本文關(guān)鍵詞：多孔芳香骨架膜材料的合成及性質(zhì)研究　出處：《吉林大學》2015年碩士論文　論文類型：學位論文

  更多相關(guān)文章： 多孔材料 有機膜材料 PAF膜材料 氣體分離

【摘要】：多孔材料由于具有高的比表面積，孔道結(jié)構(gòu)多樣性的特點引起了材料領(lǐng)域的科學家們廣泛關(guān)注，尤其在氣體分離與存儲領(lǐng)域，多孔材料的應用最為廣泛。目前，合成的多孔材料主要為顆粒狀的，并且需要苛刻的條件進行氣體的存儲與分離，因此，將其制備成膜材料將更具有應用價值。本論文設計合成了自身具有孔道結(jié)構(gòu)的多孔芳香骨架化合物（PAF）膜材料并研究其在CO2/N2氣體分離方面的性質(zhì)。 多孔芳香骨架化合物（PAFs）是一種剛性芳香結(jié)構(gòu)基元連接而成的有機多孔材料，，具有骨架密度低，穩(wěn)定性高的特點，其本身的孔結(jié)構(gòu)及其官能團的可加工性被認為是最合適的成膜材料。本論文第二部分中我們首先通過三氟甲磺酸（CF3SO3H）催化含有氰基的芳香單體自身聚合制備出自支撐的柔性膜（PAF-57）。通過FTIR和NMR表征，證實了氰基（-CN）發(fā)生了聚合反應生成三嗪環(huán)結(jié)構(gòu)，SEM顯示膜表面光滑連續(xù)，無明顯裂縫缺陷。氣體分離實驗發(fā)現(xiàn)該膜有反常的膜分離效果。于是我們又進一步做了氣體透量隨壓力變化的實驗：隨著進氣壓力的增大，CO2的透量幾乎無明顯變化，與此同時N2的透量隨著壓力增大而增大。因此，理想的氣體分離系數(shù)逐漸增大。實驗測得將N2/CO2（體積比為1:1）的混合氣體通過膜時，壓力從0.1MPa到0.5MPa時，N2/CO2的分離系數(shù)為1.7~4.5，N2的透量從2.3×10-7mol m-2s-1Pa-1增大到7.7×10-7mol m-2s-1Pa-1。在與傳統(tǒng)的膜選擇性與透量的權(quán)衡關(guān)系中，PAF-57膜表現(xiàn)出反常的膜分離效果。在較高滲透壓力下，該膜將具有更加優(yōu)異的膜分離效果。 本文的第三部分我們用含有烷烴鏈（-CH3）的有機單體在CF3SO3H為催化劑的條件下，制備出枝狀的多孔芳香骨架膜材料（PAF-58）。同樣，通過FTIR和NMR等基礎(chǔ)表征，證明制備出的PAF-58膜符合設計預期。在273K，1bar條件下，PAF-58膜表現(xiàn)出對CO2很強的吸附能力，CO2/N2吸附分離比為119.3。此歸因于膜骨架中含大量堿性給電子基團N，易于與CO2之間發(fā)生相互作用，同時烷烴鏈的引入具有一定的位阻效應，阻礙了N2與膜之間的相互作用，兩種作用同時存在，增大了膜的選擇性，提高PAF-58膜的氣體分離能力。膜分離實驗也證實了上面的結(jié)果，在室溫下，將CO2/N2（體積比1：1）混合氣體通過膜后，該膜具有很好的膜分離效果，CO2的透量約為5.2×10-8mol m-2s-1Pa-1。長時間進行膜分離實驗時，CO2的透量幾乎無變化，說明PAF-58膜具有良好的穩(wěn)定性。
[Abstract]:Because of its high specific surface area and diversity of pore structure, porous materials have attracted wide attention of scientists in the field of materials, especially in the field of gas separation and storage, porous materials are most widely used. At present, porous materials are widely used in the field of gas separation and storage. The synthesized porous materials are mainly granular and require harsh conditions for gas storage and separation. In this thesis, we designed and synthesized the porous aromatic skeleton compound (PAF) with its own pore structure. Membrane materials and their properties in CO2/N2 gas separation were studied. Porous aromatic matrix compound (PAFs) is an organic porous material with rigid aromatic structure elements, which has the characteristics of low skeleton density and high stability. Its pore structure and the processability of its functional groups are considered to be the most suitable film-forming materials. In the second part of this thesis, we first adopted CF3SO3H- (trifluoromethyl sulfonic acid). The self-polymerization of aromatic monomers containing cyanide was used to prepare the self-supporting flexible membrane PAF-57. It was characterized by FTIR and NMR. It is proved that the surface of the film is smooth and continuous due to the polymerization of cyanobutadiene (CNN) and the formation of triazine ring structure (SEM). There is no obvious crack defect. Gas separation experiment found that the membrane has abnormal membrane separation effect. So we further do the gas permeability with the pressure change experiment: with the increase of inlet gas pressure. The permeability of CO2 hardly changed, while the permeability of N2 increased with the increase of pressure. The ideal gas separation coefficient increases gradually. The experimental results show that when the mixture of N _ 2 / CO _ 2 (volume ratio is 1: 1) passes through the membrane, the pressure ranges from 0.1 MPA to 0.5 MPA. The separation coefficient of N _ 2 / CO _ 2 is 1.7% 4.5. The penetration of N2 increased from 2.3 脳 10-7mol m-2s-1Pa-1 to 7.7 脳 10-7mol. M-2s-1Pa-1. In the tradeoff between traditional membrane selectivity and permeability. PAF-57 membrane shows abnormal membrane separation effect, and it will have better membrane separation effect at higher osmotic pressure. In the third part of this paper, we use organic monomers containing alkane chain-CH3 under the condition of CF3SO3H as catalyst. The branched porous aromatic framework membrane (PAF-58) was prepared. Similarly, FTIR and NMR were used to characterize the prepared PAF-58 membrane. The results showed that the prepared PAF-58 membrane was in line with the design expectation at 273K. The adsorption and separation ratio of CO _ 2 / N _ 2 on PAF-58 membrane was 119.3 under the condition of 1 bar, which was attributed to the existence of a large number of basic electron donor groups N in the membrane skeleton. It is easy to interact with CO2, and the introduction of alkane chain has a certain steric resistance effect, which hinders the interaction between N2 and membrane. The two kinds of interaction exist at the same time, and increase the selectivity of the membrane. The experiment of membrane separation also confirmed the above results. At room temperature, the mixture of CO _ 2 / N _ 2 (volume ratio 1: 1) was passed through the membrane. The membrane has a good membrane separation effect. The permeability of CO _ 2 is about 5.2 脳 10 ~ (-8) mol m ~ (-2) s-1Pa-1.When the membrane separation experiment is carried out for a long time, there is almost no change in the permeability of CO _ 2. It shows that PAF-58 film has good stability.
【學位授予單位】：吉林大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：O625;TB383.2

【參考文獻】

相關(guān)期刊論文 前1條

1 吳家睿;;通向生命科學未來的路線圖[J];科學;2004年01期

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