【摘要】：光催化的有機(jī)反應(yīng)已成為化學(xué)研究的熱點(diǎn),其中光催化劑發(fā)揮了關(guān)鍵作用。傳統(tǒng)的金屬光催化劑適用范圍廣、催化效果好,但毒性高、難回收、稀有金屬價(jià)格昂貴,所以發(fā)展有機(jī)光催化劑成為國內(nèi)外科學(xué)家關(guān)注的重點(diǎn)。輔酶NADH具有較低的還原電勢,可以在光的作用下激發(fā)給出電子,具有光催化劑的潛質(zhì)。我們使用輔酶NADH模型物作為光催化劑,進(jìn)行光催化的兩分子或多分子間有機(jī)反應(yīng)的研究。在本論文中我們介紹了 NADH模型物的研究進(jìn)展,主要作為還原劑用于有機(jī)反應(yīng)中,近年來國際上對NAD+模型物作為光催化劑的研究引人注目,而作為NAD+的還原態(tài),NADH模型物作為光催化劑將會成為國際社會下一個(gè)研究的熱點(diǎn)。我們目前的重點(diǎn)是找出合適的底物可以接受NADH模型物在光照下給出的電子,暫時(shí)發(fā)現(xiàn)了兩種:一種是重氮鹽,另一種是高價(jià)碘摀鹽。尤其是高價(jià)碘摀鹽,在有機(jī)合成中的應(yīng)用吸引了很多科學(xué)家的關(guān)注。我們也介紹了近幾年高價(jià)碘摀鹽在有機(jī)合成中的應(yīng)用。希望選擇合適的高價(jià)碘摀鹽用于NADH模型物作為催化劑的光反應(yīng)。我們還介紹了 C(sp3)-CF3和合成喹啉衍生物的研究進(jìn)展。通過實(shí)驗(yàn)我們發(fā)現(xiàn)了三氟甲基的高價(jià)碘摀鹽可以獲得輔酶NADH模型物提供的電子,得到三氟甲基自由基參與有機(jī)反應(yīng)。我們對反應(yīng)的條件進(jìn)行優(yōu)化,還拓展了底物。我們在實(shí)驗(yàn)中證明重氮鹽可以得到NADH提供的電子成為苯基自由基。在乙腈和烯烴或炔烴存在的條件下發(fā)生反應(yīng),得到喹啉的衍生物。我們對反應(yīng)進(jìn)行優(yōu)化和底物拓展,最后還研究這個(gè)反應(yīng)在藥物合成中的應(yīng)用。我們還研究了有機(jī)硼化物的合成。有機(jī)硼化物是一種很有用的有機(jī)物,在有機(jī)合成中有廣泛的用途,我們首先介紹合成有機(jī)硼化物的研究進(jìn)展,雖然有很多關(guān)于合成有機(jī)硼化物的報(bào)道,但是這些方法仍有很多缺點(diǎn),如需要配體、強(qiáng)堿等。我們通過納米催化劑可以不需要使用任何配體或堿,實(shí)現(xiàn)了在非常溫和條件下合成有機(jī)硼化物,而且官能團(tuán)的兼容性很好。我們也對使用的納米金屬催化劑進(jìn)行了表征。
[Abstract]:Photocatalytic organic reaction has become a hot spot in chemical research, among which photocatalyst plays a key role. Traditional metal photocatalysts have a wide range of application and good catalytic effect, but they are highly toxic, difficult to recover and expensive to rare metals. Therefore, the development of organic photocatalysts has become the focus of scientists at home and abroad. Coenzyme nadh has low reduction potential, which can excite and give electrons under the action of light, and has the potential of photocatalyst. We used coenzyme nadh as photocatalyst to study the organic reactions between two or more molecules. In this paper, we introduce the research progress of nadh model compounds, which are mainly used as reducing agents in organic reactions. In recent years, the research on NAD model compounds as photocatalysts has attracted much attention. As a reduced NAD, nadh model as photocatalyst will become the next research hotspot in the international community. Our current focus is to find suitable substrates that can accept electrons from nadh models under light. Two types of diazo salts have been found temporarily: one is diazo salt and the other is high iodide cover salt. In particular, the application of high-price iodide in organic synthesis has attracted the attention of many scientists. We also introduce the application of high-price iodide in organic synthesis in recent years. We hope to select suitable high-valence iodide for the photoreaction of nadh model. The research progress of C (sp3)-CF 3 and the synthesis of quinoline derivatives are also reviewed. Through experiments we found that trifluoromethyl iodide can obtain electrons from coenzyme nadh model and get trifluoromethyl radical to participate in organic reaction. We optimize the reaction conditions and expand the substrate. We have demonstrated in our experiments that diazonium salts can obtain nadh-supplied electrons to form phenyl radicals. In the presence of acetonitrile and alkenes or alkynes, the derivatives of quinoline were obtained. We optimize the reaction and expand the substrate. Finally, we study the application of the reaction in drug synthesis. We also studied the synthesis of organic boride. Organic boride is a very useful organic compound, which has a wide range of applications in organic synthesis. We first introduce the research progress in the synthesis of organic boride, although there are a lot of reports on the synthesis of organic boride. However, these methods still have many disadvantages, such as the need for ligands, strong bases and so on. We can synthesize organic boride under very mild conditions without using any ligands or alkaloids. The functional groups are compatible with each other. The nano-metal catalysts were also characterized.
【學(xué)位授予單位】：合肥工業(yè)大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：O627.31;O644.1

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