微生物燃料电池原位修复地下水硝酸盐污染研究
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摘要
微生物燃料电池（MFC）可从废水中回收能量，是一种新兴的环境技术。早期对MFC的研究多集中在如何提高其产电性能方面，随着研究的深入，人们发现MFC的燃料来源广泛，从易降解的葡萄糖、乙酸钠等到难生物降解的苯酚、吡啶等都已被证明可作为其燃料，这提供了一种思路，使得MFC可应用于处理污染废水的领域，但现有研究报道多限于水溶介质中的小试规模，其得到的结论并不适合地下水多孔介质体系。
目前地下水硝酸盐污染正在变得日益严重，对其进行处理的技术中较好的是原位修复技术，如原位生物修复技术、渗透性反应墙等。基于此，本文思路是设计MFC装置将其用于模拟原位修复受硝酸盐污染的地下水，研究装置在多孔介质条件下的生物修复功能和产电功能。设计了单室和双室两种大体积MFC装置进行原位修复地下水硝酸盐污染的研究，并对这两种装置的运行参数进行了较为系统的研究，包括地下水中的COD浓度，MFC的外接电阻值，以及地下水pH环境等因素对MFC装置脱氮除碳性能和产电性能的影响。论文得到的主要结论有以下几点：
1、结合将MFC应用于地下水硝酸盐污染原位修复的实际情况，设计了单室和双室两种大体积的MFC模型装置。单室MFC装置使用钛基二氧化铅电极作为阴极，埋置于沙子中的两块碳布作为阳极；双室MFC装置采用盐桥来连接阳极室和阴极室，阴、阳极均采用碳布作为电极材料，并测定了MFC模型装置的相关水理参数。研究结果表明该两种装置（特别是单室MFC装置）用于模拟处理受硝酸盐污染的地下水是有效的，为下一步将MFC应用于实际地下水硝酸盐污染原位修复打下基础。
2、本研究小组自制的钛基二氧化铅电极，在水溶介质体系的MFC研究中取得了较好的处理硝酸盐废水效果，本文使用多种电化学方法对该电极的电催化性能进行了研究。该电极的循环伏安曲线表明，其自身并没有参与MFC中的反硝化反应，它提高MFC的脱氮和去污能力主要是因为其具有较高的电流响应度；该电极的电化学阻抗谱表明，电极在经过一段反应时间后，其在MFC反应体系里的电化学活性增强，这从机理上解释了MFC要想获得稳定的电压输出，都需要一定启动时间的现象。
3、单室MFC装置模型运行结果表明，对目标污染物硝酸盐初始浓度为100mg/L的情况下，该装置可以利用废水中的有机物作为燃料（对应的COD浓度分别为1000mg/L和500mg/L），同步去除水中的有机物和硝酸盐，并获得稳定的电压输出。得出了该单室MFC装置在原位修复地下水硝酸盐污染（地下水中硝酸盐浓度为100mg/L）的最佳运行参数为：水中COD浓度为500mg/L，地下水溶液体系的pH值为7.0，MFC的外接电阻值为800Ω。此时该MFC的去污产电性能表现如下：除碳--最终溢流槽出水口的浓度为212mg/L，COD的去除率为57.6%（实验期间部分时间段COD的最大去除率达到76.2%）；脱氮--在整个运行周期硝酸盐氮数值始终处于非常低的水平，最大值仅有5.15mg/L，亚硝酸氮没有积累，氨氮浓度较大由于硝酸盐异化反应较多所致，同时与缓冲溶液里添加NH4Cl有关；产电--在整个实验运行期间，对外输出电压都相当平稳，最高电压达413mv，实验结束后的电压仍保持在300mv左右，显示了良好的持续和稳定的电压输出性能；最大功率密度为56.36mW·m-2，相应的电流密度为187.68mA·m-2，表明了该单室MFC装置的脱氮除碳和产电性能得到了最佳的统一。
4、双室MFC装置在以和单室MFC装置相同的参数运行结果表明，对处理水中目标污染物硝酸盐初始浓度为100mg/L的情况下，该装置去除废水中COD性能和硝酸盐性能较差，同时产电性能也较差。这一方面与该双室MFC运行时间较短有关以外，还说明了该装置的设计和结构尚需进一步的改进。研究了两种装置中硝酸盐浓度随时空的变化关系，为下一步建立实验砂槽装置内地下水体系溶质迁移模型，进行硝酸盐在地下水中迁移机理的理论研究，确定硝酸盐在多孔介质体系中的运移转化规律打下基础。
5、利用电化学工作站研究电极在两种MFC装置溶液体系里的电化学行为，利用扫描电镜（SEM）观察了碳布电极上附着的活性污泥生物膜的表面形貌，并用聚合酶链式反应（PCR）、变性梯度凝胶电泳（DGGE）技术对其中的细菌群落分布进行了研究。电化学研究表明，单室二氧化铅电极在长期运行后电化学活性会降低，双室阳极碳布电极在实验结束溶液体系里的电化学活性增强；SEM观察到单室碳布表面覆盖了厚厚的生物膜，双室阳极碳布被厚厚的一层盖杆状细菌覆盖，双室阴极碳布上基本没有生物膜；细菌研究表明单室碳布生物膜细菌主要是Fluviicola taffensis，Flavobacteriales bacterium，Moraxellaceae Bacterium，Acinetobacter sp，Flavobacterium sp，Janthinobacterium lividum和Comamonadaceae bacterium；双室碳布生物膜细菌主要是Hyphomicrobium sp，Rhodobacter sp，Thermomonas fusca，Thermomonas fusca，Hirschiabaltica，Arcobacter sp和Rhodobacter。
研究结果表明，利用MFC装置进行地下水硝酸盐污染原位修复理论上是可行的，只要有性能良好的电极材料和设计合理的装置，MFC技术必将在未来地下水污染原位修复工程实践中发挥重要作用。
Microbial fuel cell technology (MFC) is an emerging environmental technology for energyrecovery from the wastewater. Early studies of MFC mainly focused on how to improve itsperformance of electricity production. The further research indicated that the source of MFC fuelvaried from the easy degradation substance,such as glucose, sodium acetate to refractory organicsubstance,such as phenol, pyridine, etc. Thus an idea was provided that the MFC could be used inthe field of dealing with contaminated wastewater. But present researches were mostly limited tosmall pilot scale in the water-soluble medium, and the conclusions were not suitable for groundwaterin porous media system.
Nitrate pollution in groundwater is becoming increasingly serious presently. In-situ remediationtechnologies are better among its treatment technologies,such as in-situ bioremediation technologiesand the permeable reactive barrier(PRB). Based on this, the idea is to design MFC devices used tosimulate the in-situ remediation of nitrate contamination in groundwater and the MFC’s performanceof bioremediation and electricity generation in porous media was also investigated. Two differentstructure MFCs were designed for in-situ remediation of nitrate pollution of groundwater, one was asingle-chamber MFC and the other was a dual-chamber MFC. Some factors affecting the MFCperformance of the removal of nitrogen and carbon and electricity production were investigatedsystematicly, including the COD concentration in the groundwater, MFC’s external resistance valueand groundwater pH environment.The main results in the thesis are summarized as follows:
1.Two large volume MFC devices were construced according to the practical nitrate pollution ingroundwater.The titanium-based lead dioxide electrode was used as the cathode and two carboncloths buried in sand were usd as the anode in the single-chamber MFC device. In the dual-chamberMFC device, cathode and anode material was carbon cloth and the salt bridge was used to connectthe anode chamber and cathode chamber.Before operation,some hydrodynamic parameters of themodel device were determined. The results showed that the two devices (especially thesingle-chamber MFC device) were effective when used to simulate the processing on the nitratepollution in groundwater, and this laid the foundation for MFC’s actual application in the in-situremediation of nitrate pollution in the groundwater.
2.The self-made titanium-based lead dioxide electrode had been used in MFC for a better effecton treating nitrate wastewater in water-soluble media system.A variety of electrochemical methodswere used to study the electrode catalytic properties in this work.The cyclic voltammograms(CV) ofthe electrode shown that the electrode self was not involved in denitrification in the MFC, itincreased the nitrogen removal and decontamination of the MFC because of its higher current response. And the electrochemical impedance spectroscopy(EIS) shown that the electrode’selectrochemical activity in the MFC reaction system was enhanced after a period of reaction time,which explained the phenomenon mechanicaly that a period of set-up time was requried in order toobtain a stable voltage output from MFC device.
3.The results of single-chamber MFC device showed that it could take advantage of theorganics in the wastewater as fuel (corresponding to the COD concentration of1000mg/L and500mg/L)and obtain a stable voltage output with simultaneous removal of organic matter and nitratewhen treating the wastewater containing nitrate concentration of100mg/L. And the best operatingparameters were obtained during the period of in-situ remediation of nitrate pollution in groundwater.The reults were as follows: the COD concentration was500mg/L and the pH value was7.0ingroundwater, MFC external resistor value was800. Under this condition, the MFC’s performanceof decontamination and electricity generation was quite good as follows: removal of carbon—CODconcentration in the ultimate overflow tank outlet was212mg/L with the removal efficiency of57.6%(maximum COD removal efficiency of76.2%, part time during the experiment); remomal ofnitrate—Nitrate nitrogen value was very small during the whole period with the maximum value ofonly5.15mg/L, and nitrite nitrogen was not accumulated too. But the ammonia nitrogenconcentration was quite high due to nitrate dissimilation and the NH4Cl addition into the buffersolution; electricity production—During the entire experiment period, the external output voltagewas quite stable.The highest voltage was413mv and the value was still maintained at about300mvat the end of the experiment, which showed the device’s continuious and stable voltage outputperformance.The maximum power density was56.36mW m-2with the corresponding current densityof187.68mA m-2. All the results indicated that the single-chamber MFC device obtained highremoval of nitrogen and carbon with effective power output.
4.The results of dual-chamber MFC devices running in the same parameters withsingle-chamber MFC devices’ showed that both the performance of decontamination and theelectricity production were poor when dealing with the wastewater containing nitrate concentrationof100mg/L. This may be due to the the short length of the device operation time partialy, but it alsodemonstrated that the design and construction of the device were required further improvement. Thetime and space variation of the nitrate concentration in the two devices was investigated. for the nextstep to establish the solute transport model in groundwater within the experimental sand tank. Andthis would lay the foundation for theoretical study on the migration of nitrate in groundwater anddetermination of nitrate transport in porous media system.
5.The electrochemical workstation was used to analyse the electrode’s electrochemical behaviorin the solution obtained from the two kinds of MFC devices. The scanning electron microscopy (SEM) was used to observe the surface morphology of the activated sludge biofilm attached to thecarbon cloth electrode. The technology of polymerase chain reaction (PCR) and denaturinggradient gel electrophoresis (DGGE) were used to study the bacteria community distribution of thebiofilm. Electrochemical studies had shown that the lead dioxide electrode(used in thesingle-chamber MFC) electrochemical activity would decrease in the long run, but the anode carboncloth electrode(used in the dual-chamber MFC)electrochemical activity would increase in thesolution obtained at the end of the experiment. A thick layer of biofilm could be observed on thesingle chamber MFC carbon cloth surface, and dual-chamber anode carbon cloth was covered with athick layer of rod-shaped bacteria biofilm, but few bacteria were seen on the dual-chamber cathodecarbon cloth. The domiant species of microbial community composition of the single-chambercarbon cloth biofilm were Fluviicola taffensis, Flavobacteriales bacterium, MoraxellaceaeBacterium, Acinetobacter sp, Flavobacterium sp, Janthinobacterium lividum, Comamonadaceaebacterium; while the domiant species of microbial community composition of the dual-chambercarbon cloth biofilm were Hyphomicrobium sp, Rhodobacter sp, Thermomonas fusca, Thermomonasfusca, Hirschia baltica, Arcobacter sp and Rhodobacter.
The results show that in-situ remediation of nitrate pollution in groundwater by MFC deviceis theoretically possible. As long as the good performance of the electrode material and reasonabledesign of the device, MFC technology will play an important role in the engineering practice of.in-situ remediation of groundwater pollution.
目前地下水硝酸盐污染正在变得日益严重，对其进行处理的技术中较好的是原位修复技术，如原位生物修复技术、渗透性反应墙等。基于此，本文思路是设计MFC装置将其用于模拟原位修复受硝酸盐污染的地下水，研究装置在多孔介质条件下的生物修复功能和产电功能。设计了单室和双室两种大体积MFC装置进行原位修复地下水硝酸盐污染的研究，并对这两种装置的运行参数进行了较为系统的研究，包括地下水中的COD浓度，MFC的外接电阻值，以及地下水pH环境等因素对MFC装置脱氮除碳性能和产电性能的影响。论文得到的主要结论有以下几点：
1、结合将MFC应用于地下水硝酸盐污染原位修复的实际情况，设计了单室和双室两种大体积的MFC模型装置。单室MFC装置使用钛基二氧化铅电极作为阴极，埋置于沙子中的两块碳布作为阳极；双室MFC装置采用盐桥来连接阳极室和阴极室，阴、阳极均采用碳布作为电极材料，并测定了MFC模型装置的相关水理参数。研究结果表明该两种装置（特别是单室MFC装置）用于模拟处理受硝酸盐污染的地下水是有效的，为下一步将MFC应用于实际地下水硝酸盐污染原位修复打下基础。
2、本研究小组自制的钛基二氧化铅电极，在水溶介质体系的MFC研究中取得了较好的处理硝酸盐废水效果，本文使用多种电化学方法对该电极的电催化性能进行了研究。该电极的循环伏安曲线表明，其自身并没有参与MFC中的反硝化反应，它提高MFC的脱氮和去污能力主要是因为其具有较高的电流响应度；该电极的电化学阻抗谱表明，电极在经过一段反应时间后，其在MFC反应体系里的电化学活性增强，这从机理上解释了MFC要想获得稳定的电压输出，都需要一定启动时间的现象。
3、单室MFC装置模型运行结果表明，对目标污染物硝酸盐初始浓度为100mg/L的情况下，该装置可以利用废水中的有机物作为燃料（对应的COD浓度分别为1000mg/L和500mg/L），同步去除水中的有机物和硝酸盐，并获得稳定的电压输出。得出了该单室MFC装置在原位修复地下水硝酸盐污染（地下水中硝酸盐浓度为100mg/L）的最佳运行参数为：水中COD浓度为500mg/L，地下水溶液体系的pH值为7.0，MFC的外接电阻值为800Ω。此时该MFC的去污产电性能表现如下：除碳--最终溢流槽出水口的浓度为212mg/L，COD的去除率为57.6%（实验期间部分时间段COD的最大去除率达到76.2%）；脱氮--在整个运行周期硝酸盐氮数值始终处于非常低的水平，最大值仅有5.15mg/L，亚硝酸氮没有积累，氨氮浓度较大由于硝酸盐异化反应较多所致，同时与缓冲溶液里添加NH4Cl有关；产电--在整个实验运行期间，对外输出电压都相当平稳，最高电压达413mv，实验结束后的电压仍保持在300mv左右，显示了良好的持续和稳定的电压输出性能；最大功率密度为56.36mW·m-2，相应的电流密度为187.68mA·m-2，表明了该单室MFC装置的脱氮除碳和产电性能得到了最佳的统一。
4、双室MFC装置在以和单室MFC装置相同的参数运行结果表明，对处理水中目标污染物硝酸盐初始浓度为100mg/L的情况下，该装置去除废水中COD性能和硝酸盐性能较差，同时产电性能也较差。这一方面与该双室MFC运行时间较短有关以外，还说明了该装置的设计和结构尚需进一步的改进。研究了两种装置中硝酸盐浓度随时空的变化关系，为下一步建立实验砂槽装置内地下水体系溶质迁移模型，进行硝酸盐在地下水中迁移机理的理论研究，确定硝酸盐在多孔介质体系中的运移转化规律打下基础。
5、利用电化学工作站研究电极在两种MFC装置溶液体系里的电化学行为，利用扫描电镜（SEM）观察了碳布电极上附着的活性污泥生物膜的表面形貌，并用聚合酶链式反应（PCR）、变性梯度凝胶电泳（DGGE）技术对其中的细菌群落分布进行了研究。电化学研究表明，单室二氧化铅电极在长期运行后电化学活性会降低，双室阳极碳布电极在实验结束溶液体系里的电化学活性增强；SEM观察到单室碳布表面覆盖了厚厚的生物膜，双室阳极碳布被厚厚的一层盖杆状细菌覆盖，双室阴极碳布上基本没有生物膜；细菌研究表明单室碳布生物膜细菌主要是Fluviicola taffensis，Flavobacteriales bacterium，Moraxellaceae Bacterium，Acinetobacter sp，Flavobacterium sp，Janthinobacterium lividum和Comamonadaceae bacterium；双室碳布生物膜细菌主要是Hyphomicrobium sp，Rhodobacter sp，Thermomonas fusca，Thermomonas fusca，Hirschiabaltica，Arcobacter sp和Rhodobacter。
研究结果表明，利用MFC装置进行地下水硝酸盐污染原位修复理论上是可行的，只要有性能良好的电极材料和设计合理的装置，MFC技术必将在未来地下水污染原位修复工程实践中发挥重要作用。
Microbial fuel cell technology (MFC) is an emerging environmental technology for energyrecovery from the wastewater. Early studies of MFC mainly focused on how to improve itsperformance of electricity production. The further research indicated that the source of MFC fuelvaried from the easy degradation substance,such as glucose, sodium acetate to refractory organicsubstance,such as phenol, pyridine, etc. Thus an idea was provided that the MFC could be used inthe field of dealing with contaminated wastewater. But present researches were mostly limited tosmall pilot scale in the water-soluble medium, and the conclusions were not suitable for groundwaterin porous media system.
Nitrate pollution in groundwater is becoming increasingly serious presently. In-situ remediationtechnologies are better among its treatment technologies,such as in-situ bioremediation technologiesand the permeable reactive barrier(PRB). Based on this, the idea is to design MFC devices used tosimulate the in-situ remediation of nitrate contamination in groundwater and the MFC’s performanceof bioremediation and electricity generation in porous media was also investigated. Two differentstructure MFCs were designed for in-situ remediation of nitrate pollution of groundwater, one was asingle-chamber MFC and the other was a dual-chamber MFC. Some factors affecting the MFCperformance of the removal of nitrogen and carbon and electricity production were investigatedsystematicly, including the COD concentration in the groundwater, MFC’s external resistance valueand groundwater pH environment.The main results in the thesis are summarized as follows:
1.Two large volume MFC devices were construced according to the practical nitrate pollution ingroundwater.The titanium-based lead dioxide electrode was used as the cathode and two carboncloths buried in sand were usd as the anode in the single-chamber MFC device. In the dual-chamberMFC device, cathode and anode material was carbon cloth and the salt bridge was used to connectthe anode chamber and cathode chamber.Before operation,some hydrodynamic parameters of themodel device were determined. The results showed that the two devices (especially thesingle-chamber MFC device) were effective when used to simulate the processing on the nitratepollution in groundwater, and this laid the foundation for MFC’s actual application in the in-situremediation of nitrate pollution in the groundwater.
2.The self-made titanium-based lead dioxide electrode had been used in MFC for a better effecton treating nitrate wastewater in water-soluble media system.A variety of electrochemical methodswere used to study the electrode catalytic properties in this work.The cyclic voltammograms(CV) ofthe electrode shown that the electrode self was not involved in denitrification in the MFC, itincreased the nitrogen removal and decontamination of the MFC because of its higher current response. And the electrochemical impedance spectroscopy(EIS) shown that the electrode’selectrochemical activity in the MFC reaction system was enhanced after a period of reaction time,which explained the phenomenon mechanicaly that a period of set-up time was requried in order toobtain a stable voltage output from MFC device.
3.The results of single-chamber MFC device showed that it could take advantage of theorganics in the wastewater as fuel (corresponding to the COD concentration of1000mg/L and500mg/L)and obtain a stable voltage output with simultaneous removal of organic matter and nitratewhen treating the wastewater containing nitrate concentration of100mg/L. And the best operatingparameters were obtained during the period of in-situ remediation of nitrate pollution in groundwater.The reults were as follows: the COD concentration was500mg/L and the pH value was7.0ingroundwater, MFC external resistor value was800. Under this condition, the MFC’s performanceof decontamination and electricity generation was quite good as follows: removal of carbon—CODconcentration in the ultimate overflow tank outlet was212mg/L with the removal efficiency of57.6%(maximum COD removal efficiency of76.2%, part time during the experiment); remomal ofnitrate—Nitrate nitrogen value was very small during the whole period with the maximum value ofonly5.15mg/L, and nitrite nitrogen was not accumulated too. But the ammonia nitrogenconcentration was quite high due to nitrate dissimilation and the NH4Cl addition into the buffersolution; electricity production—During the entire experiment period, the external output voltagewas quite stable.The highest voltage was413mv and the value was still maintained at about300mvat the end of the experiment, which showed the device’s continuious and stable voltage outputperformance.The maximum power density was56.36mW m-2with the corresponding current densityof187.68mA m-2. All the results indicated that the single-chamber MFC device obtained highremoval of nitrogen and carbon with effective power output.
4.The results of dual-chamber MFC devices running in the same parameters withsingle-chamber MFC devices’ showed that both the performance of decontamination and theelectricity production were poor when dealing with the wastewater containing nitrate concentrationof100mg/L. This may be due to the the short length of the device operation time partialy, but it alsodemonstrated that the design and construction of the device were required further improvement. Thetime and space variation of the nitrate concentration in the two devices was investigated. for the nextstep to establish the solute transport model in groundwater within the experimental sand tank. Andthis would lay the foundation for theoretical study on the migration of nitrate in groundwater anddetermination of nitrate transport in porous media system.
5.The electrochemical workstation was used to analyse the electrode’s electrochemical behaviorin the solution obtained from the two kinds of MFC devices. The scanning electron microscopy (SEM) was used to observe the surface morphology of the activated sludge biofilm attached to thecarbon cloth electrode. The technology of polymerase chain reaction (PCR) and denaturinggradient gel electrophoresis (DGGE) were used to study the bacteria community distribution of thebiofilm. Electrochemical studies had shown that the lead dioxide electrode(used in thesingle-chamber MFC) electrochemical activity would decrease in the long run, but the anode carboncloth electrode(used in the dual-chamber MFC)electrochemical activity would increase in thesolution obtained at the end of the experiment. A thick layer of biofilm could be observed on thesingle chamber MFC carbon cloth surface, and dual-chamber anode carbon cloth was covered with athick layer of rod-shaped bacteria biofilm, but few bacteria were seen on the dual-chamber cathodecarbon cloth. The domiant species of microbial community composition of the single-chambercarbon cloth biofilm were Fluviicola taffensis, Flavobacteriales bacterium, MoraxellaceaeBacterium, Acinetobacter sp, Flavobacterium sp, Janthinobacterium lividum, Comamonadaceaebacterium; while the domiant species of microbial community composition of the dual-chambercarbon cloth biofilm were Hyphomicrobium sp, Rhodobacter sp, Thermomonas fusca, Thermomonasfusca, Hirschia baltica, Arcobacter sp and Rhodobacter.
The results show that in-situ remediation of nitrate pollution in groundwater by MFC deviceis theoretically possible. As long as the good performance of the electrode material and reasonabledesign of the device, MFC technology will play an important role in the engineering practice of.in-situ remediation of groundwater pollution.
引文
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