生物阴极微生物燃料电池处理垃圾渗滤液及产电性能研究
发布时间：2018-08-17 17:44
【摘要】：垃圾渗滤液因其较高的COD、BOD、NH3-N、重金属离子及复杂的有毒有机污染物等，而呈现出色度大、臭味大、毒性大及难处理的特点，对环境危害严重。而生物阴极型微生物燃料电池(MFC)在具备微生物燃料电池产电及去除污染物的基础上，具有构建运行成本低、避免二次污染、可进行反硝化反应实现脱氮等优点。本文通过以铁氰化钾为阴极电子受体的双室化学MFC为参照，构建双室曝气MFC和双室不曝气MFC，跟踪对比各MFCs的启动情况及性能，，并在此基础上对不同阴极型MFCs处理垃圾渗滤液的产电及对污染物的降解效果进行探索。 MFC启动实质上是产电微生物在阳极表面逐渐富集形成生物膜的过程，在以NaAC为阳极碳源的条件下，启动用时长短依次为：化学MFC (1d)曝气MFC (5d)不曝气MFC(10d)；稳定周期长短依次为：不曝气MFC (30d)曝气MFC (25d)化学MFC (20d)；产电稳定电压的大小依次为：曝气MFC (618mV)不曝气MFC(561mV)化学MFC (467mV)。电池启动完成后稳定运行，开路电压大小顺序为：曝气MFC (835.30mV)不曝气MFC (790.26mV)化学MFC (546.23mV)；最大功率密度大小顺序为：曝气MFC (442.54mW/m3)不曝气MFC(237.04mW/m3)化学MFC(201.8mW/m3)；电池自身内阻大小顺序为：不曝气MFC(450)曝气MFC(600)化学MFC(620)。以NaAC为阳极碳源的条件下，生物阴极MFC的产电性能要好于以铁氰化钾为电子受体的化学阴极MFC。 不同阴极型MFCs处理垃圾渗滤液的产电电压与阳极渗滤液的稀释倍数间呈现一定的周期性规律，各周期内电池的平均最高产电电压依次为化学MFC(约630mV)曝气MFC(约380mV)不曝气MFC(约330mV)；各周期内产电电压变化受阴极液的影响较大，化学MFC主要受铁氰化钾的含量影响，曝气MFC主要与阴极溶解氧量及微生物菌群的稳定有关，不曝气MFC主要受阴极营养物质含量影响。 在处理不同体积比的渗滤液时，各MFCs阳极COD去除率的变化趋势与输出电压的基本一致即先增加后降低，曝气/不曝气MFC阴极COD去除率高于阳极去除率；各组MFCs库伦效率随阳极初始渗滤液比例增大而依次降低，各组MFCs中最大库伦效率依次为曝气MFC(10.26%)化学MFC(4.3%)不曝气MFC(1.46%)。不曝气MFC更利于渗滤液中COD的去除，但曝气MFC更利于将从COD获得的能量转化为电能。 3组MFCs阳极NH4+-N的去除量也随渗滤液比例的增加而增大，且在浓度梯度的作用下部分迁移至阴极；NO3--N去除率均呈现升高后降低的趋势，且阳极室均未发现NO2--N的积累现象；同等稀释倍数的渗滤液经处理后，三种N的去除量依次为曝气MFC不曝气MFC化学MFC。结果表明，曝气MFC更利于渗滤液中N的去除。另外，阴极缓冲液对MFC处理垃圾渗滤液液有一定影响，其中扩散至阳极的TP随渗滤液浓度的升高而减小，且低于阴极TP的去除量；各组MFCs的阳极出水中TP均维持在一定的浓度范围，依次为曝气MFC(16.55mg/L)不曝气MFC (19.13mg/L)化学MFC (23.65mg/L)。 化学MFC和曝气MFC利用100%的垃圾渗滤液进行产电时，最大输出电压分别为698.9715mV、459.4029mV，最大输出功率为197.73mW/m3、147.65mW/m3，内阻均上升分别为900、700；经过45d运行产电后，COD由初始的6332.11mg/L分别降至2752.41mg/L、2261.72mg/L，去除率分别为56.53%、64.28%，库伦效率分别为14.28%、17.10%；氨氮的去除比例分别为53.78%、58.09%，均出现了阳极室中高浓度的NH4+通过质子交换膜扩散到阴极的现象。
[Abstract]:Landfill leachate is harmful to the environment because of its high COD, BOD, NH3-N, heavy metal ions and complex toxic organic pollutants. Biocathodic microbial fuel cell (MFC) has the characteristics of high excellence, strong odor, high toxicity and difficult treatment, and it is harmful to the environment. In this paper, two-chamber aerated MFC and two-chamber non-aerated MFC were constructed by using potassium ferricyanide as cathode electron acceptor, and the start-up and performance of each MFC were tracked and compared. On this basis, different cathode MFCs were used to treat waste. The electricity generation of landfill leachate and the degradation effect of pollutants are explored.
MFC start-up is essentially a process of gradual enrichment of microorganisms on the anode surface to form biofilm. Under the condition of NaAC as the anode carbon source, the start-up time of MFC (1d) aerated MFC (5d) non-aerated MFC (10d), and the stable period of MFC (30d) aerated MFC (25d) chemical MFC (20d) is in turn. The order of voltage is: aerated MFC (618 mV) non-aerated MFC (561 mV) chemical MFC (467 mV). After the start-up, the battery runs stably. The order of open-circuit voltage is: aerated MFC (835.30 mV) non-aerated MFC (790.26 mV) chemical MFC (546.23 mV); the order of maximum power density is: aerated MFC (442.54 mW/m3) non-aerated MFC (237.04 mW/m3). MFC (201.8 mW/m3) was used as the cathode carbon source. The order of internal resistance of the cell was as follows: no aerated MFC (450) aerated MFC (600) chemical MFC (620). With NaAC as the anode carbon source, the power generation performance of the cathode MFC was better than that of the cathode MFC with potassium ferricyanide as the electron acceptor.
There is a periodic relationship between the generation voltage of different cathode MFCs and the dilution ratio of anode leachate. The average maximum generation voltage of batteries in each cycle is chemical MFC (about 630 mV) aerated MFC (about 380 mV) non-aerated MFC (about 330 mV). Chemical MFC is mainly affected by the content of potassium ferricyanide, aerated MFC is mainly related to the cathodic dissolved oxygen and the stability of microbial flora, non-aerated MFC is mainly affected by the content of cathodic nutrients.
In the treatment of leachate with different volume ratios, the change trend of COD removal rate of MFCs anode is basically the same as that of output voltage, that is, the COD removal rate of aerated/non-aerated MFC cathode is higher than that of anode; the Coulomb efficiency of MFCs in each group decreases with the increase of initial leachate ratio and the maximum Coulomb efficiency of MFCs in each group. The order is aerated MFC (10.26%) chemical MFC (4.3%) non-aerated MFC (1.46%).
The removal rate of NH4 + - N increased with the increase of leachate proportion, and partially migrated to cathode under the action of concentration gradient; the removal rate of NO3 - N increased and then decreased, and the accumulation of NO2 - N was not found in the anode chamber; the removal rate of three kinds of N was in turn aerated after the treatment of leachate with the same dilution ratio. In addition, cathode buffer had some effect on MFC treatment of landfill leachate, in which TP diffused to the anode decreased with the leachate concentration increasing, and was lower than cathode TP removal; TP in the anode effluent of all MFCs maintained a certain concentration. The degree range is aeration MFC (16.55mg/L), non aeration MFC (19.13mg/L) chemical MFC (23.65mg/L).
The maximum output voltage of chemical MFC and aerated MFC was 698.9715 mV, 459.4029 mV, the maximum output power was 197.73 mW/m3, 147.65 mW/m3, and the internal resistance increased by 900,700 respectively when 100% landfill leachate was used for power generation. After 45 days of operation, COD decreased from 6332.11 mg/L to 2752.41 mg/L and 2261.72 mg/L, respectively, and the removal rate was 5.73 mW/m3 and 147.65 mW/m3, respectively. The removal ratios of ammonia and nitrogen were 53.78% and 58.09%, respectively. The diffusion of NH4+ from anode chamber to cathode through proton exchange membrane was observed.
【学位授予单位】：重庆大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：X703;TM911.45
本文编号：2188404
[Abstract]:Landfill leachate is harmful to the environment because of its high COD, BOD, NH3-N, heavy metal ions and complex toxic organic pollutants. Biocathodic microbial fuel cell (MFC) has the characteristics of high excellence, strong odor, high toxicity and difficult treatment, and it is harmful to the environment. In this paper, two-chamber aerated MFC and two-chamber non-aerated MFC were constructed by using potassium ferricyanide as cathode electron acceptor, and the start-up and performance of each MFC were tracked and compared. On this basis, different cathode MFCs were used to treat waste. The electricity generation of landfill leachate and the degradation effect of pollutants are explored.
MFC start-up is essentially a process of gradual enrichment of microorganisms on the anode surface to form biofilm. Under the condition of NaAC as the anode carbon source, the start-up time of MFC (1d) aerated MFC (5d) non-aerated MFC (10d), and the stable period of MFC (30d) aerated MFC (25d) chemical MFC (20d) is in turn. The order of voltage is: aerated MFC (618 mV) non-aerated MFC (561 mV) chemical MFC (467 mV). After the start-up, the battery runs stably. The order of open-circuit voltage is: aerated MFC (835.30 mV) non-aerated MFC (790.26 mV) chemical MFC (546.23 mV); the order of maximum power density is: aerated MFC (442.54 mW/m3) non-aerated MFC (237.04 mW/m3). MFC (201.8 mW/m3) was used as the cathode carbon source. The order of internal resistance of the cell was as follows: no aerated MFC (450) aerated MFC (600) chemical MFC (620). With NaAC as the anode carbon source, the power generation performance of the cathode MFC was better than that of the cathode MFC with potassium ferricyanide as the electron acceptor.
There is a periodic relationship between the generation voltage of different cathode MFCs and the dilution ratio of anode leachate. The average maximum generation voltage of batteries in each cycle is chemical MFC (about 630 mV) aerated MFC (about 380 mV) non-aerated MFC (about 330 mV). Chemical MFC is mainly affected by the content of potassium ferricyanide, aerated MFC is mainly related to the cathodic dissolved oxygen and the stability of microbial flora, non-aerated MFC is mainly affected by the content of cathodic nutrients.
In the treatment of leachate with different volume ratios, the change trend of COD removal rate of MFCs anode is basically the same as that of output voltage, that is, the COD removal rate of aerated/non-aerated MFC cathode is higher than that of anode; the Coulomb efficiency of MFCs in each group decreases with the increase of initial leachate ratio and the maximum Coulomb efficiency of MFCs in each group. The order is aerated MFC (10.26%) chemical MFC (4.3%) non-aerated MFC (1.46%).
The removal rate of NH4 + - N increased with the increase of leachate proportion, and partially migrated to cathode under the action of concentration gradient; the removal rate of NO3 - N increased and then decreased, and the accumulation of NO2 - N was not found in the anode chamber; the removal rate of three kinds of N was in turn aerated after the treatment of leachate with the same dilution ratio. In addition, cathode buffer had some effect on MFC treatment of landfill leachate, in which TP diffused to the anode decreased with the leachate concentration increasing, and was lower than cathode TP removal; TP in the anode effluent of all MFCs maintained a certain concentration. The degree range is aeration MFC (16.55mg/L), non aeration MFC (19.13mg/L) chemical MFC (23.65mg/L).
The maximum output voltage of chemical MFC and aerated MFC was 698.9715 mV, 459.4029 mV, the maximum output power was 197.73 mW/m3, 147.65 mW/m3, and the internal resistance increased by 900,700 respectively when 100% landfill leachate was used for power generation. After 45 days of operation, COD decreased from 6332.11 mg/L to 2752.41 mg/L and 2261.72 mg/L, respectively, and the removal rate was 5.73 mW/m3 and 147.65 mW/m3, respectively. The removal ratios of ammonia and nitrogen were 53.78% and 58.09%, respectively. The diffusion of NH4+ from anode chamber to cathode through proton exchange membrane was observed.
【学位授予单位】：重庆大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：X703;TM911.45
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