本文關(guān)鍵詞：刺激響應(yīng)性聚合物的制備與表征及其固定化酶的研究　出處：《陜西師范大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 智能型材料 超分子聚合物 固定化酶

【摘要】：當(dāng)今的聚合物己向智能材料發(fā)展,經(jīng)過多年的對于刺激響應(yīng)聚合物的深入研究,刺激響應(yīng)聚合物已獲得了越來越多的關(guān)注,刺激響應(yīng)是能使外部物理變化致使其產(chǎn)生智能的變化。由于它們有非常多的應(yīng)用,因此聚合有響應(yīng)基團(tuán)的聚合物豐富了智能材料的世界。多種響應(yīng)性的基團(tuán)整合到聚合物中,從而表現(xiàn)出多響應(yīng)的性質(zhì),這些刺激響應(yīng)性聚合物的響應(yīng)行為能夠縮小或擴(kuò)大來改變它們的光學(xué)性質(zhì)或根據(jù)環(huán)境的變化來改變它們的電性能。由于對于材料科學(xué)的發(fā)展是社會的發(fā)展的需求,因此我們需調(diào)整自己的方向為社會發(fā)展做貢獻(xiàn)。顯然,近些年產(chǎn)生了許多智能聚合物,并且事實說明刺激響應(yīng)性聚合物在我們生活中不可缺少的。智能聚合物其刺激響應(yīng)行為基本上是由聚合物鏈上存在的官能團(tuán)決定的。不同的功能基團(tuán)可產(chǎn)生不同的刺激。最常用的刺激有溫度、pH、光、離子強(qiáng)度、電子轉(zhuǎn)移(氧化還原)和主客體相互作用。在刺激響應(yīng)性聚合物中一種新穎的聚合物是多刺激響應(yīng)性高分子,雙響應(yīng)性或多響應(yīng)性聚合物是可以根據(jù)不同的刺激作出反應(yīng)產(chǎn)生疊加效果,這種智能高分子材料可以被用到更為精細(xì)的過程。基于此,本論文主要設(shè)計制備了三種新型的多刺激響應(yīng)性的聚合物,并研究了其響應(yīng)性質(zhì),為刺激響應(yīng)型材料的應(yīng)用奠定了基礎(chǔ)。本論文的研究內(nèi)容如下所示：(1) 基于主客體化學(xué)構(gòu)建Janus型超分子聚合物通過原子轉(zhuǎn)移自由基聚合、疊氮化反應(yīng)、點擊反應(yīng)和酯水解反應(yīng)合成pH響應(yīng)的客體高分子Ad-(PMAA)7,通過原子轉(zhuǎn)移自由基聚合的方法合成了溫度響應(yīng)的主體高分子β-CD-(PNIPAAm)4。通過紅外光譜、核磁和GPC對所涉及到的聚合物進(jìn)行了確認(rèn),通過測試數(shù)據(jù)證明了客體高分子己成功制得。在水溶液中,主客體高分子可自組裝具有Janus型超分子聚合物,通過紫外吸收光譜儀證實了設(shè)計合成的超分子具有溫度和pH雙響應(yīng)的性質(zhì),通過透射電鏡圖觀測其自組裝的膠束形態(tài)。在pH=5.4時,形成了以主體分子為殼,客體分子為核的球狀膠束,其粒徑尺寸為100nm；在溫度為35℃時,自組裝成以主體分子為核,客體分子為殼的球狀膠束,其粒徑尺寸為200nm, DLS測試了自組裝的粒徑分布。(2) 基于光和pH響應(yīng)客體高分子和溫度響應(yīng)的主體高分子構(gòu)建超分子聚合物通過原子轉(zhuǎn)移自由基聚合,點擊反應(yīng)和酯水解反應(yīng)成功的制備了一種具有溫度和pH雙響應(yīng)的超分子聚合物β-CD-(PNIPAAm)4-Azo-(PMAA)7,并用FTIR、NMR和GPC分析進(jìn)行了確認(rèn),證實了主客體高分子材料已被成功制備。通過紫外可見分光光度計研究結(jié)果可以推斷：超分子體系具有溫度、pH和光多響應(yīng)的特點,并驗證其存在主客體的相互作用。通過透射電鏡圖觀測其自組裝的膠束形態(tài)。在pH=5.4時,形成了以主體分子為殼,客體分子為核的球狀膠束,其粒徑尺寸為100nm；在溫度為35℃時,自組裝成以主體分子為核,客體分子為殼的球狀膠束,其粒徑尺寸為20Onm, DLS的測試表明形成的膠束具有較高的穩(wěn)定性,通過透射電鏡證實了超分子聚合物β-CD-(PNIPAAm)4-Azo-(PMAA)7的組裝和重組。(3)pH/光雙響應(yīng)高分子的制備及其固定化酶的研究通過原子轉(zhuǎn)移自由基聚合,點擊反應(yīng)和酯水解反應(yīng)成功的制備了一種具有光和pH雙響應(yīng)的聚合物mPEG-hv-PNB-PMAA-b-PS,并用FTIR, NMR和GPC分析進(jìn)行了確認(rèn)。通過紫外可見吸收光譜、GPC確定了此高分子具有光響應(yīng)的性質(zhì)。通過紫外-可見分光光度計確定其臨界膠束濃度。通過透射電鏡圖可觀測其自組裝的膠束形態(tài),合成的嵌段聚合物在水溶液條件下自組裝成具有核殼結(jié)構(gòu)的球狀膠柬,通過在不同pH條件下測試其粒徑尺寸,證明其具有pH響應(yīng)的性質(zhì),可通過改變pH值,從而調(diào)節(jié)膠束尺寸的大小。通過固定α-淀粉酶于此刺激響應(yīng)性高分子膠束,研究了此高分子膠束固定化酶的應(yīng)用,通過一系列測試,得出了最佳的條件,固定化酶溫度為45℃,給酶量為10U/mL,最大固定化酶的量為240mg/g,最適反應(yīng)溫度為65℃,最佳反應(yīng)pH為5.6,酶儲存日期為40天左右。
[Abstract]:The polymer has to intelligent material development, after years of in-depth research on stimuli responsive polymer, stimuli responsive polymers have gained more and more attention, stimulus response can make external physical changes cause a smart change. Because they have a lot of applications, so the polymerization of polymers enriched the intelligent response the material in the world. Many responsive groups into the polymer, which exhibit properties of multi response, the stimulus response response behavior of polymer to shrink or expand to change their optical properties or according to changes in the environment to change their electrical properties. Due to the development of material science is the social development needs therefore, we need to adjust their direction to make a contribution to the social development. Obviously, in recent years has produced many intelligent polymers, and the fact that. Response of polymer is indispensable in our life. The intelligent polymer responsive behavior basically is decided by the functional groups present on the polymer chain. Different functional groups can produce different stimuli. The most commonly used stimulus light, temperature, pH, ionic strength, electron transfer (redox) and host guest in response to stimulus interaction. A novel polymer polymer is more responsive polymer stimulation, dual responsive or more responsive polymers can make reaction superposition effect according to different stimuli, this intelligent high molecular materials can be used for more elaborate process. Based on this, this paper mainly design preparation three kinds of new polymer prickly response, and to study the response properties, which laid the foundation for the application of stimulus response materials. The research contents of this thesis are as follows: (1) base In the main object of chemical building Janus type supramolecular polymers via atom transfer radical polymerization, azidation reaction and hydrolysis of esters, click on the Ad- pH response object polymer synthesis (PMAA) of 7, the main polymer beta -CD- temperature response was synthesized via atom transfer radical polymerization (PNIPAAm) of the 4. polymer by infrared spectra. NMR and GPC of the involved was confirmed through the test data to prove the object of polymer has been successfully prepared. In aqueous solution, the main object of polymer self-assembly with Janus type supramolecular polymers, confirmed the properties with temperature and pH dual responsive supramolecular synthesis by UV absorption spectroscopy, the micellar morphology TEM observation of the self-assembly. In pH=5.4, formed the main molecular shell, spherical micelles of guest molecules, the particle size of 100nm in temperature; 35 degrees, to the main molecular self-assembled into spherical micelles as the core, the guest molecules as shell, the particle size is 200nm, DLS tested the self-assembly of particle size distribution. (2) the main polymer light and pH response object construction and temperature response of polymer supramolecular polymer polymerized by atom transfer radical based on, click on the reaction and the hydrolysis of esters was successfully prepared with a temperature and pH dual responsive supramolecular polymer beta -CD- (PNIPAAm) 4-Azo- (PMAA) 7, and FTIR, NMR and GPC analysis confirmed, confirmed that the subject and object of polymer materials has been successfully prepared by UV Vis. The spectrophotometer results can be inferred: supramolecular system with temperature, characteristics of pH and optical multi response, and verify the interaction of its existence. The main object of the micellar morphology by transmission electron microscopy observation its self-assembly. In pH=5.4, formed the main molecular shell The object, molecule as spherical micelle core, the particle size is 100nm; the temperature is 35 degrees centigrade to the main molecular self assemble into spherical micelles as the core, the guest molecules as shell, the particle size is 20Onm, the DLS test showed that the micelles has high stability, supramolecular polymer beta -CD- confirmed by transmission electron microscopy (PNIPAAm) and 4-Azo- (PMAA) assembly and reorganization of 7. (3) pH/ light responsive polymer preparation and immobilized enzyme by atom transfer radical polymerization, click on the reaction and hydrolysis of esters was successfully prepared with a polymer with mPEG-hv-PNB-PMAA-b-PS and pH double light response. And with FTIR, NMR and GPC analysis confirmed by UV Vis absorption spectra, GPC determines the polymer has the property of light response. By UV VIS spectrophotometer to determine the critical micelle concentration can be observed by TEM. The micellar morphology of self-assembly, synthesis of block copolymer in aqueous solution under the condition of self assemble into spherical core-shell micelles, through the test under conditions of different pH particle size, prove its properties of the pH response, by changing the pH value, so as to adjust the size of the micelles by fixing. Alpha amylase in the stimuli responsive polymeric micelles, the application of the polymer micelle immobilized enzyme, through a series of tests, the optimum conditions of immobilized enzyme, the temperature is 45 DEG C, the amount of enzyme is 10U/mL, the maximum of the immobilized enzyme was 240mg/g, the optimal reaction temperature is 65 DEG C, the optimum pH is 5.6, the enzyme storage date for 40 days.

【學(xué)位授予單位】：陜西師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：O631;Q814.2

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