基于四醛基配體的三維亞胺類COFs材料的設(shè)計(jì)合成與結(jié)構(gòu)表征
發(fā)布時(shí)間:2018-04-27 23:40
本文選題:四醛基配體 + 三維亞胺類COFs; 參考:《吉林大學(xué)》2017年碩士論文
【摘要】:共價(jià)有機(jī)骨架材料(COFs)是一類新興的多孔結(jié)晶聚合物材料,它有著廣泛的應(yīng)用如氣體吸附和分離、催化、光電子學(xué)、化學(xué)傳感、藥物遞送和清潔能源等。與其它結(jié)晶多孔材料相比,COFs材料具有很多獨(dú)特的優(yōu)勢(shì),例如密度低、表面積大、孔徑和結(jié)構(gòu)可調(diào)、易功能化等。這一領(lǐng)域的快速發(fā)展吸引了科研工作者的廣泛關(guān)注。盡管二維COFs材料設(shè)計(jì)合成已經(jīng)很好的建立起來(lái),然而目前三維COFs材料的設(shè)計(jì)與合成卻仍是個(gè)挑戰(zhàn)。因此探索開(kāi)發(fā)新型三維COFs材料,使它們性能多樣化是至關(guān)重要的。這些在本論文的第一章緒論中進(jìn)行了詳細(xì)的討論,除此之外,還在第一章緒論中討論了COFs材料的分類、設(shè)計(jì)原則、合成方法以及它們?cè)诓煌I(lǐng)域的應(yīng)用。在第二章中,一種新型結(jié)晶亞胺類共價(jià)有機(jī)骨架材料TA-COF-1,在溶劑熱條件下由四-(4-酰基苯基)甲烷與對(duì)苯二胺首次通過(guò)縮合反應(yīng)生成。TA-COF-1晶體結(jié)構(gòu)通過(guò)PXRD、SEM、FT-IR以及TGA等表征進(jìn)行了研究。結(jié)果表明TA-COF-1具有良好的熱穩(wěn)定性,高Langmuir表面積(1771.19 m2g-1),小孔徑(1.28 nm)和大的孔體積(0.753 cm3g-1)。此外,TA-COF-1對(duì)H2的吸附量高達(dá)61.78 cm3 g-1的。值得一提的是,這是第一次使用四面體結(jié)構(gòu)的醛基配體來(lái)成功合成三維結(jié)晶亞胺類COFs。在第三章中,另一種新型結(jié)晶亞胺類共價(jià)有機(jī)骨架材料TA-COF-2,是在溶劑熱條件下由四-(4-;交)甲烷與四-(4-氨基苯基)甲烷首次通過(guò)縮合反應(yīng)生成。TA-COF-2晶體結(jié)構(gòu)通過(guò)PXRD、SEM、FT-IR以及TGA等表征進(jìn)行了研究。結(jié)果顯示TA-COF-2具有好的熱穩(wěn)定性和化學(xué)穩(wěn)定性,高Langmuir表面積(1313.91 m2 g-1),小孔徑(0.73 nm)和大的孔體積(0.474 cm3 g-1)。此外,TA-COF-2對(duì)H2的吸附量高達(dá)106.02 cm3 g-1,對(duì)CO2的吸附量為43.64 cm3 g-1。值得一提的是,這是第一次使用兩個(gè)同為四面體結(jié)構(gòu)的醛基/氨基配體來(lái)成功合成三維COFs.在第四章中,我們借鑒傳統(tǒng)多級(jí)孔沸石分子篩的合成方法,選取硅藻土作為合成多級(jí)孔COFs材料的基底,通過(guò)原位合成策略首次成功制備出具有多級(jí)孔結(jié)構(gòu)的硅藻土/共價(jià)有機(jī)骨架復(fù)合材料(標(biāo)記為Dt-EA/TA-COF-2)。該復(fù)合材料因硅藻土中大孔的引入,克服了TA-COF-2自身的單級(jí)微孔劣勢(shì),這也為該復(fù)合材料更多的潛在應(yīng)用優(yōu)勢(shì)提供了可能,并且這種基于硅藻土合成多級(jí)孔COFs材料的策略也為后續(xù)相關(guān)合成工作提供了寶貴的參考價(jià)值。
[Abstract]:Covalent organic framework material (COFs) is a new class of porous crystalline polymer materials, which has been widely used in gas adsorption and separation, catalysis, optoelectronics, chemical sensing, drug delivery and clean energy. Compared with other crystalline porous materials, COFs have many unique advantages, such as low density, large surface area, adjustable pore size and structure, easy functionalization and so on. The rapid development of this field has attracted wide attention of researchers. Although the design and synthesis of 2D COFs materials have been well established, the design and synthesis of 3D COFs materials is still a challenge. Therefore, it is very important to explore and develop new three-dimensional COFs materials and to diversify their properties. These are discussed in detail in the first chapter of this paper, in addition to the introduction of the first chapter, the classification of COFs materials, design principles, synthesis methods and their applications in different fields are discussed. In the second chapter, a new crystalline imine covalent organic skeleton material, TA-COF-1, was synthesized by condensation reaction of tetrachloro-4-acylphenyl) methane with p-phenylenediamine under solvothermal conditions. The crystal structure of TA-COF-1 was characterized by PXRDNSEMFT-IR and TGA. The results show that TA-COF-1 has good thermal stability, high Langmuir surface area of 1771.19 m2g-1g ~ (-1), small pore size of 1.28 nm) and large pore volume of 0.753 cm ~ (-3) g ~ (-1). In addition, the adsorption capacity of TA-COF-1 for H _ 2 was 61.78 cm3 / g ~ (-1). It is worth mentioning that this is the first time that three dimensional crystalline imines have been successfully synthesized by using tetrahedral aldehydes as ligands. In chapter III, Another new crystalline imine covalent organic skeleton material, TA-COF-2, was first synthesized by condensation reaction of tetramethane-4-acylphenyl) methane with tetra-butadiene-4-aminophenyl) methane in solvothermal condition. The crystal structure of .TA-COF-2 was characterized by PXRDX SEMT-IR and TGA etc. The results show that TA-COF-2 has good thermal and chemical stability, with high Langmuir surface area of 1313.91 m2 / g ~ (-1), small pore size of 0.73 nm) and large pore volume of 0.474 cm3 / g ~ (-1). In addition, the adsorption capacity of TA-COF-2 for H _ 2 and CO2 for H _ 2 and CO2 was 106.02 cm3 g-1 and 43.64 cm3 g-1, respectively. It is worth mentioning that this is the first time that three dimensional COFs have been successfully synthesized using two aldehydes / amino ligands with the same tetrahedron structure. In the fourth chapter, we choose diatomite as the substrate for the synthesis of multi-porous COFs materials by using the traditional synthesis method of multi-porous zeolite molecular sieve. Diatomite / covalent organic skeleton composites with multilevel pore structure (labeled Dt-EA-TA-COF-2) were successfully prepared by in-situ synthesis strategy for the first time. Because of the introduction of macropores in diatomite, the composite overcomes the single-stage micropore disadvantage of TA-COF-2 itself, which provides the possibility for the composite to have more potential application advantages. The strategy of synthesizing multilevel porous COFs materials based on diatomite also provides valuable reference value for the subsequent synthesis work.
【學(xué)位授予單位】:吉林大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:O641.4
【相似文獻(xiàn)】
相關(guān)碩士學(xué)位論文 前2條
1 陳婷婷;基于四醛基配體的三維亞胺類COFs材料的設(shè)計(jì)合成與結(jié)構(gòu)表征[D];吉林大學(xué);2017年
2 鄭俊蘭;中英學(xué)術(shù)英語(yǔ)中的強(qiáng)勢(shì)限制語(yǔ):一項(xiàng)基于COFS和MICUSP語(yǔ)料庫(kù)的對(duì)比研究[D];廣西師范大學(xué);2014年
,本文編號(hào):1812845
本文鏈接:http://sikaile.net/kejilunwen/huaxue/1812845.html
最近更新
教材專著