本文選題：多金屬氧酸鹽 + 石墨烯�。� 參考：《遼寧師范大學(xué)》2015年碩士論文

【摘要】：多金屬氧酸鹽(簡稱多酸)易于在原子和分子水平上進(jìn)行結(jié)構(gòu)調(diào)變和修飾,因多樣的幾何與電子結(jié)構(gòu),具有優(yōu)異的氧化還原性質(zhì)和較好穩(wěn)定性。同時(shí),多酸還是一類環(huán)境友好型功能材料,在催化、醫(yī)藥、磁性及光學(xué)材料等領(lǐng)域具有廣泛的應(yīng)用前景。然而,多金屬氧簇比表面積小、不易分離和回收困難等缺點(diǎn)限制了它的應(yīng)用。實(shí)現(xiàn)多金屬氧簇與其他功能材料的復(fù)合,是突破多金屬氧酸鹽應(yīng)用瓶頸的重要途徑。本工作以制備氧化石墨工藝為主體,通過原位合成法合成石墨烯基多酸(POMs/GS)復(fù)合材料。探索了反應(yīng)條件對(duì)實(shí)驗(yàn)結(jié)果的影響,優(yōu)化了各項(xiàng)合成工藝參數(shù),制備出一系列石墨烯基多酸復(fù)合材料。利用紅外光譜(FT-IR)、X-射線粉末衍射(XRD)、拉曼光譜(Raman)、掃描電鏡(SEM)、熱重(TG)等技術(shù)手段,對(duì)自制復(fù)合物的結(jié)構(gòu)進(jìn)行了科學(xué)表征。通過對(duì)該類復(fù)合材料進(jìn)行循環(huán)伏安(CV)及氧化脫硫性能測(cè)試,深入研究并討論了新型復(fù)合材料的電化學(xué)性能和催化氧化脫硫特性。論文主要工作和研究結(jié)果如下:1.采用原位合成法制備了石墨烯基Dawson類型磷鉬酸復(fù)合物。通過大量實(shí)驗(yàn)研究,對(duì)各項(xiàng)合成條件進(jìn)行探索,選擇并確定了最佳工藝條件及路線。結(jié)果表明,當(dāng)?shù)蜏夭鍖訒r(shí)間7h,中溫氧化時(shí)間為40min時(shí),得到產(chǎn)物中磷鉬酸微�？删鶆蚍植荚谘趸┢瑢又�,石墨烯片層結(jié)構(gòu)完整,表面缺陷相對(duì)較少。2.石石墨烯基取代型磷鉬酸復(fù)合材料的合成。選取石墨烯及PMo11V、PMo10V2等取代型磷鉬酸為構(gòu)筑基元,合成了系列取代型磷鉬酸石墨烯雜化材料。對(duì)新材料進(jìn)行了IR、Raman、XRD、TG等結(jié)構(gòu)測(cè)試,實(shí)驗(yàn)結(jié)果表明,復(fù)合材料中各取代型磷鉬酸的結(jié)構(gòu)完整,石墨烯片層的缺陷度較少。所選工藝的氧化程度適中,石墨化效果優(yōu)異。新材料的對(duì)熱穩(wěn)定性較比多酸原料得到了較大改善。3.石墨烯基多酸復(fù)合材料的電化學(xué)性能研究。以碳糊電極為基底,用滴涂法制得多酸石墨烯復(fù)合材料的修飾電極。循環(huán)伏安實(shí)驗(yàn)測(cè)試結(jié)果表明,自制復(fù)合材料的電化學(xué)性能與母體多酸相似,循環(huán)伏安曲線中顯現(xiàn)出明顯的多酸的電化學(xué)特征。這預(yù)期該類復(fù)合材料具有潛在的催化氧化活性。4.石墨烯基多酸復(fù)合材料催化氧化脫硫?qū)嶒?yàn)研究。以所制石墨烯基多酸催化材料為催化劑,H2O2為氧化劑,進(jìn)行催化二苯并噻吩氧化脫硫?qū)嶒?yàn)研究。結(jié)果表明,新型催化材料對(duì)二苯并噻吩催化脫硫效果明顯。由于新型催化材料難溶于反應(yīng)體系中的極性有機(jī)溶劑,催化劑的分離和回收問題得到很好的解決,降低了生產(chǎn)成本。催化劑的重復(fù)使用研究表明,新型復(fù)合材料可循環(huán)再生利用。新催化材料具有催化活性高、選擇性好且壽命較長的優(yōu)異特性。
[Abstract]:Polyoxometalates (polyoxometalates) are easy to modify and modify at the atomic and molecular levels. Because of their various geometric and electronic structures, polyoxometalates have excellent redox properties and good stability.At the same time, polyacids are also a class of environment-friendly functional materials, which have a wide range of applications in catalysis, medicine, magnetic and optical materials.However, its application is limited by its small specific surface area, difficulty in separation and recovery.It is an important way to break through the bottleneck of application of polyoxometalates to realize the compounding of polyoxometalates with other functional materials.In this work, graphene polyacid POMs / GScomposites were synthesized by in-situ synthesis of graphite oxide.The influence of reaction conditions on the experimental results was explored. The synthesis parameters were optimized and a series of graphene polyacid composites were prepared.The structure of the self-made composite was characterized scientifically by means of infrared spectroscopy (FT-IR), X-ray powder diffraction (XRDX), Raman spectroscopy (Ram), scanning electron microscope (SEM), thermogravimetric (TG) and so on.The electrochemical and catalytic oxidation desulfurization properties of the composites were studied and discussed by means of cyclic voltammetry (CV) and oxidative desulfurization test.The main work and results are as follows: 1.Graphene-based Dawson-type phosphomolybdate complexes were prepared by in situ synthesis.Through a large number of experimental studies, various synthetic conditions were explored, and the optimum technological conditions and routes were selected and determined.The results show that when the intercalation time at low temperature is 7 h and the oxidation time is 40min at moderate temperature, the phosphomolybdic acid particles in the product can be uniformly distributed in the graphene oxide lamellae, the structure of the graphene layer is complete, and the surface defects are relatively few. 2.Synthesis of Shigene substituted phosphomolybdic Acid Composites.A series of substituted graphene phosphomolybdate hybrid materials were synthesized by using substituted phosphomolybdic acid, such as graphene and PMo11V, PMo10V2, as building units.The structure of the new material was tested by IR Ramanhe XRDX TG and the experimental results showed that the structure of the substituted phosphomolybdic acid in the composite was complete and the defect degree of the graphene lamellar was less.The oxidation degree of the selected process is moderate and the graphitization effect is excellent.The thermal stability of the new material is much better than that of the polyacid raw material.Study on Electrochemical Properties of Graphene Polyacid Composites.The modified carbon paste electrode was prepared by drip coating method.The results of cyclic voltammetry test show that the electrochemical properties of the composite are similar to those of the parent polyacid, and the electrochemical characteristics of polyacid are obvious in the cyclic voltammetry curve.It is expected that the composite has potential catalytic oxidation activity. 4. 4.Experimental study on Catalytic Oxidation Desulfurization of Graphene Polyacid Composites.The catalytic oxidation desulfurization of dibenzothiophene was studied using graphene polyacid as catalyst and H _ 2O _ 2 as oxidant.The results showed that the catalytic desulfurization of dibenzothiophene by the new catalytic material was obvious.The separation and recovery of the catalyst are well solved and the production cost is reduced because the new catalytic materials are insoluble in the polar organic solvents in the reaction system.The study of catalyst reuse shows that the new composite material can be recycled and reused.The new catalytic materials have the advantages of high catalytic activity, good selectivity and long life.
【學(xué)位授予單位】：遼寧師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TB332

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