本文選題：藍多銅氧化酶　切入點：直接電子遷移　出處：《新疆師范大學》2017年碩士論文　論文類型：學位論文

【摘要】：藍多銅氧化酶作為酶燃料電池陰極和酶電化學傳感器的電催化劑近年來得到了廣泛的應用,但一些缺陷限制了它在工業(yè)生產(chǎn)中的進一步應用,例如酶基電子器件制備工序復雜,力學、熱穩(wěn)定性以及抗干擾性差等。更重要的是載體上固定酶分子難以實現(xiàn)其活性中心與導電基體之間的有效電子導通。針對上述問題,本文選擇幾種含有疏水芳環(huán)或芳雜環(huán)以及含鍵合基團的分子(芳族化合物作為單體聚合得到的導電聚合物,殼聚糖的衍生物以及含雙重鍵合基團的芳族化合物)與納米材料復合的方式制備固酶載體,利用固酶載體與酶分子間的化學偶聯(lián),配位絡合以及物理吸附等相互作用的協(xié)同效應,使得蛋白質(zhì)分子以特定取向或是隨機排列在載體表面。本論文使用電化學和光譜學方法研究和評估了載體表面固定酶-導電基體間的直接電化學,固酶電極對特定底物的催化性能以及酶-載體間相互作用對酶催化性能的影響,并評估了這些電極對特定底物的傳感性能。1以芳環(huán)功能化納米金粒子和殼聚糖衍生物混合所得復合物作為固酶載體,利用前述協(xié)同效應,不但能使酶分子采取特定排列形式固載于固酶載體表面,具有良好的力學穩(wěn)定性,還促進了酶電極間的直接電子遷移。并評估了該納米復合物固定漆酶基電極對兒茶酚的傳感性能�；诠潭ㄆ崦讣{米復合物的兒茶酚電化學傳感器擁有靈敏度高,對底物特異選擇性和低檢測限的優(yōu)勢,而且這種傳感器檢測兒茶酚不受到共存氧分子的干擾。2以聚苯胺-草酸鈷(CoC_2O_4)作為固定酶載體,制備得到藍多銅氧化酶基電極,研究了該固酶電極的直接電化學以及催化氧還原性能。實驗結(jié)果表明:該固酶電極在不含電子介體的溶液中可以實現(xiàn)酶活性中心T2與導電基體之間的直接電子遷移,而且可以有效地催化氧還原,但催化反應受制于酶吸附氧分子形成的中間產(chǎn)物分解為水分子的過程。3采用羧甲基殼聚糖化學偶聯(lián)磁性四氧化三鐵磁性納米粒子作為固酶載體,制備了固定漆酶基電極,研究了這種固酶電極的有效電子遷移和催化氧還原性能。實驗結(jié)果表明:只是單純依靠酶-載體間化學偶聯(lián)使酶分子隨機分布在載體表面的磁性納米粒子固酶電極,只有加入電子介體才能得以實現(xiàn)酶-電極間的有效電子遷移和有效催化氧還原,其催化氧還原反應的決速步是電子介體的擴散過程。
[Abstract]:Blue polycopper oxidase has been widely used as an electrocatalyst for enzyme fuel cell cathodes and enzyme electrochemical sensors in recent years, but some defects limit its further application in industrial production, such as the complex preparation process of enzyme based electronic devices. Mechanics, thermal stability and poor anti-interference. More importantly, it is difficult for immobilized enzyme molecules on the carrier to realize effective electronic conduction between their active center and conductive matrix. In this paper, several kinds of molecules containing hydrophobic aromatic rings or aromatic heterocycles and containing bonding groups (aromatic compounds) were selected as conductive polymers by monomer polymerization. Chitosan derivatives and aromatic compounds containing double binding groups) were used to prepare immobilized enzyme carriers by combining with nanomaterials, and the immobilized enzyme carriers were chemically coupled with enzyme molecules. The synergistic effects of coordination complexation and physical adsorption. In this paper, electrochemical and spectroscopic methods were used to study and evaluate the direct electrochemistry between the immobilized enzyme and conductive matrix on the surface of the carrier. The catalytic activity of solid enzyme electrode to specific substrate and the effect of enzyme carrier interaction on enzyme catalytic performance. The sensing performance of these electrodes to specific substrates was also evaluated. 1. The complexes of aromatic ring functionalized gold nanoparticles and chitosan derivatives were used as carriers for enzyme fixation, and the synergistic effects were utilized. Not only can the enzyme molecules be immobilized on the surface of the enzyme carrier in a specific arrangement form, but also have good mechanical stability. It also promoted the direct electron transport between enzyme electrodes, and evaluated the sensing performance of the nano-complex immobilized laccase based electrode to catechol. The electrochemical sensor of catechol based on the immobilized laccase nanocomplex has high sensitivity. The biosensor was not interfered by coexisting oxygen molecules. 2. Polyaniline-Cobalt oxalate CoC2O4) was used as the carrier of the enzyme to prepare the blue polycopper oxidase electrode. The direct electrochemistry and catalytic oxygen reduction of the electrode were studied. The experimental results show that the direct electron transfer between the enzyme active center T2 and the conductive matrix can be realized in the solution without electron medium. Moreover, oxygen reduction can be effectively catalyzed, but the catalytic reaction is restricted by the process of decomposing the intermediate products formed by enzyme adsorbing oxygen molecules into water molecules. 3. 3. Carboxymethyl chitosan chemically coupled magnetic ferromagnetic nanoparticles are used as solid enzyme carriers. Immobilized laccase based electrodes were prepared. The effective electron transport and catalytic oxygen reduction properties of this kind of enzyme electrode were studied. The results showed that the magnetic nanoparticles immobilized enzyme electrode was only dependent on the chemical coupling between the enzyme and the carrier to make the enzyme molecule distribute randomly on the surface of the carrier. Only the addition of electronic medium can realize the effective electron transfer between enzyme and electrode and the effective catalytic oxygen reduction. The fast step of the catalytic oxygen reduction is the diffusion process of the electron medium.
【學位授予單位】：新疆師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O657.1

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