过硫酸盐阴极型微生物燃料电池降解活性艳蓝及产电性能的研究
发布时间：2019-01-16 04:51
【摘要】：本论文以蒽醌染料活性艳蓝KN-R作为目标污染物，以零价铁（Fe0）和二价铁（Fe2+）活化过硫酸盐（PDS）的高级氧化技术降解KN-R作为对照，研究了将Fe2+和Fe0活化PDS高级氧化体系耦合到微生物燃料电池阴极，并探讨了体系初始pH值，Fen和PDS初始投加量对活性艳蓝KN-R的降解和MFC的产电性能的影响。实验结论如下： 1.以Fe2+和Fe0来分别活化PDS时降解KN-R。在Fe2+/PDS体系中，KN-R的降解分为快速反应阶段和慢速反应阶段，并且两个阶段都符合一级反应动力学模型。pH值和Fe2+投加量是限制体系氧化降解污染物能力的主要因素，，随着PDS的浓度增大，体系中KN-R的降解率逐渐增加。在Fe0/PDS体系中，KN-R的降解遵循准一级动力学方程。体系能够很好的克服Fe2+/PDS体系中pH和Fe2+投加量阈值较低问题，在中性条件下（pH=7），KN-R取得最大的降解率，为93.12%；同时，随着初始Fe0投加量的增加，KN-R的降解速度明显加快，当Fe0投加量为448mg/L，PDS为2mmol/L时，KN-R的降解反应速率常数为0.0414min-1。 2.在耦合MFC之前研究了阳极为连续型时，HRT和阴极电子受体对MFC产电性能的影响，当HRT为18h时，阴极曝空气时MFC的最大功率密度达到最大为34.15mW/m2，在此条件下将Fe2+/PDS体系和Fe0/PDS体系分别作为MFC阴极液时，探讨活性艳蓝KN-R的降解情况以及体系的产电性能。在Fe2+/PDS-MFC体系中， KN-R的降解遵循二级反应动力学方程。与Fe2+/PDS体系相比，Fe2+/PDS-MFC体系并没有突破pH值和Fe2+投加量的限制，对体系的氧化能力影响不大，但能够显著加快体系中PDS的消耗速度，并且在弱酸性（pH=5）条件下KN-R也几乎完全降解；体系的产电能力受到pH值限制比较严重，但Fe2+投加量对体系的产电性能抑制作用并不明显，随着初始PDS浓度的增加，体系的输出功率逐渐增大。当初始pH为3，PDS初始浓度为2mmol/L，Fe2+投加量为1mmo/L时，体系的最大功率密度为294.07mW/m2。 与Fe0/PDS体系相同，在Fe0/PDS-MFC体系中，KN-R的降解也遵循准一级动力学方程，体系受pH值、Fe0投加量和PDS浓度影响较弱，在本研究的各参数条件下都能获得较高的KN-R降解率，且污染物的降解速度明显高于Fe0/PDS体系，在相同的Fe0投加量时，KN-R的降解反应速率提高了4.26-7.39倍；体系的产电能力低于Fe2+/PDS-MFC体系，受各参数条件的影响较大，当初始pH为3，PDS初始浓度为1mmol/L，Fe0投加量为28mg/L时体系各项性能达到最佳，此时KN-R的降解率为98.98%，最大功率密度为127.66mW/m2。 3.考察了四个体系最佳条件下TOC的去除率和活性艳蓝KN-R的降解光谱。结果表明在Fe0/PDS-MFC体系中TOC的去除率最大，Fe2+/PDS-MFC体系中TOC的去除率高于Fe2+/PDS体系。Fe0/PDS体系TOC低于Fe0/PDS-MFC体系的原因是前者PDS活化产生SO4-·的速度较低，在有限的时间内不能很好的矿化污染物。对KN-R降解过程中的UV-vis光谱分析得知，体系中产生的SO4-·先破坏KN-R结构中的2-磺酸-1，4二氨基蒽醌大共轭发色体系，使活性艳蓝KN-R脱色，然后再对蒽醌结构和苯环结构进行开环反应。
[Abstract]:In this paper, the degradation of KN-R with the high-level oxidation technology of zero-valent iron (Fe0) and divalent iron (Fe2 +)-activated persulfate (PDS) was used as the control for the high-grade oxidation of the dye-reactive brilliant blue KN-R as the target pollutant. The effects of the initial pH value of the system, the initial investment of Fen and PDS on the degradation of the reactive brilliant blue KN-R and the electrical properties of the MFC were studied. The experimental conclusion is as follows: 1. Degradation of KN-when the PDS is activated with Fe2 + and Fe0, respectively. R. In the Fe2 +/ PDS system, the degradation of KN-R is divided into a rapid reaction stage and a slow reaction stage, As the concentration of PDS increased, the degradation rate of KN-R in the system increased gradually. Plus. In the Fe0/ PDS system, the degradation of KN-R follows the quasi-first-order kinetics. In the neutral condition (pH = 7), the maximum degradation rate of KN-R was 93. 12%. At the same time, with the increase of initial Fe0, the degradation rate of KN-R was increased obviously. When the addition of Fe0 was 448mg/ L, the PDS was 2mmol/ L. The degradation reaction rate constant of KN-R is 0.0414min-1. 2. The effect of the HRT and the cathode electron acceptor on the electrical properties of the MFC was studied before the MFC was coupled. When HRT was 18h, the maximum power density of MFC reached to 34. 15mW/ m2 when the HRT was 18h, and the Fe2 +/ PDS system and the Fe0/ PDS system were used as MFC in this condition. The degradation of reactive brilliant blue KN-R and the production of the system were discussed. Electrical performance. In the Fe2 +/ PDS-MFC system, the degradation of KN-R follows the secondary reaction power. Compared with the Fe2 +/ PDS system, the Fe2 +/ PDS-MFC system does not break through the limit of the pH value and the amount of Fe 2 +, but the oxidation capacity of the system is not large, but the consumption rate of the PDS in the system can be obviously accelerated, and the KN-R is almost finished under the condition of weak acid (pH = 5). Total degradation; the electric capacity of the system is limited by the pH value, but the effect of the addition of Fe2 + on the electrical property of the system is not obvious, and the output power of the system is determined by the increase of the initial PDS concentration. The maximum power density of the system is 294.07mW when the initial pH is 3, the initial concentration of the PDS is 2mmol/ L, the addition amount of the Fe2 + is 1mmo/ L. In the same way as the Fe0/ PDS system, in the Fe0/ PDS-MFC system, the degradation of KN-R also follows the quasi-first-order kinetic equation, and the system is affected by the pH value, the concentration of Fe0 and the concentration of the PDS, and the high KN-R degradation rate can be obtained under the conditions of each parameter of the study, and the degradation speed of the pollutants is obviously higher than that of the Fe0/ PDS. The degradation reaction rate of KN-R is increased by 4.26-7.39 times when the same Fe0 is added, and the electric capacity of the system is lower than that of the Fe2 +/ PDS-MFC system. The initial pH is 3, the initial concentration of PDS is 1mmol/ L and the addition of Fe0 is 28mg/ L. At this time, the degradation rate of KN-R is 98. 98% and the maximum power density is 127.66. The removal rate and reactive brilliant blue KN of the TOC under the optimum conditions of the four systems were investigated. The results show that the removal rate of TOC in the Fe0/ PDS-MFC system is the most, and the removal rate of TOC in the Fe2 +/ PDS-MFC system is higher than that of the Fe2 +/ PDS-MFC system. +/ PDS system. The reason that the TOC of the Fe0/ PDS system is lower than that of the Fe0/ PDS-MFC system is that the former PDS is activated to produce SO4-. The speed is low, and it can't be very effective in a limited time. In the process of KN-R degradation, the UV-vis spectrum analysis was carried out. The results of UV-vis analysis in the system of KN-R were obtained. The 2-sulfonic acid-1, 4-diamino-1, 4-diamino-1, and the large-scale co-emission color system in KN-R structure were destroyed, and the active brilliant blue KN-R was decolorized, and then the structure of the disulfide bond and the benzene ring junction were carried out.
【学位授予单位】：中国海洋大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：TM911.45;X703
本文编号：2409483
[Abstract]:In this paper, the degradation of KN-R with the high-level oxidation technology of zero-valent iron (Fe0) and divalent iron (Fe2 +)-activated persulfate (PDS) was used as the control for the high-grade oxidation of the dye-reactive brilliant blue KN-R as the target pollutant. The effects of the initial pH value of the system, the initial investment of Fen and PDS on the degradation of the reactive brilliant blue KN-R and the electrical properties of the MFC were studied. The experimental conclusion is as follows: 1. Degradation of KN-when the PDS is activated with Fe2 + and Fe0, respectively. R. In the Fe2 +/ PDS system, the degradation of KN-R is divided into a rapid reaction stage and a slow reaction stage, As the concentration of PDS increased, the degradation rate of KN-R in the system increased gradually. Plus. In the Fe0/ PDS system, the degradation of KN-R follows the quasi-first-order kinetics. In the neutral condition (pH = 7), the maximum degradation rate of KN-R was 93. 12%. At the same time, with the increase of initial Fe0, the degradation rate of KN-R was increased obviously. When the addition of Fe0 was 448mg/ L, the PDS was 2mmol/ L. The degradation reaction rate constant of KN-R is 0.0414min-1. 2. The effect of the HRT and the cathode electron acceptor on the electrical properties of the MFC was studied before the MFC was coupled. When HRT was 18h, the maximum power density of MFC reached to 34. 15mW/ m2 when the HRT was 18h, and the Fe2 +/ PDS system and the Fe0/ PDS system were used as MFC in this condition. The degradation of reactive brilliant blue KN-R and the production of the system were discussed. Electrical performance. In the Fe2 +/ PDS-MFC system, the degradation of KN-R follows the secondary reaction power. Compared with the Fe2 +/ PDS system, the Fe2 +/ PDS-MFC system does not break through the limit of the pH value and the amount of Fe 2 +, but the oxidation capacity of the system is not large, but the consumption rate of the PDS in the system can be obviously accelerated, and the KN-R is almost finished under the condition of weak acid (pH = 5). Total degradation; the electric capacity of the system is limited by the pH value, but the effect of the addition of Fe2 + on the electrical property of the system is not obvious, and the output power of the system is determined by the increase of the initial PDS concentration. The maximum power density of the system is 294.07mW when the initial pH is 3, the initial concentration of the PDS is 2mmol/ L, the addition amount of the Fe2 + is 1mmo/ L. In the same way as the Fe0/ PDS system, in the Fe0/ PDS-MFC system, the degradation of KN-R also follows the quasi-first-order kinetic equation, and the system is affected by the pH value, the concentration of Fe0 and the concentration of the PDS, and the high KN-R degradation rate can be obtained under the conditions of each parameter of the study, and the degradation speed of the pollutants is obviously higher than that of the Fe0/ PDS. The degradation reaction rate of KN-R is increased by 4.26-7.39 times when the same Fe0 is added, and the electric capacity of the system is lower than that of the Fe2 +/ PDS-MFC system. The initial pH is 3, the initial concentration of PDS is 1mmol/ L and the addition of Fe0 is 28mg/ L. At this time, the degradation rate of KN-R is 98. 98% and the maximum power density is 127.66. The removal rate and reactive brilliant blue KN of the TOC under the optimum conditions of the four systems were investigated. The results show that the removal rate of TOC in the Fe0/ PDS-MFC system is the most, and the removal rate of TOC in the Fe2 +/ PDS-MFC system is higher than that of the Fe2 +/ PDS-MFC system. +/ PDS system. The reason that the TOC of the Fe0/ PDS system is lower than that of the Fe0/ PDS-MFC system is that the former PDS is activated to produce SO4-. The speed is low, and it can't be very effective in a limited time. In the process of KN-R degradation, the UV-vis spectrum analysis was carried out. The results of UV-vis analysis in the system of KN-R were obtained. The 2-sulfonic acid-1, 4-diamino-1, 4-diamino-1, and the large-scale co-emission color system in KN-R structure were destroyed, and the active brilliant blue KN-R was decolorized, and then the structure of the disulfide bond and the benzene ring junction were carried out.
【学位授予单位】：中国海洋大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：TM911.45;X703
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