【摘要】：在化學反應中,為了使反應更加的高效,催化劑的加入顯得尤為重要,超過80%的反應都需要加入催化劑,而其中使用金屬催化占一半以上。在過去,人們在均相催化反應中使用大量傳統(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,產物不環(huán)保等缺點,研究學者開始研究經過修飾的傳統(tǒng)催化劑,以提高過渡金屬催化劑的穩(wěn)定性,提高其催化反應的效率與選擇性。本文設計構建合成了多種帶有鄰、對位羥基吡啶配體的新型過渡金屬配合物,通過核磁氫譜、核磁碳譜、X射線晶體衍射等手段對其結構進行了表征,并對其催化性能進行了系統(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移反應并表現(xiàn)出了優(yōu)異的催化效果,通過反應時間、反應溫度、堿的種類、催化劑的種類以及堿和催化劑的用量等方面進行優(yōu)化實現(xiàn)了多種催化劑催化苯乙酮到1-苯乙醇的反應,我們所合成出的催化劑轉化率都在90%以上,甚至可實現(xiàn)99%的轉化。其次,本文設計合成出的經修飾的過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,通過反應時間、反應溫度、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)過渡金屬催化劑表現(xiàn)出良好的催化性能,比簡單合成和其他催化劑的合成效果優(yōu)秀多倍,在該反應體系中可以實現(xiàn)50%左右的產率。通過研究我們發(fā)現(xiàn)加入經修飾的過渡金屬催化劑可以實現(xiàn)反應無污染、原子利用率高、反應安全溫和,實現(xiàn)了綠色化學的目標,為催化劑領域又提供了新的思路和想法。通過本文的研究,我們可以發(fā)現(xiàn)經過修飾的過渡金屬催化劑具有結構穩(wěn)定、選擇性好、底物豐富、產物潔凈、反應安全、操作簡單等優(yōu)點。因此,我們認為經過修飾的過渡金屬催化劑具有廣闊的研究領域,深遠的研究價值,本文的研究可以實現(xiàn)綠色化學的目標,實現(xiàn)原子經濟性,在未來可以廣泛應用于醫(yī)藥等領域。
[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.
【學位授予單位】：遼寧大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O641.4;O643.36

【參考文獻】

相關碩士學位論文 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;2012年

，

本文編號：2285947