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微生物燃料电池降解高氯酸盐特性及介体调控机理研究

发布时间:2018-07-17 19:10
【摘要】:高氯酸盐是一种持久性有毒物质,其使用和生产过程中的违规排放带来了严重的环境污染问题。作为一种新型处理技术,微生物燃料电池(MFC)可在降解污染物的同时输出电能,已成为环境能源技术的研究重点。因此,本研究以高氯酸钠为模型污染物,开展了单室MFC反应器处理高氯酸盐废水的研究。通过优化MFC反应器的启动条件,考察了不同共存电子受体、不同氧化还原介体对MFC性能的影响,并探讨了介体调控MFC性能的电子传递机理。MFC经过140 h连续运行,高氯酸盐还原速率和产生的电压趋于稳定;初始高氯酸盐浓度为150 mg·L-1和以乙酸钠作为碳源时MFC的性能较好。不同种类、浓度的电子受体,对MFC性能产生了不同的影响。硝酸盐和氯酸盐的存在均抑制了高氯酸盐的还原,当硝酸盐和氯酸盐还原完全后高氯酸盐开始还原,在硝酸盐还原时产生了较高的电压,而在氯酸盐还原时产生了较低的电压,当硝酸盐和氯酸盐还原完全时电压恢复到58 m V左右;高浓度硫酸盐对MFC性能产生了不可恢复的抑制。热力学分析结果表明,硝酸盐、氯酸盐和高氯酸盐之间是电子竞争关系;电化学分析表明,硝酸盐和氯酸盐还原时提高了阳极电化学活性。通过分别考察抑制剂CuCl_2、NaN_3、双香豆素、鱼藤酮、二盐酸喹吖因水化合物(QDH)、二环己基碳二亚胺(DCCD)、羰基氰基-3-氯苯腙(CCCP)和辣椒素对MFC性能的影响,结果表明NADH脱氢酶、NADH-Q还原酶、甲基萘醌、Fe-S蛋白(复合体Ⅰ)、ATP合成酶和FAD还原酶是MFC阳极呼吸链的重要组成部分。氧化还原介体刃天青、中性红、亚甲基蓝、蒽醌2,6-二磺酸钠(AQDS)和铁氰化钾的添加,显著的提高了MFC的性能。以刃天青为例,探讨了氧化还原介体对MFC性能调控机理。结果表明:刃天青的存在降低了微生物胞外多糖分泌和增加了腐殖酸分泌,从而减少了从微生物胞外到阳极的电子转移阻力;刃天青在MFC阳极呼吸链上的加速位点为:NADH还原酶,NADH-Q还原酶和甲基萘醌。
[Abstract]:Perchlorate is a persistent toxic substance, which causes serious environmental pollution due to illegal discharge during its use and production. As a new treatment technology, microbial fuel cell (MFC) can degrade pollutants and output electric energy at the same time, which has become the focus of environmental energy technology. Therefore, using sodium perchlorate as model pollutant, the treatment of perchlorate wastewater by single-chamber MFC reactor was studied. By optimizing the start-up conditions of MFC reactor, the effects of different co-existing electron receptors and different redox mediators on the performance of MFC were investigated. The reduction rate and voltage of perchlorate tend to be stable, and MFC has better performance when the initial concentration of perchlorate is 150 mg 路L ~ (-1) and sodium acetate is used as carbon source. Different types and concentrations of electron receptors have different effects on MFC performance. The presence of nitrate and chlorate inhibited the reduction of perchlorate. When the reduction of nitrate and chlorate was complete, the perchlorate began to reduce, which produced a higher voltage in nitrate reduction, but a lower voltage in chlorate reduction. When the reduction of nitrate and chlorate was complete, the voltage recovered to about 58 MV, and the high concentration sulfate inhibited the performance of MFC irreversibly. The results of thermodynamic analysis showed that there was an electronic competition between nitrate, chlorate and perchlorate, and the electrochemical analysis showed that the electrochemical activity of the anode was improved during the reduction of nitrate and chlorate. The effects of CuCl2NaN3, biscoumarin, rotenone, quinacrine dihydrochloride (QDH), dicyclohexyl carbodiimide (DCCD), carbonyl cyano-3-chlorophenylhydrazone (CCCP) and capsaicin on the performance of MFC were investigated. Methylnaphthoquinone Fe-S protein (complex 鈪,

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