本文選題：石墨烯　切入點：催化　出處：《濟南大學》2017年碩士論文

【摘要】：作為21世紀的新型材料,石墨烯是由碳原子以sp2雜化連接的單原子層構(gòu)成的新型二維原子晶體,它具有優(yōu)異的電學,力學,熱學,光學性能和大的比表面積,這使得石墨烯成為理想的金屬納米材料的負載體,在高新技術(shù)領域,如:光電轉(zhuǎn)換應用、能源催化應用、生物醫(yī)學應用等方面展現(xiàn)出巨大的應用前景。本論文通過對石墨烯材料的研究,進行了功能化石墨烯材料的探索的研究,對石墨烯為載體的催化反應進行了深入研究。在本論文中,我們合成了一系列銅鈀功能化的石墨烯材料并將其運用到鹵代烴的Suzuki偶聯(lián)反應之中,并利用高效液相色譜和氣相色譜對其催化活性進行了評價,結(jié)果證明具有優(yōu)越的效率和選擇性。主要研究內(nèi)容和成果如下:(1)我們通過對Hummers方法的改進,選用了兩種途徑來制備氧化石墨烯(GO),并通過對形貌的表征,選取了合適的制備途徑,制備了在水溶劑中具有很好分散性和低晶格缺陷的溫和氧化的氧化石墨烯;(2)我們對銅鈀功能化石墨烯的制備路線進行了探索,選用了以堿性條件下的水合肼作為還原劑和乙二醇作為溶劑的溶劑熱還原法兩種方法為制備路徑,實驗證明我們選用乙二醇作為溶劑的溶劑熱法為制備方法,制備出了具有高效催化活性且粒子附著較為均勻和密集的石墨烯材料。(3)我們對不同鈀銅比例的石墨烯材料的催化效率進行了分析,并且對實驗條件進行了探索,最終,確定了最佳效率的催化材料為銅鈀比例為1:1的功能化石墨烯材料,最佳的實驗反應溫度為80oC,實驗的最佳溶劑為乙醇和水比例為1:1。(4)我們對不同的鹵代烴進行了Suzuki偶聯(lián)反應的效率和選擇的探討,我們發(fā)現(xiàn),所制備的銅鈀功能化石墨烯具有十分優(yōu)越的效率和選擇性。鹵代烴化合物轉(zhuǎn)化率超過90%,聯(lián)苯化合物選擇性達到95%,對多種鹵代烴化合物有優(yōu)秀的催化適用性。(5)對于催化的循環(huán)利用效率,我們以溴苯作為模型了探討,發(fā)現(xiàn)銅鈀功能化石墨烯這一非均相催化劑有著十分優(yōu)越的效率和轉(zhuǎn)化率,循環(huán)五次后,效率仍能達到90%以上,選擇性在95%以上,用TEM進行了形貌特征的檢測,發(fā)現(xiàn)催化劑仍保持良好的形貌特征和密集的粒子附著。
[Abstract]:As a new material in the 21st century, graphene is a new two-dimensional atomic crystal composed of carbon atoms connected by sp2 hybrid monatomic layer. It has excellent electrical, mechanical, thermal, optical properties and large specific surface area.This makes graphene an ideal negative carrier for metal nanomaterials and has shown great application prospects in high-tech fields such as optoelectronic conversion applications, energy catalytic applications, biomedical applications, and so on.Through the study of graphene materials, the functional graphene materials were studied, and the catalytic reaction of graphene as the carrier was studied.In this thesis, a series of copper-palladium functionalized graphene materials were synthesized and applied to the Suzuki coupling reactions of halogenated hydrocarbons, and their catalytic activity was evaluated by high performance liquid chromatography (HPLC) and gas chromatography (GC).The results show that it has superior efficiency and selectivity.The main research contents and results are as follows: (1) by improving the Hummers method, we have selected two ways to prepare graphene oxide.A mild oxidized graphene oxide with good dispersion and low lattice defects in aqueous solvents was prepared. We have explored the preparation route of copper-palladium functionalized graphene.The solvothermal reduction method with hydrazine hydrate as reducing agent and ethylene glycol as solvent was chosen as the route of preparation. The experiment proved that the solvothermal method with ethylene glycol as solvent was used as the preparation method.The graphene materials with high catalytic activity and uniform and dense particle adhesion were prepared. We analyzed the catalytic efficiency of graphene materials with different palladium and copper ratios, and explored the experimental conditions.The best efficient catalyst is functionalized graphene material with the ratio of copper and palladium 1:1.The optimum reaction temperature is 80oC and the optimum solvent is ethanol / water ratio of 1: 1.0.We have studied the efficiency and selection of Suzuki coupling reaction for different halogenated hydrocarbons.The copper-palladium functionalized graphene has excellent efficiency and selectivity.The conversion of halogenated hydrocarbons exceeds 90, the selectivity of biphenyl compounds reaches 95%, and has excellent catalytic applicability for various halogenated hydrocarbons.It was found that the copper-palladium functionalized graphene was a heterogeneous catalyst with excellent efficiency and conversion. After five cycles, the efficiency was still over 90% and the selectivity was over 95%. The morphologic characteristics of the catalyst were examined by TEM.It was found that the catalyst maintained good morphology and dense particle adhesion.
【學位授予單位】：濟南大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TQ127.11;O621.251

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本文編號：1706463