【摘要】：在化學(xué)反應(yīng)中,為了使反應(yīng)更加的高效,催化劑的加入顯得尤為重要,超過(guò)80%的反應(yīng)都需要加入催化劑,而其中使用金屬催化占一半以上。在過(guò)去,人們?cè)诰啻呋磻?yīng)中使用大量傳統(tǒng)催化劑,但是傳統(tǒng)催化劑有著許多弊端。為解決傳統(tǒng)催化劑催化性能不佳,產(chǎn)物不環(huán)保等缺點(diǎn),研究學(xué)者開(kāi)始研究經(jīng)過(guò)修飾的傳統(tǒng)催化劑,以提高過(guò)渡金屬催化劑的穩(wěn)定性,提高其催化反應(yīng)的效率與選擇性。本文設(shè)計(jì)構(gòu)建合成了多種帶有鄰、對(duì)位羥基吡啶配體的新型過(guò)渡金屬配合物,通過(guò)核磁氫譜、核磁碳譜、X射線晶體衍射等手段對(duì)其結(jié)構(gòu)進(jìn)行了表征,并對(duì)其催化性能進(jìn)行了系統(tǒng)的考察。催化性能的研究首先是利用上述配合物催化酮類化合物的氫轉(zhuǎn)移反應(yīng)并表現(xiàn)出了優(yōu)異的催化效果,通過(guò)反應(yīng)時(shí)間、反應(yīng)溫度、堿的種類、催化劑的種類以及堿和催化劑的用量等方面進(jìn)行優(yōu)化實(shí)現(xiàn)了多種催化劑催化苯乙酮到1-苯乙醇的反應(yīng),我們所合成出的催化劑轉(zhuǎn)化率都在90%以上,甚至可實(shí)現(xiàn)99%的轉(zhuǎn)化。其次,本文設(shè)計(jì)合成出的經(jīng)修飾的過(guò)渡金屬催化劑還可以有效催化以鄰苯二胺及環(huán)氧化合物為原料合成2-苯基-1,2,3,4-四氫喹喔啉的新型反應(yīng),通過(guò)反應(yīng)時(shí)間、反應(yīng)溫度、催化劑的種類以及酸和催化劑的用量的不斷優(yōu)化和摸索,我們發(fā)現(xiàn)過(guò)渡金屬催化劑表現(xiàn)出良好的催化性能,比簡(jiǎn)單合成和其他催化劑的合成效果優(yōu)秀多倍,在該反應(yīng)體系中可以實(shí)現(xiàn)50%左右的產(chǎn)率。通過(guò)研究我們發(fā)現(xiàn)加入經(jīng)修飾的過(guò)渡金屬催化劑可以實(shí)現(xiàn)反應(yīng)無(wú)污染、原子利用率高、反應(yīng)安全溫和,實(shí)現(xiàn)了綠色化學(xué)的目標(biāo),為催化劑領(lǐng)域又提供了新的思路和想法。通過(guò)本文的研究,我們可以發(fā)現(xiàn)經(jīng)過(guò)修飾的過(guò)渡金屬催化劑具有結(jié)構(gòu)穩(wěn)定、選擇性好、底物豐富、產(chǎn)物潔凈、反應(yīng)安全、操作簡(jiǎn)單等優(yōu)點(diǎn)。因此,我們認(rèn)為經(jīng)過(guò)修飾的過(guò)渡金屬催化劑具有廣闊的研究領(lǐng)域,深遠(yuǎn)的研究?jī)r(jià)值,本文的研究可以實(shí)現(xiàn)綠色化學(xué)的目標(biāo),實(shí)現(xiàn)原子經(jīng)濟(jì)性,在未來(lái)可以廣泛應(yīng)用于醫(yī)藥等領(lǐng)域。
[Abstract]:In chemical reaction, in order to make the reaction more efficient, the addition of catalyst is particularly important. More than 80% of the reactions need to add catalyst, and metal catalyst is used in more than half of the reactions. In the past, a large number of traditional catalysts were used in homogeneous catalytic reactions, but the traditional catalysts had many disadvantages. In order to solve the shortcomings of traditional catalysts such as poor catalytic performance and environmental protection, researchers have begun to study modified traditional catalysts to improve the stability of transition metal catalysts and improve the efficiency and selectivity of their catalytic reactions. In this paper, a variety of novel transition metal complexes with p-hydroxypyridine ligand were designed and synthesized, and their structures were characterized by nuclear magnetic hydrogen spectrum, nuclear magnetic carbon spectrum and X-ray crystal diffraction. The catalytic performance of the catalyst was systematically investigated. First of all, the above mentioned complexes are used to catalyze the hydrogen transfer reaction of ketone compounds and show excellent catalytic effect by reaction time, reaction temperature, kinds of alkaloids. The kinds of catalysts and the amount of alkali and catalyst were optimized to realize the reaction of acetophenone to 1-phenylethanol. The conversion of the catalysts was above 90% or even 99%. Secondly, the modified transition metal catalyst can also effectively catalyze the synthesis of 2-phenyl-1- (2-trihydroquinoxaline) from o-phenylenediamine and epoxy compounds. The reaction temperature and reaction time are determined. The kinds of catalysts and the amount of acid and catalyst were optimized and groped. We found that the transition metal catalysts showed good catalytic performance, which was many times better than that of simple synthesis and other catalysts. The yield of about 50% can be achieved in this reaction system. It is found that the modified transition metal catalyst can achieve no pollution, high atomic utilization rate, safe and mild reaction, achieve the goal of green chemistry, and provide new ideas and ideas for the field of catalyst. Through the research in this paper, we can find that the modified transition metal catalyst has the advantages of stable structure, good selectivity, abundant substrate, clean product, safe reaction, simple operation and so on. Therefore, we think that the modified transition metal catalysts have a wide range of research fields and far-reaching research value, the research in this paper can achieve the goal of green chemistry, achieve atomic economy, In the future can be widely used in medicine and other fields.
【學(xué)位授予單位】：遼寧大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O641.4;O643.36

【參考文獻(xiàn)】

相關(guān)碩士學(xué)位論文 前1條

1 郭培江;銅催化C-N交叉偶聯(lián)合成四氫喹喔啉類化合物[D];成都理工大學(xué);2012年

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本文編號(hào)：2285947