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新型聚醚離子液體的制備及其改性PP與催化性能研究

發(fā)布時間:2018-07-11 11:42

  本文選題:聚醚離子液體 + 改性��; 參考:《沈陽工業(yè)大學(xué)》2017年碩士論文


【摘要】:首先通過環(huán)氧氯丙烷開環(huán)聚合及與N-甲基咪唑反應(yīng)合成了氯化1-羥基聚醚-3-甲基咪唑離子液體([HO-PECH-MIM]Cl),然后利用活性端基轉(zhuǎn)化技術(shù)制備出氯化1-羧基聚醚-3-甲基咪唑離子液體([HOOC-PECH-MIM]Cl)及氯化1-氨基聚醚-3-甲基咪唑離子液體([H_2N-PECH-MIM]Cl)。采用IR與HNMR檢測儀對以上三種聚醚離子液體的化學(xué)結(jié)構(gòu)進行分析。將合成的聚醚咪唑離子液體與聚丙烯(PP)熔融共混,得到聚醚咪唑離子液體/PP復(fù)合材料,且對得到的復(fù)合材料的力學(xué)性能與結(jié)晶結(jié)構(gòu)等進行了表征與性能測試。再將上述聚醚離子液體分別負載無機粒子硅和金屬鋯,得到硅膠負載聚醚離子液體與負載鋯型聚醚咪唑離子液體催化劑,采用紅外(IR)和核磁(HNMR)對上述制備的負載型聚醚離子液體化學(xué)結(jié)構(gòu)進行分析,同時采用熱重分析儀(TGA)與電鏡掃描儀(SEM)對其熱性能與表觀形貌進行測定。再將三種聚醚離子液體及其負載硅/鋯的聚醚離子液體分別催化二氧化碳(CO2)與環(huán)氧丙烷(PO)合成碳酸丙烯酯(PC),優(yōu)化工藝參數(shù),對影響催化性能的因素如壓力、溫度、催化劑用量等進行考察,建立催化機理模型。實驗結(jié)果表明,新型聚醚離子液體與負載型聚醚離子液體均制備成功,且純度較高,而負載后的聚醚離子液體的相態(tài)發(fā)生了改變,具有很好的熱穩(wěn)定性。實驗結(jié)果說明,當(dāng)聚醚離子液體的含量為6%時,材料的拉伸強度提高了31%,彎曲強度提高了11%,而當(dāng)聚醚咪唑離子液體含量為9%時,改性后PP的沖擊強度相比之前提高了約132%,而斷裂伸長率則提高了75%。這說明聚醚離子液體改性后的PP強度和韌性均有顯著變化,其原因是聚醚離子液體起到了成核劑的作用,使PP結(jié)晶結(jié)構(gòu)發(fā)生改變,同時聚醚離子液體特有的柔性長鏈,使其能與PP基體很好地相容,對PP起到增強增韌作用。催化實驗結(jié)果說明,制備的新型聚醚離子液體催化劑催化轉(zhuǎn)化CO2與PO反應(yīng)合成碳酸丙烯酯的效果很好,且催化過程操作簡單,反應(yīng)時間短,催化劑易分離,催化劑重復(fù)使用多次后催化性能仍然很穩(wěn)定,這為實現(xiàn)固定床連續(xù)催化反應(yīng)提供數(shù)據(jù)基礎(chǔ),同時也為二氧化碳的直接高效利用提供了有效途徑。
[Abstract]:At first, 1-hydroxypolyether 3-methyl imidazole chloride ionic liquid ([HO-PECH-MIM] Cl) was synthesized by ring-opening polymerization of epichlorohydrin and reaction with N- methyl imidazole, and then 1-carboxyl polyether 3-methyl imidazole chloride was prepared by active terminal conversion technique. [HOOC-PECH-MIM] Cl and 1-aminopolyether 3-methyl imidazole chloride ([H2N-PECH-MIM] Cl). The chemical structures of the above three polyether ionic liquids were analyzed by IR and HNMR. The polyether imidazole ionic liquid / PP composites were prepared by melt blending the synthesized polyether imidazole ionic liquids with polypropylene (PP). The mechanical properties and crystalline structure of the composites were characterized and tested. Then the above polyether ionic liquids were loaded with inorganic particles silicon and metal zirconium respectively to obtain silica gel supported polyether ionic liquids and zirconium type polyether imidazole ionic liquid catalysts. The chemical structure of the supported polyether ionic liquids was analyzed by IR and HNMR, and the thermal properties and morphology were measured by thermogravimetric analyzer (TGA) and electron microscope scanner (SEM). Three polyether ionic liquids and polyether ionic liquids loaded with silicon / zirconium were used to catalyze the synthesis of propylene carbonate (PC) from carbon dioxide (CO _ 2) and propylene oxide (PO) respectively. The catalyst dosage was investigated and the catalytic mechanism model was established. The experimental results show that both the new polyether ionic liquid and the supported polyether ionic liquid have been prepared successfully, and the purity of the polyether ionic liquid is high. However, the phase state of the loaded polyether ionic liquid has changed and has good thermal stability. The experimental results show that when the content of polyether ionic liquid is 6, the tensile strength and bending strength of the material are increased by 31 and 11, respectively, and when the content of polyether imidazole ionic liquid is 9, The impact strength of the modified PP was increased by about 132 and the elongation at break was increased by 75%. This shows that the strength and toughness of PP modified by polyether ionic liquid have significant changes, the reason is that the polyether ionic liquid acts as a nucleating agent, which changes the crystalline structure of PP and the flexible long chain of polyether ionic liquid. It can be well compatible with PP matrix and plays a reinforcing and toughening role on PP. The results of catalytic experiments show that the new polyether ionic liquid catalyst is effective in the catalytic conversion of CO _ 2 and PO to propylene carbonate, and the catalytic process is simple, the reaction time is short, and the catalyst is easy to be separated. After repeated use of the catalyst, the catalytic performance is still very stable, which provides a data basis for the continuous catalytic reaction in a fixed bed, and also provides an effective way for the direct and efficient utilization of carbon dioxide.
【學(xué)位授予單位】:沈陽工業(yè)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:O645.1;O643.36

【參考文獻】

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