微生物燃料电池中污染物的强化降解
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摘要
能源短缺和环境污染是当今世界的两大挑战。最近发展起来的微生物燃料电池技术因其可以同时产电和去除污染而为同时解决这两大问题提供了一条新的可能途径。此文研究了微生物燃料电池中难降解污染物,特别是偶氮染料和硝基芳香化合物的强化降解。并通过阴极修饰或生物阴极来提高污染物的降解效率。
首先研究了一种典型的偶氮染料—甲基橙在微生物燃料电池阴极的脱色。通过原位利用阳极的有机底物厌氧转化产生的电子,甲基橙在阴极被逐步还原。其还原过程可以通过假一级反应动力学来描述,相应的动力学常数为1.29／天。电化学阻抗谱分析表明,阴极具有较高的阻抗从而限制电子转移速率和阴极反应速率。为加快电子从阴极到甲基橙的转移以提高其脱色速率,我们利用一种典型的氧化还原介体硫堇,采用简单的电化学方法修饰阴极。阴极阻抗经过修饰降低了50%,而相应的甲基橙的脱色速率提高了20%。这些研究结果为偶氮染料脱色中限制性关键因素的识别及如何提高脱色速率提供了有价值的信息。然而偶氮染料的还原产物为有毒的芳香氨基化合物,仍需进一步处理。
其次探索了完全矿化偶氮染料偶氮苯一种新颖方法,其通过耦合微生物燃料电池阴极的还原和阳极的氧化来实现偶氮染料的完全降解。偶氮苯首先在微生物燃料电池的阴极被还原成苯胺,与此同时苯胺在阳极则被(产电)微生物进一步氧化,并将氧化过程中产生的电子用于阴极偶氮染料的还原。该过程实现了偶氮苯中电子的充分利用而无需额外提供电能或有机碳源。同时,电流在此过程中得以产生。与闭路状态的微生物燃料电池比较,苯胺在开路时降解速率仅有前者的一半。通过循环伏安,电化学阻抗谱和扫描电子显微镜对阳极的分析表明,附着在阳极表面的产电微生物的直接电子转移和氧化还原介体的穿梭电子转移这两种方式共同参与了苯胺氧化过程中电子向阳极的转移。同时,电极电势对苯胺降解速率的影响实验表明,更高的阳极电势有利于苯胺的降解。该研究对处理含吸电子基团污染物的工业废水或生物修复这一类污染物提供了一个低能耗的有潜力的方法。
最后,我们采用生物阴极来增强代表性的硝基芳香化合物—硝基苯的还原速率,并原位降解还原产物苯胺。硝基苯首先在生物阴极被还原为苯胺,然后苯胺被进一步好氧降解。通过分别以硝基苯或曝入的氧气作为电子受体,电流在这一氧化还原过程中始终产生。相比于非生物阴极,生物阴极极大的提高了硝基苯的还原速率,这要归功于微生物的催化作用,其大大降低了电荷转移阻抗进而促进了电子从生物阴极向硝基苯的转移速率。对于初始浓度为40mg/l的硝基苯,超过90%在4天内被还原,其速率常数为0.46/天；而还原生成的苯胺中有97%在一天内被进一步原位去除,相应的速率常数为3.5/天。这一策略不仅为含硝基苯或类似具有吸电子基团污染物的工业废水的处理,而且为这一类污染物的地下水或沉积物的生物电化学修复,提供了又一新颖的处理途径。
Energy shortage and environment pollution are two of the largest challenges around the world. Microbial fuel cells (MFCs), a recently developed technology which simultaneously generate electricity and reduce pollution, might provide an alternative solution to these problems. In this work, we studied the enhanced degradation of recalcitrant contaminants, especially azo dyes and nitroaromatic compounds, in MFCs. Also, cathode modification or biocathode was introduced to improve the degradation efficiency.
Firstly, methyl orange (MO), a typical azo dye, was decolorized at the cathode of MFCs. With in situ utilization of the electrons derived from the anaerobic conversion of organics, MO was steadily reduced in the abiotic cathode. The MO reduction could be described by a pseudo first-order kinetic model with a rate constant of1.29day-1. Electrochemical impedance spectroscopic analysis shows the cathode had a high polarization resistance, which could decrease the reaction rate and limit the electron transfer. To enhance the electron transfer from cathode to MO for its reduction, the cathode was modified with a redox mediator, thionine. Then the polarization resistance significantly decreased by over50%and the MO decolorization efficiency increased by about20%. These results provide useful information about the key factors limiting the azo dye reduction in the MFCs and measures to improve such a process. However, the reduced products of azo dyes-aromatic amines, are reported to be toxic and carcinogenic, and should be further treated.
Secondly, a novel approach was developed to completely mineralize azobenzene, a typical azo dye with simple structure, through coupling cathodic reduction and anodic oxidation processes in MFCs. Azobenzene was first electrochemically reduced at the abiotic cathode of MFCs to aniline, which was then further oxidized and degraded by the microorganisms at the anodic chamber of the same MFCs. Thus, the electrons present in azobenzene were fully utilized and no supply of external power or additional organic carbon source was needed in this process. Meanwhile, electricity was simultaneously produced. Compared with open circuit control, degradation rate of aniline was two-times higher. A characterization of the anode by cyclic voltammetry, electrochemical impedance spectroscopy and scanning electron microscopy indicate that both the electrochemically active microorganisms on the anode and the redox mediators contributed to the electron transfer in enhanced aniline oxidation. Furthermore, the aniline oxidation was favored by a higher applied anodic potential. This method provides a promising energy-efficient way to treat wastewater containing electron-withdrawing substances and may offer valuable reference for bioremediation of these pollutants.
Lastly, biocathode was adopted to enhance the reduction rate of nitrobezene and reduced product was further degraded in situ the biocathode of MFCs. Nitrobenzene, a representative nitroaromtaic pollutant, was first reduced to aniline and then oxidized to inorganic carbons in the biocathode of MFCs with aeration. At initial concentration of40mg/1, over90%nitrobenzene was reduced to aniline in4days while97%aniline was further in situ degraded with aeration within1day. Electricity was generated in the whole reduction and oxidation processes with nitrobenzene and oxygen as electron acceptor respectively. Compared with abiotic cathode, biocathode obviously enhanced the reduction of nitrobenzene through catalysis by microorganisms, which greatly decreased the charge transfer resistance and then promoted electron transfer from biocathode to nitrobenzene. This strategy might provide another novel approach not only for treatment of industry wastewater containing nitrobenzene or other electron-withdrawing structure contaminants, but also for in situ bioelectrochemical remediation of groundwater and sediment contaminated by these pollutants.
Energy shortage and environment pollution are two of the largest challenges around the world. Microbial fuel cells (MFCs), a recently developed technology which simultaneously generate electricity and reduce pollution, might provide an alternative solution to these problems. In this work, we studied the enhanced degradation of recalcitrant contaminants, especially azo dyes and nitroaromatic compounds, in MFCs. Also, cathode modification or biocathode was introduced to improve the degradation efficiency.
Firstly, methyl orange (MO), a typical azo dye, was decolorized at the cathode of MFCs. With in situ utilization of the electrons derived from the anaerobic conversion of organics, MO was steadily reduced in the abiotic cathode. The MO reduction could be described by a pseudo first-order kinetic model with a rate constant of1.29day-1. Electrochemical impedance spectroscopic analysis shows the cathode had a high polarization resistance, which could decrease the reaction rate and limit the electron transfer. To enhance the electron transfer from cathode to MO for its reduction, the cathode was modified with a redox mediator, thionine. Then the polarization resistance significantly decreased by over50%and the MO decolorization efficiency increased by about20%. These results provide useful information about the key factors limiting the azo dye reduction in the MFCs and measures to improve such a process. However, the reduced products of azo dyes-aromatic amines, are reported to be toxic and carcinogenic, and should be further treated.
Secondly, a novel approach was developed to completely mineralize azobenzene, a typical azo dye with simple structure, through coupling cathodic reduction and anodic oxidation processes in MFCs. Azobenzene was first electrochemically reduced at the abiotic cathode of MFCs to aniline, which was then further oxidized and degraded by the microorganisms at the anodic chamber of the same MFCs. Thus, the electrons present in azobenzene were fully utilized and no supply of external power or additional organic carbon source was needed in this process. Meanwhile, electricity was simultaneously produced. Compared with open circuit control, degradation rate of aniline was two-times higher. A characterization of the anode by cyclic voltammetry, electrochemical impedance spectroscopy and scanning electron microscopy indicate that both the electrochemically active microorganisms on the anode and the redox mediators contributed to the electron transfer in enhanced aniline oxidation. Furthermore, the aniline oxidation was favored by a higher applied anodic potential. This method provides a promising energy-efficient way to treat wastewater containing electron-withdrawing substances and may offer valuable reference for bioremediation of these pollutants.
Lastly, biocathode was adopted to enhance the reduction rate of nitrobezene and reduced product was further degraded in situ the biocathode of MFCs. Nitrobenzene, a representative nitroaromtaic pollutant, was first reduced to aniline and then oxidized to inorganic carbons in the biocathode of MFCs with aeration. At initial concentration of40mg/1, over90%nitrobenzene was reduced to aniline in4days while97%aniline was further in situ degraded with aeration within1day. Electricity was generated in the whole reduction and oxidation processes with nitrobenzene and oxygen as electron acceptor respectively. Compared with abiotic cathode, biocathode obviously enhanced the reduction of nitrobenzene through catalysis by microorganisms, which greatly decreased the charge transfer resistance and then promoted electron transfer from biocathode to nitrobenzene. This strategy might provide another novel approach not only for treatment of industry wastewater containing nitrobenzene or other electron-withdrawing structure contaminants, but also for in situ bioelectrochemical remediation of groundwater and sediment contaminated by these pollutants.
首先研究了一种典型的偶氮染料—甲基橙在微生物燃料电池阴极的脱色。通过原位利用阳极的有机底物厌氧转化产生的电子,甲基橙在阴极被逐步还原。其还原过程可以通过假一级反应动力学来描述,相应的动力学常数为1.29／天。电化学阻抗谱分析表明,阴极具有较高的阻抗从而限制电子转移速率和阴极反应速率。为加快电子从阴极到甲基橙的转移以提高其脱色速率,我们利用一种典型的氧化还原介体硫堇,采用简单的电化学方法修饰阴极。阴极阻抗经过修饰降低了50%,而相应的甲基橙的脱色速率提高了20%。这些研究结果为偶氮染料脱色中限制性关键因素的识别及如何提高脱色速率提供了有价值的信息。然而偶氮染料的还原产物为有毒的芳香氨基化合物,仍需进一步处理。
其次探索了完全矿化偶氮染料偶氮苯一种新颖方法,其通过耦合微生物燃料电池阴极的还原和阳极的氧化来实现偶氮染料的完全降解。偶氮苯首先在微生物燃料电池的阴极被还原成苯胺,与此同时苯胺在阳极则被(产电)微生物进一步氧化,并将氧化过程中产生的电子用于阴极偶氮染料的还原。该过程实现了偶氮苯中电子的充分利用而无需额外提供电能或有机碳源。同时,电流在此过程中得以产生。与闭路状态的微生物燃料电池比较,苯胺在开路时降解速率仅有前者的一半。通过循环伏安,电化学阻抗谱和扫描电子显微镜对阳极的分析表明,附着在阳极表面的产电微生物的直接电子转移和氧化还原介体的穿梭电子转移这两种方式共同参与了苯胺氧化过程中电子向阳极的转移。同时,电极电势对苯胺降解速率的影响实验表明,更高的阳极电势有利于苯胺的降解。该研究对处理含吸电子基团污染物的工业废水或生物修复这一类污染物提供了一个低能耗的有潜力的方法。
最后,我们采用生物阴极来增强代表性的硝基芳香化合物—硝基苯的还原速率,并原位降解还原产物苯胺。硝基苯首先在生物阴极被还原为苯胺,然后苯胺被进一步好氧降解。通过分别以硝基苯或曝入的氧气作为电子受体,电流在这一氧化还原过程中始终产生。相比于非生物阴极,生物阴极极大的提高了硝基苯的还原速率,这要归功于微生物的催化作用,其大大降低了电荷转移阻抗进而促进了电子从生物阴极向硝基苯的转移速率。对于初始浓度为40mg/l的硝基苯,超过90%在4天内被还原,其速率常数为0.46/天；而还原生成的苯胺中有97%在一天内被进一步原位去除,相应的速率常数为3.5/天。这一策略不仅为含硝基苯或类似具有吸电子基团污染物的工业废水的处理,而且为这一类污染物的地下水或沉积物的生物电化学修复,提供了又一新颖的处理途径。
Energy shortage and environment pollution are two of the largest challenges around the world. Microbial fuel cells (MFCs), a recently developed technology which simultaneously generate electricity and reduce pollution, might provide an alternative solution to these problems. In this work, we studied the enhanced degradation of recalcitrant contaminants, especially azo dyes and nitroaromatic compounds, in MFCs. Also, cathode modification or biocathode was introduced to improve the degradation efficiency.
Firstly, methyl orange (MO), a typical azo dye, was decolorized at the cathode of MFCs. With in situ utilization of the electrons derived from the anaerobic conversion of organics, MO was steadily reduced in the abiotic cathode. The MO reduction could be described by a pseudo first-order kinetic model with a rate constant of1.29day-1. Electrochemical impedance spectroscopic analysis shows the cathode had a high polarization resistance, which could decrease the reaction rate and limit the electron transfer. To enhance the electron transfer from cathode to MO for its reduction, the cathode was modified with a redox mediator, thionine. Then the polarization resistance significantly decreased by over50%and the MO decolorization efficiency increased by about20%. These results provide useful information about the key factors limiting the azo dye reduction in the MFCs and measures to improve such a process. However, the reduced products of azo dyes-aromatic amines, are reported to be toxic and carcinogenic, and should be further treated.
Secondly, a novel approach was developed to completely mineralize azobenzene, a typical azo dye with simple structure, through coupling cathodic reduction and anodic oxidation processes in MFCs. Azobenzene was first electrochemically reduced at the abiotic cathode of MFCs to aniline, which was then further oxidized and degraded by the microorganisms at the anodic chamber of the same MFCs. Thus, the electrons present in azobenzene were fully utilized and no supply of external power or additional organic carbon source was needed in this process. Meanwhile, electricity was simultaneously produced. Compared with open circuit control, degradation rate of aniline was two-times higher. A characterization of the anode by cyclic voltammetry, electrochemical impedance spectroscopy and scanning electron microscopy indicate that both the electrochemically active microorganisms on the anode and the redox mediators contributed to the electron transfer in enhanced aniline oxidation. Furthermore, the aniline oxidation was favored by a higher applied anodic potential. This method provides a promising energy-efficient way to treat wastewater containing electron-withdrawing substances and may offer valuable reference for bioremediation of these pollutants.
Lastly, biocathode was adopted to enhance the reduction rate of nitrobezene and reduced product was further degraded in situ the biocathode of MFCs. Nitrobenzene, a representative nitroaromtaic pollutant, was first reduced to aniline and then oxidized to inorganic carbons in the biocathode of MFCs with aeration. At initial concentration of40mg/1, over90%nitrobenzene was reduced to aniline in4days while97%aniline was further in situ degraded with aeration within1day. Electricity was generated in the whole reduction and oxidation processes with nitrobenzene and oxygen as electron acceptor respectively. Compared with abiotic cathode, biocathode obviously enhanced the reduction of nitrobenzene through catalysis by microorganisms, which greatly decreased the charge transfer resistance and then promoted electron transfer from biocathode to nitrobenzene. This strategy might provide another novel approach not only for treatment of industry wastewater containing nitrobenzene or other electron-withdrawing structure contaminants, but also for in situ bioelectrochemical remediation of groundwater and sediment contaminated by these pollutants.
Energy shortage and environment pollution are two of the largest challenges around the world. Microbial fuel cells (MFCs), a recently developed technology which simultaneously generate electricity and reduce pollution, might provide an alternative solution to these problems. In this work, we studied the enhanced degradation of recalcitrant contaminants, especially azo dyes and nitroaromatic compounds, in MFCs. Also, cathode modification or biocathode was introduced to improve the degradation efficiency.
Firstly, methyl orange (MO), a typical azo dye, was decolorized at the cathode of MFCs. With in situ utilization of the electrons derived from the anaerobic conversion of organics, MO was steadily reduced in the abiotic cathode. The MO reduction could be described by a pseudo first-order kinetic model with a rate constant of1.29day-1. Electrochemical impedance spectroscopic analysis shows the cathode had a high polarization resistance, which could decrease the reaction rate and limit the electron transfer. To enhance the electron transfer from cathode to MO for its reduction, the cathode was modified with a redox mediator, thionine. Then the polarization resistance significantly decreased by over50%and the MO decolorization efficiency increased by about20%. These results provide useful information about the key factors limiting the azo dye reduction in the MFCs and measures to improve such a process. However, the reduced products of azo dyes-aromatic amines, are reported to be toxic and carcinogenic, and should be further treated.
Secondly, a novel approach was developed to completely mineralize azobenzene, a typical azo dye with simple structure, through coupling cathodic reduction and anodic oxidation processes in MFCs. Azobenzene was first electrochemically reduced at the abiotic cathode of MFCs to aniline, which was then further oxidized and degraded by the microorganisms at the anodic chamber of the same MFCs. Thus, the electrons present in azobenzene were fully utilized and no supply of external power or additional organic carbon source was needed in this process. Meanwhile, electricity was simultaneously produced. Compared with open circuit control, degradation rate of aniline was two-times higher. A characterization of the anode by cyclic voltammetry, electrochemical impedance spectroscopy and scanning electron microscopy indicate that both the electrochemically active microorganisms on the anode and the redox mediators contributed to the electron transfer in enhanced aniline oxidation. Furthermore, the aniline oxidation was favored by a higher applied anodic potential. This method provides a promising energy-efficient way to treat wastewater containing electron-withdrawing substances and may offer valuable reference for bioremediation of these pollutants.
Lastly, biocathode was adopted to enhance the reduction rate of nitrobezene and reduced product was further degraded in situ the biocathode of MFCs. Nitrobenzene, a representative nitroaromtaic pollutant, was first reduced to aniline and then oxidized to inorganic carbons in the biocathode of MFCs with aeration. At initial concentration of40mg/1, over90%nitrobenzene was reduced to aniline in4days while97%aniline was further in situ degraded with aeration within1day. Electricity was generated in the whole reduction and oxidation processes with nitrobenzene and oxygen as electron acceptor respectively. Compared with abiotic cathode, biocathode obviously enhanced the reduction of nitrobenzene through catalysis by microorganisms, which greatly decreased the charge transfer resistance and then promoted electron transfer from biocathode to nitrobenzene. This strategy might provide another novel approach not only for treatment of industry wastewater containing nitrobenzene or other electron-withdrawing structure contaminants, but also for in situ bioelectrochemical remediation of groundwater and sediment contaminated by these pollutants.
引文
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