本文選題：多巴胺　切入點：漆酶　出處：《中國科學院大學(中國科學院過程工程研究所)》2017年碩士論文　論文類型：學位論文

【摘要】：生物催化膜將物質選擇性傳遞與化學反應結合,可以極大地提高反應效率,在醫(yī)藥、食品、水處理等領域應用前景廣泛。然而目前生物催化膜制備過程中存在的載酶率不高、酶活保持低和膜本身性能下降等問題限制了其應用。針對上述問題,本論文重點研究了同時具備分離、吸附、催化功能的多功能膜的制備及其在水處理過程的應用。研究內容和成果主要分為以下兩個部分:(1)受到貽貝粘蛋白和細胞膜結構的啟發(fā),將漆酶通過逆向過濾的方式包埋在納濾膜支撐層內,再利用聚多巴胺(PDA)仿生涂層將漆酶封裝在膜內,制備了同時具有截留、催化、吸附三種功能的多功能膜,并將其應用于水中微量污染物的去除。以去除水中雙酚A(BPA)為例(原料液中BPA濃度為10mg.L-1),NF270多功能膜對BPA的去除率達到84.3±7.3%,遠遠高于傳統(tǒng)的芬頓氧化(BPA去除率55%)。對其多功能協(xié)同作用機制的研究表明,納濾膜本身具有的截留功能截留部分污染物,減少了酶催化負荷;而膜以及PDA涂層的吸附功能將未被截留的微量污染物在膜內富集并且延長了底物與酶分子的反應時間,進而大大提高酶促反應效率;同時生物酶的催化功能打破了膜材料"吸附飽和"的限制,使得"吸附-催化"過程連續(xù)進行,且協(xié)同效應的存在大大提高了整體效果。(2)為了解決多功能膜在長期使用過程中由于PDA涂層不夠致密導致的酶泄露問題,進一步提高載酶量和酶活力,分別利用多巴胺/聚乙烯亞胺(DA/PEI)和多巴胺/銅離子(DA/Cu2+)共沉淀方法在載酶納濾膜支撐層內形成新型仿生涂層。研究結果表明共沉淀不僅縮短DA自聚時間,增強PDA涂層的均一性和穩(wěn)定性,還極大地降低酶泄露,增加封裝效率,提高酶活性。此外,采用該種方法制備的多功能膜,其特殊的"分離層-漆酶-支撐層/封裝層"三明治結構使得該多功能膜兩面均具有催化活性,可以利用其構建雙面酶膜反應器(EMR),高效去除水中污染物,其中以DA/Cu2+共沉淀制備的多功能膜構建的EMR具有最高的BPA去除率,且由于流通模式下的強制對流有效移除產物,打破膜穩(wěn)定性與去除率之間平衡,EMR的使用穩(wěn)定性得以大幅度提高。研究表明通過調控多功能膜的載酶量、固定化酶位置、酶活性以及底物/產物傳質,可以優(yōu)化EMR對微量污染物的去除效率和穩(wěn)定性。本研究不僅提出了一種新的生物催化膜制備方法和多功能膜新概念,解決了傳統(tǒng)分離膜對水中微量污染物去除效率不高、生物催化膜穩(wěn)定性不佳等問題,為生物催化膜的制備和應用打開了新思路,而且制備的多功能膜和雙面EMR在深度尾水處理及家用凈水器上具有較大的應用潛力。
[Abstract]:Biocatalysis membrane can greatly improve the reaction efficiency by combining the selective transport of substances with chemical reaction, and has a wide application prospect in medicine, food, water treatment and other fields. However, the enzyme carrier rate in the preparation process of biocatalysis membrane is not high at present. The low activity of enzyme and the degradation of membrane properties limit its application. In view of the above problems, this paper focuses on simultaneous separation, adsorption, and so on. Preparation of catalytic multifunctional membrane and its application in water treatment. The research contents and results are divided into the following two parts: 1) inspired by mussel mucin and membrane structure. The laccase was encapsulated in the supporting layer of nanofiltration membrane by reverse filtration, and then encapsulated in the membrane by polydopamine PDA-bionic coating. The multifunctional membrane with three functions of interception, catalysis and adsorption was prepared. It was applied to the removal of micro-pollutants in water. Take the removal of bisphenol A and BPA in water as an example. (the concentration of BPA in the feedstock solution is 10 mg 路L ~ (-1) BPA). The removal rate of BPA by NF270 multifunctional membrane is 84.3 鹵7.3%, which is much higher than that of traditional Fenton oxidation (55%). Studies of synergistic mechanisms show that, Nanofiltration membrane itself has the function of intercepting some pollutants, which reduces the catalytic load of enzyme, while the adsorption function of membrane and PDA coating enriches the unintercepted trace pollutants in the membrane and prolongs the reaction time of substrate and enzyme molecule. At the same time, the catalytic function of biological enzymes broke the limit of "adsorption saturation" of membrane materials and made the "adsorption-catalysis" process go on continuously. In order to solve the problem of enzyme leakage caused by the lack of compactness of PDA coating during the long-term use of multifunctional membrane, the amount and activity of enzyme carrier were further increased. A novel biomimetic coating was formed in the supporting layer of enzyme carrier nanofiltration membrane by using dopamine / polyvinyleneimide (DA / PEI) and dopamine / copper ion (DA / Cu ~ (2)) coprecipitation, respectively. The results show that coprecipitation not only shortens the time of DA self-polymerization. Enhancing the homogeneity and stability of PDA coating can greatly reduce enzyme leakage, increase encapsulation efficiency and increase enzyme activity. The special sandwich structure of "separating layer laccase-supporting layer / encapsulation layer" makes the multifunctional membrane have catalytic activity on both sides. It can be used to construct a bihedral enzyme membrane reactor (EMRs) to efficiently remove pollutants in water. The EMR prepared by multifunctional membrane prepared by DA/Cu2 coprecipitation has the highest removal rate of BPA, and because of the forced convection in the flow mode, the product can be removed effectively. The stability of EMR was greatly improved by changing the balance between membrane stability and removal efficiency. It was found that the enzyme activity and substrate / product mass transfer were regulated by regulating the enzyme load, immobilized enzyme location, enzyme activity and substrate / product mass transfer. This study not only proposed a new method of preparing biocatalysis membrane and a new concept of multifunctional membrane, but also solved the low removal efficiency of trace pollutants in water by traditional separation membrane. The instability of biocatalysis membrane has opened a new way for the preparation and application of biocatalysis membrane, and the multifunctional membrane and double-sided EMR have great application potential in deep tail water treatment and household water purifier.
【學位授予單位】：中國科學院大學(中國科學院過程工程研究所)
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TB383.2;TQ085.4

【相似文獻】

相關期刊論文 前10條

1 劉麗宏;;《功能膜及其應用》新書已出版發(fā)行[J];膜科學與技術;2013年02期

2 ;中日功能膜交流會在滬召開[J];水處理技術;1984年06期

3 賀倩;郭文迅;彭蕩;何姣;;淀粉基可降解高吸水性功能膜的制備及性能[J];石油化工;2011年06期

4 趙宏生;陳煒;翁端;李恒德;;玻璃表面功能膜的研究進展[J];材料導報;2004年06期

5 劉富;陶慷;杜旭東;黃燕;薛立新;;功能膜材料發(fā)展概況及應用進展(待續(xù))[J];化工生產與技術;2012年06期

6 徐應明,王榕樹;介孔鈦硅分子篩表面功能膜的制備及對水體中鉛的去除作用[J];高等學�；瘜W學報;1999年07期

7 袁飛;;聚酰胺復合反滲透功能膜的研究及應用[J];廣東化工;2011年09期

8 劉富;陶慷;杜旭東;黃燕;薛立新;;功能膜材料發(fā)展概況及應用進展(續(xù)完)[J];化工生產與技術;2013年01期

9 任勝利;金繼軍;劉英華;;長效流滴功能膜工業(yè)化生產的研究[J];塑料;2008年01期

10 馮素波;嵇書偉;董鳳龍;王立祥;李曉杰;;建筑玻璃功能膜的制備及檢驗方法[J];玻璃;2011年10期

相關會議論文 前4條

1 ;前言[A];第四屆中國膜科學與技術報告會論文集[C];2010年

2 洪軍;A.A.Mosavi-Movahedi;H.Ghourchian;A.A.Saboury;S.Rezaei-Zarchi;;氧化還原蛋白質在納米簇功能膜修飾金電極上的直接電化學[A];第十一次中國生物物理學術大會暨第九屆全國會員代表大會摘要集[C];2009年

3 張海濤;韓梅;崔學軍;王洪艷;;功能膜材料耐水性的多尺度關聯(lián)建模探索[A];第十屆全國計算(機)化學學術會議論文摘要集[C];2009年

4 孫俊奇;;功能性層狀組裝膜的快速構筑[A];2009年全國高分子學術論文報告會論文摘要集（上冊）[C];2009年

相關重要報紙文章 前5條

1 李榮;凱鑫森建全國最大功能膜產業(yè)基地[N];中國化工報;2011年

2 張瑾 記者 吳長鋒;新型復合軟包裝功能膜開始批量面市[N];科技日報;2012年

3 駐太倉首席記者 徐允上;功能膜 讓電容能量增強5000倍[N];蘇州日報;2011年

4 景后寅;高檔功能膜將主導我國膜市場[N];江蘇農業(yè)科技報;2006年

5 本報記者 景后寅;高檔功能膜行情看好 推廣佳機已至[N];經濟日報.農村版;2006年

相關碩士學位論文 前2條

1 李森森;基于卟啉功能膜的制備及其對鎘離子的檢測[D];天津工業(yè)大學;2017年

2 曹曉彤;基于聚多巴胺仿生涂層的分離、吸附、催化多功能膜的制備、優(yōu)化及應用[D];中國科學院大學(中國科學院過程工程研究所);2017年

，

本文編號：1599153