesized by montmorillonite 96.3%. 400 calcined / (0.2g) on Knoevenagel condensation reactions of lithium nitrate composite solid alkali catalyst repeated experiments, the catalyst can be reused 3 times. (4) using montmorillonite and sodium hydroxide as raw materials, synthesis of 3 kinds of montmorillonite /NaOH composite solid alkali and through the infrared spectrum, XRD, nitrogen adsorption desorption were used to characterize the structure of the product, melting point Knoevenagel after catalytic condensation reaction were determined by melting point meter when. Benzaldehyde and propylene nitrile two molar ratio of mmol:10 was 10 mmol, the reaction time is 1 h, the reaction temperature is 60 DEG C, the condition of catalyst is 0.1 g, as a catalyst synthesized by 3 kinds of montmorillonite /NaOH composite solid base, through the experiment of catalytic Knoevenagel condensation reaction, the catalytic effect of 550 calcined Montmorillonite Solid /NaOH/CTAB the best reaction products of alkali, the yield was 88.2%. with 2 kinds of catalysts on the synthesis of Knoevenagel condensation reaction to repeat the experiment, these 2 kinds of catalysts can be reused 3 times. (5) with montmorillonite, sulfuric acid and 3- aminopropyltrimethoxysilane as raw materials, synthesis of 3 kinds of H- montmorillonite -NH2 composite solid alkali and through the infrared spectrum, XRD and thermogravimetric analysis were used to characterize its structure, the melting point of Knoevenagel catalytic condensation reaction after the products were determined by melting point apparatus. When the benzaldehyde and propylene nitrile two molar ratio 10 mmol:10 mmol, the reaction time is 1 h, the reaction temperature is 60 DEG C, the condition of catalyst is 0.1 g, as a catalyst synthesized by 3 kinds of H- montmorillonite -NH2 composite solid base, through the experiment of catalytic Knoevenagel condensation reaction, in which (acidification 2H) had the best catalytic effect of H- montmorillonite -NH2 composite solid alkali, reaction product yield 90.1%. use the 3 kinds of catalysts on the synthesis of Knoevenagel condensation reaction to repeat the experiment, these 3 kinds of catalysts can be reused 3 times.

【學(xué)位授予單位】：南昌航空大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：O643.36

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