本文選題：水處理 + 電輔助微生物��； 參考：《天津工業(yè)大學》2017年碩士論文

【摘要】：由于偶氮染料在印染、造紙等工業(yè)生產(chǎn)中的廣泛使用,造成全世界染料廢水大部分都是偶氮染料廢水,并且其廢水具有高毒性、高色度、成分復雜等特點對環(huán)境危害極大,成為公認的難處理廢水。研究發(fā)現(xiàn),單純的物理、化學或生物方法,雖然對偶氮染料有一定的降解,但使用任一種處理手段都不太理想。本文將電化學和微生物體系相結合,組成電輔助微生物體系還原污染物。前期研究發(fā)現(xiàn)電輔助微生物對氯酚類難降解污染物有良好的去除效果,但是否對偶氮染料也能達到較好的去除,以及降解過程和機理,目前較少,需要進行深入研究。本文選取偶氮染料活性艷紅X-3B為處理對象,首先對比研究了電輔助微生物體系(EAMS)、電化學體系(ECS)和微生物體系(MS)厭氧條件下對活性艷紅X-3B的降解性能。其次在EAMS中研究關鍵影響因素,包括外電壓、溫度、硫酸根以及硝酸根對降解活性艷紅X-3B的影響,確定最佳電壓以及反應的活化能,并通過紫外-可見分光光度計、GC-MS對降解產(chǎn)物進行分析,推測EAMS對活性艷紅X-3B降解機理。最后,在EAMS中加入氧化還原介體蒽醌-2-磺酸鹽(AQS),研究AQS對偶氮染料降解的強化效果以及反應體系的電流變化,并對其強化機理進行分析。研究結果表明:與ECS和MS相比,EAMS中電化學催化和微生物降解技術對染料降解存在協(xié)同作用,大大提升了活性艷紅X-3B的降解率。不同電壓下染料的降解符合一級動力學特征,且0.4V電壓下染料降解最快。在一定溫度范圍內(nèi),溫度升高有助于染料的降解,由阿倫尼烏斯方程估算得EAMS降解活性艷紅X-3B的活化能為60.526kJ/mol,說明染料降解主要依靠微生物的氧化還原,而不是生物吸附。硫酸根對染料還原影響不大,只有當濃度高達600mg/L后,染料降解率略微降低。硝酸根對染料還原影響較大,加入任何濃度的硝酸鹽,前6h染料降解速率均下降,主要原因是反硝化菌奪電子能力較強,硝酸根優(yōu)先被還原。在EAMS中,活性艷紅X-3B中偶氮鍵首先斷裂,三嗪結構以及萘環(huán)結構也可被降解,苯環(huán)部分被降解為烷烴,并且有新的苯類物質產(chǎn)生。對EAMS和MS中活性艷紅X-3B的產(chǎn)物進行GC-MS分析,發(fā)現(xiàn)EAMS中主要產(chǎn)物為無毒的烷烴類物質,而MS中主要產(chǎn)物為有毒的苯類物質。當c(AQS)為0.050mmo1/L時,染料降解最快,一級動力學常數(shù)為1.962 h-1,是未添加AQS的(0.2644 h-1)7.42倍。加入AQS后,體系中電流升高,說明AQS加快了降解過程中電子傳遞速率。研究顯示,AQS的加入實現(xiàn)了電極-遠離電極的微生物-染料之間多相反應界面遠程電子傳遞過程,使整個體系的微生物都可以快速發(fā)揮作用,達到強化降解偶氮染料。
[Abstract]:Due to the widespread use of azo dyes in printing and dyeing, papermaking and other industries, most of the world's dye wastewater is azo dye wastewater, and its wastewater has the characteristics of high toxicity, high chromaticity and complex composition, which is harmful to the environment. Become a recognized refractory wastewater. It is found that only physical, chemical or biological methods are not ideal for the degradation of azo dyes. In this paper, electrochemistry and microbial system are combined to form electroassisted microbial system to reduce pollutants. Previous studies have found that electroassisted microbes have a good removal effect on chlorophenol refractory pollutants, but whether to achieve better removal of azo dyes, as well as the degradation process and mechanism, is less, so it needs to be further studied. In this paper, the reactive brilliant red X-3B of azo dyes was selected as the treatment object. Firstly, the biodegradability of reactive brilliant red X-3B was studied under the anaerobic conditions of electroassisted microbial system (EAMSG), electrochemical system (ECS) and microbial system (MSS). Secondly, the key influencing factors were studied in EAMS, including external voltage, temperature, the influence of sulfate and nitrate on the degradation of reactive brilliant red X-3B, and the optimum voltage and the activation energy of the reaction were determined. The degradation products were analyzed by GC-MS with UV-Vis spectrophotometer, and the degradation mechanism of reactive brilliant red X-3B was inferred by EAMS. Finally, the enhancement effect of AQS on the degradation of azo dyes and the current change of the reaction system were studied by adding the redox medium, anthraquinone -2-sulfonate, to EAMS, and the strengthening mechanism was analyzed. The results showed that compared with ECS and MS, the degradation rate of reactive brilliant red X-3B was greatly enhanced by the synergistic effect of electrochemical catalysis and microbial degradation on the degradation of dyes. The degradation of dyes at different voltages accords with the first-order kinetic characteristics, and the degradation of dyes is the fastest at 0.4 V voltage. The activation energy of reactive brilliant red X-3B degraded by EAMS was estimated to be 60.526kJ / mol from Arrhenius equation, which indicated that the degradation of dyes mainly depended on the redox of microorganisms, not on biosorption. Sulfate had little effect on the reduction of dyes, but the degradation rate of dyes decreased slightly when the concentration was as high as 600mg/L. Nitrate had a great effect on the reduction of dyes. The degradation rate of dyes decreased 6 hours before adding nitrate at any concentration. The main reason was that denitrifying bacteria had strong electron capture ability and nitrate was reduced preferentially. In EAMS, the azo bond in reactive brilliant red X-3B breaks first, the triazine structure and naphthalene ring structure can also be degraded, the benzene ring is partially degraded to alkane, and new benzenes are produced. The products of reactive brilliant red X-3B in EAMS and MS were analyzed by GC-MS. It was found that the main products of EAMS were nontoxic alkanes, while the main products of MS were toxic benzenes. When 0.050mmo1/L was 0.050mmo1/L, the dye degradation was the fastest, and the first-order kinetic constant was 1.962 h-1, which was 7.42 times as high as 0.2644h-1H ~ (-1) without AQS. After the addition of AQS, the current in the system increased, which indicated that AQS accelerated the electron transfer rate in the degradation process. The results show that the addition of AQS can realize the long-distance electron transfer process between the electrode and the microorganism far away from the electrode and the multiphase reaction interface, so that the microorganism of the whole system can play a rapid role to enhance the degradation of azo dyes.
【學位授予單位】：天津工業(yè)大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X703

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