【摘要】：木質(zhì)素作為植物骨架的三大主要成分之一,在煙草中的含量在4-8%,這部分木質(zhì)素是造成煙氣中木質(zhì)氣息重,以至于產(chǎn)生強烈的嗆感、咳嗽、灼喉等不適的主要原因之一;且熱解時會產(chǎn)生兒茶酚、烷基兒茶酚等引起澀口且有促癌活性的物質(zhì),影響卷煙品質(zhì)和安全。因此,在煙草薄片制備過程中的木質(zhì)素的降解和脫除有利于提升其品質(zhì)。漆酶能選擇性地催化木質(zhì)素降解,不會產(chǎn)生有毒物質(zhì),并且生產(chǎn)通常在低溫、常壓的溫和條件下進行,易于實現(xiàn)工業(yè)化。開展漆酶脫除煙梗中木質(zhì)素以制備高品質(zhì)的煙草薄片,并利用木質(zhì)素模型物來探討漆酶降解煙梗中木質(zhì)素的機理,對提高煙草薄片的品質(zhì)提供工藝參數(shù)和理論指導具有良好的意義。研究了XSLacc、SUKALacc、YCLacc、DENYKEM PAP-5、DENYKEM INDICLEAN 6G+、GrenLacc 6種不同產(chǎn)地漆酶對煙梗中木質(zhì)素的降解的影響,結果表明DENYKEM PAP-5對煙梗中木質(zhì)素降解效果最好。再分別從固液比、反應溫度、pH、反應時間、搖床轉速等工藝參數(shù)對DENYKEM PAP-5酶解工藝條件進行優(yōu)化,結果表明酶解過程中,固液比越小,酶解效果越好,考慮到酶解率與成本,實驗選擇的固液比為3.0:100;在漆酶用量1.3%,反應溫度為50℃,pH=5.0,反應時間為4h,搖床轉速為150 r/min時,煙梗中木質(zhì)素的降解率為15.92%。研究了香草酸、丁香醛、對羥基苯乙酮等9種天然介體的添加對漆酶降解煙梗中木質(zhì)素的影響,結果表明,丁香酸對煙梗中木質(zhì)素的降解有一定的促進作用,降解率為16.64%。優(yōu)化的酶解煙梗中木質(zhì)素工藝經(jīng)工廠中試放大試驗后專家評吸,由煙梗制備的煙草薄片的煙氣細膩感有提升,木質(zhì)雜氣和枯焦雜氣下降比較明顯。以異丁香酚和2-溴-4-羥基苯乙酮等物質(zhì)為原料,在DMF/NaH體系中合成了酚型β-O-4二聚體木質(zhì)素模型物(Ⅰ),分別研究了反應溫度和反應時間對目標產(chǎn)物收率的影響,結果表明反應時間為50℃,反應時間為60 min,模型物(Ⅰ)的收率可以達到75.8%;以4-甲氧基-2-溴苯乙酮和2-甲氧基苯酚為原料,在K2CO3和丙酮體系中合成非酚型β-O-4二聚體模型物(Ⅱ);采用辣根過氧化物酶(HRP)催化異丁香酚合成包含α-O-4和β-5鍵的香豆?jié)M型二聚體木質(zhì)素模型物(Ⅲ);然后以香豆?jié)M型二聚體模型物(Ⅲ)為底物,在過硫酸鉀和硫酸亞鐵的氧化還原引發(fā)體系中催化合成了包含5-5、α-O-4、β-5鍵的四聚體木質(zhì)素模型物(Ⅳ),研究了溶劑比、反應時間、反應溫度對目標產(chǎn)物收率的的影響,結果表明:丙酮/水為2:1,反應時間為10 min,反應溫度為80℃時,模型物(Ⅳ)的收率達到33.8%。分別對合成的模型物進行高分辨質(zhì)譜(HRMS)、元素分析(EA)、核磁共振光譜(NMR)等表征,確定合成的模型物的結構。以酚型β-O-4二聚體模型物(Ⅰ)、非酚型β-O-4二聚體(Ⅱ)和含β-5、5-5鍵的酚型四聚體模型物(Ⅳ)作為研究對象,利用優(yōu)化的酶解條件進行酶解,結果表明:漆酶可以導致木質(zhì)素酚型模型物(Ⅰ)中β-O-4鍵的部分斷裂,從而導致木質(zhì)素的降解;而漆酶對于非酚型β-O-4二聚體(Ⅱ)和含β-5、5-5鍵的酚型四聚體模型物(Ⅳ)中的聯(lián)接鍵都不能發(fā)生斷裂。可以推斷漆酶因為斷裂酚型木質(zhì)素中的β-O-4鍵而導致木質(zhì)素的部分降解而脫除。
[Abstract]:As one of the three main components of plant skeleton, lignin content in tobacco is 4-8%. This part of lignin is caused by smoke lignin heavy aroma, so that strong choke, cough, burning throat and other discomfort one of the main reasons; and pyrolysis will produce catechins, alkyl catechins and other astringent mouth and carcinogenic substances. Laccase can selectively catalyze the degradation of lignin without producing toxic substances, and the production is usually carried out under mild conditions at low temperature and atmospheric pressure, which is easy to realize industrialization. The lignin was used to prepare high quality tobacco slices and the lignin model was used to study the mechanism of lignin degradation in tobacco stem by laccase. It is of great significance to provide technological parameters and theoretical guidance for improving the quality of tobacco slices. XSLacc, SUKALacc, YCLacc, DENYKEM PAP-5, DENYKEM INDICLEAN 6G+, GrenLacc from six different producing areas were studied. The results showed that DENYKEM PAP-5 had the best effect on lignin degradation in tobacco stem. Then the enzymatic hydrolysis conditions of DENYKEM PAP-5 were optimized from the aspects of solid-liquid ratio, reaction temperature, pH, reaction time and rotational speed of shaker. The results showed that the smaller the solid-liquid ratio, the better the enzymatic hydrolysis effect. Considering the enzymatic hydrolysis rate and cost, the solid-liquid ratio was 3.0:100, the degradation rate of lignin in tobacco stem was 15.92% when laccase dosage was 1.3%, reaction temperature was 50%, pH was 5.0, reaction time was 4 h, and the rotational speed of shaker was 150 r/min. The degradation of wood in tobacco stem by laccase of 9 natural mediators, such as vanillic acid, eugenol aldehyde and p-hydroxyphenylacetone, was studied. The results showed that eugenoic acid could promote the degradation of lignin in tobacco stem, and the degradation rate was 16.64%. The optimized enzymatic lignin hydrolysis process was evaluated by experts after pilot scale-up test in a factory. The smoke fineness of tobacco leaf prepared from tobacco stem was improved, and the lignin impurity and charred impurity decreased significantly. Phenolic beta-O-4 dimer lignin model compound (I) was synthesized from isoeugenol and 2-bromo-4-hydroxyacetophenone in DMF/NaH system. The effects of reaction temperature and time on the yield of the target product were studied. The results showed that the yield of the model compound (I) could reach 75. 8%; non-phenolic beta-O-4 dimer model compounds (II) were synthesized from 4-methoxy-2-bromoacetophenone and 2-methoxyphenol in K2CO3 and acetone systems; isoeugenol was catalyzed by horseradish peroxidase (HRP) to synthesize coumarin dimer lignin model compounds (III) containing alpha-O-4 and beta-5 bonds; then coumarin dimer model compounds (III) were prepared by coumarin dimer model compounds (HRP). A tetramer lignin model compound (IV) containing 5-5, a-O-4, and a-5 bond was synthesized by using potassium persulfate and ferrous sulfate as substrates. The effects of solvent ratio, reaction time and reaction temperature on the yield of the target product were studied. The results showed that acetone/water ratio was 2:1, reaction time was 10 min, reaction temperature was 80 C. High resolution mass spectrometry (HRMS), elemental analysis (EA), nuclear magnetic resonance spectroscopy (NMR) were used to characterize the synthesized model compounds, and the structure of the synthesized model compounds was determined. The results showed that laccase could induce the partial breakage of the beta-O-4 bond in the phenolic lignin model compound (I) and lead to the degradation of lignin, while laccase could not induce the bond formation in the non-phenolic beta-O-4 dimer (II) and the phenolic tetramer model compound (IV) containing the beta-5,5-5 bond. Fracture. It can be deduced that laccase is partially degraded by breaking the beta-O-4 bond in phenolic lignin.
【學位授予單位】：華南理工大學
【學位級別】：碩士
【學位授予年份】：2016
【分類號】：Q814;O636.2

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