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  本文選題：木質(zhì)素　切入點：愈創(chuàng)木酚　出處：《湖南大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

【摘要】：木質(zhì)素是一種自然界中儲量僅次于纖維素的有機高分子物質(zhì),能夠以每年500億噸左右的速度再生。造紙制漿工業(yè)每年要從植物中分離出大約1.4億噸纖維素,同時得到5000萬噸左右的木質(zhì)素副產(chǎn)品;分散劑、吸附劑/解吸劑、石油回收助劑、瀝青乳化劑等工業(yè)產(chǎn)品中也用到了木質(zhì)素及其衍生物,迄今為止,每年有超過95%的木質(zhì)素以“黑液”形式直接排入江河或濃縮后燒掉,很少得到有效利用。反膠束(reversed micelle)或逆膠束、反膠團是表面活性劑溶于非極性的有機溶劑內(nèi)濃度超過臨界膠束濃度(CMC)時,自發(fā)形成的穩(wěn)定澄清的均相W/O納米尺寸聚集體。反膠束中,表面活性劑的非極性疏水基團與外部非極性的有機溶劑接觸,極性基團排列在內(nèi)圍繞成一個具有溶解極性物質(zhì)能力的極性核(polar core)。極性核溶解水后,就形成了“水池”(water pool),反膠束的這種結(jié)構(gòu)能夠同時增溶親水性的酶和疏水性的底物,模擬生物分子中酶反應(yīng)的天然微環(huán)境,使得酶在其中表現(xiàn)出優(yōu)于水介體中反應(yīng)的活性。因此,近年來反膠束酶催化體系得到了廣泛的關(guān)注和研究。本課題將親脂性的木質(zhì)素模式物愈創(chuàng)木酚與親水性的漆酶溶解于反膠束溶液中,探究反膠束中漆酶對木質(zhì)素的作用機制,并通過實驗建立改變反應(yīng)條件反膠束中漆酶的酶活變化和最佳反應(yīng)條件下漆酶對愈創(chuàng)木酚的催化效率、建立反應(yīng)的動力學(xué)模型和動力學(xué)參數(shù),深入研究反膠束中漆酶催化愈創(chuàng)木酚的反應(yīng)機理。本文的具體研究工作及成果包括以下內(nèi)容:本課題首先構(gòu)建CTAB,Tween-80,AOT以及鼠李糖脂四種反膠束體系,然后研究CTAB,Tween-80,AOT以及鼠李糖脂的最佳表面活性劑濃度、相對應(yīng)的最佳含水率條件下漆酶催化愈創(chuàng)木酚的效率和動力學(xué)機制。并且對反膠束體系中酶催化愈創(chuàng)木酚降解的反應(yīng)機制進行研究,測定反應(yīng)產(chǎn)物,參照已有研究,分析漆酶催化愈創(chuàng)木酚的反應(yīng)機制。最后引入甘油對鼠李糖脂構(gòu)建的反膠束體系進行改性,構(gòu)建鼠李糖脂/異辛烷/正己醇/甘油/水反膠束體系并且篩選出最佳表面活性劑濃度以及對應(yīng)的最大增溶水量,測定優(yōu)化反應(yīng)條件下反膠束中漆酶催化愈創(chuàng)木酚的效率,對甘油改性前后漆酶的催化效率進行分析比較。通過對不同反膠束環(huán)境中漆酶酶活的對比分析,確定在CTAB,Tween-80,AO T以及鼠李糖脂4種表面活性劑構(gòu)建的反膠束體系中,適合酶解反應(yīng)的最佳表面活性劑濃度和對應(yīng)的最佳含水率W0分別為:CTAB濃度20mmol/L,W0=20;Tween 80濃度50 mmo l/L,W0=25;AO T濃度30 mmo l/L,W0=10;鼠李糖脂濃度10mmo l/L,W0=30。在陽離子、陰離子和非離子幾種類型的表面活性劑中,同屬于陰離子表面活性劑的AOT和鼠李糖脂構(gòu)建的反膠束體系的底物降解率均高于CTAB和Tween 80體系,說明陰離子表面活性劑更適宜漆酶的反應(yīng),并且同屬于陰離子表面活性劑的生物表面活性劑鼠李糖脂構(gòu)建的反膠束體系中漆酶的活性和穩(wěn)定性均高于AOT反膠束,在最適含水率條件下制備構(gòu)建的反膠束體系中,反應(yīng)6h后,各反膠束體系在底物愈創(chuàng)木酚濃度為1mmol/L時,CTAB、Tween80、AO T和鼠李糖脂4種表面活性劑構(gòu)建的反膠束體系中木質(zhì)素模式物的漆酶降解效率分別為21.33%、30.85%、36.02%、65.45%。四種反膠束體系中漆酶對愈創(chuàng)木酚的催化反應(yīng)遵循均Michaelis-Menten動力學(xué)。漆酶通過參與愈創(chuàng)木酚的解聚和聚合反應(yīng),將愈創(chuàng)木酚催化為水溶性底物4-鄰甲基苯酚。通過甘油對鼠李糖脂構(gòu)建的反膠束體系進行改性,可以增加反膠束體系膠團半徑,有利于反膠束中漆酶分子的溶入,增強反膠束中酶構(gòu)象的穩(wěn)定性,有利于提高漆酶的活性和穩(wěn)定性。
[Abstract]:Lignin is a kind of nature reserves after cellulose organic polymer material, to 500 tons per year. The regeneration rate of paper pulp industry each year to about 1.4 tons of cellulose were isolated from the plant, and 50 million tons of lignin by-product; dispersant, adsorption / desorption agent, oil recovery agent asphalt emulsifier and other industrial products were also used in lignin and its derivatives, so far, more than 95% of the wood known as "black liquor" form directly into rivers or concentrated burned every year, have not been effectively used. The reverse micelles (reversed micelle) or reverse micelles, reverse micelles is a surface active agent is dissolved in an organic solvent within the concentration exceeds the critical micelle concentration (CMC), homogeneous W/O nanoparticles size of the spontaneous formation of stable clarification. In reverse micelles, non-polar hydrophobic groups and surfactant Non polar organic solvent exposure outside, polar groups, arranged around the polar nucleus of a solution with polar material capability (polar core). The polar nucleus dissolved water, formed a "pool" (water pool), the structure of reverse micelles can also hydrophilic and hydrophobic solubilization enzyme the substrate, enzyme reaction simulating molecular biology in natural micro environment, the enzyme showed superior water reaction mediator in activity in them. Therefore, in recent years the reversed micellar enzymatic system has received wide attention and research. This paper will lipophilic lignin model compounds guaiacol and hydrophilic the laccase dissolved in reverse micelles, explore the laccase in reverse micelles on the lignin mechanism, and through the experiment to establish change reaction conditions in reverse micelles laccase enzyme catalytic efficiency change and the optimum reaction conditions of laccase of guaiacol, establish The kinetic model and kinetic parameters of the reaction, the catalytic reaction mechanism of guaiacol laccase in-depth study in reverse micelles of guaiacol. The specific research work and achievements of this paper include the following contents: firstly the construction of CTAB, Tween-80, AOT four and rhamnolipid reverse micellar system, then CTAB, Tween-80, AOT and the best surfactant rhamnolipid glycolipid surfactant concentration efficiency and kinetics of laccase catalyzed conditions of guaiacol guaiacol corresponding to the optimum water ratio. And study the reaction mechanism of reverse micelles enzyme catalyzed degradation of guaiacol, determination of reaction products, according to the existing research, analysis of the reaction mechanism catalyzed by guaiacol. Finally the introduction of reverse micelles the system construction of the glycerol rhamnolipid was modified to construct rhamnolipid / isooctane / hexanol / glycerol / water reverse micelles and selected the best surfactant concentration And the maximum water solubilization efficiency, catalytic determination of guaiacol under the optimal reaction conditions of laccase in reverse micelles of guaiacol, glycerol modified laccase catalytic efficiency of comparison. Through the contrastive analysis of different reverse micelles laccase activity in the environment, in CTAB, Tween-80, AO, T and rhamnolipid 4 surface active agent construction in the reverse micelles, the best surface activity suitable for enzymatic hydrolysis agent concentration and the optimum water ratio corresponding to the W0 were: CTAB concentration 20mmol/L, W0=20; Tween 80 concentration of 50 MMO l/L, W0=25 AO; T W0=10; l/L MMO 30 concentration, the concentration of rhamnolipid 10mmo l/L, W0=30. in the surface of cation. The active agent of anionic and nonionic types of substrate degradation of reverse micelles constructed belong to anionic surfactant AOT and rhamnolipid were higher than that of CTAB and Tween 80 system, that the anionic surface active Agent is more suitable for the laccase reaction, laccase reverse micelles of rhamnolipid biosurfactant and belong to anionic surfactant in the construction of the activity and stability of AOT were higher than that of reverse micelles, reverse micelles in the optimum moisture content under the condition of the preparation of construction, after reaction of 6h, the reverse micelles in the substrate guaiacol concentration of 1mmol/L, CTAB, Tween80, laccase degradation efficiency of AO T and rhamnolipid 4 surfactant constructed in the reverse micelles of lignin model compounds were 21.33%, 30.85%, 36.02%, four 65.45%. of laccase in reverse micelles catalysis of guaiacol reaction followed Michaelis-Menten kinetics. Laccase by participating in guaiacol depolymerization and polymerization, the guaiacol catalyzed water soluble o-cresol. The substrate 4- was modified by reverse micelles of glycerol on the construction of rhamnolipid can increase Reverse micelle micelle radius, in favor of laccase in reverse micelles into the molecular conformation of the enzyme, enhance the stability of reverse micelles, could enhance the laccase activity and stability.

【學(xué)位授予單位】：湖南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：O643.3;X703

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