零价铁强化厌氧废水处理的研究
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摘要
厌氧生物处理技术由于其在降解污染物的同时能够产生可利用的能源,被广泛地应用于废水的处理过程。其中,颗粒污泥的形成是上流式厌氧污泥床反应器的主要特征,因为其具有较高的生物处理能力。但是污泥颗粒化需要较长的时间,因而关于强化这一过程的方法被广泛研究。同时,厌氧断裂偶氮键在处理印染废水时展现出了经济和环境友好性,但是在处理较高浓度的染料废水时,其性能会大幅下降。另外,水解酸化作为一种厌氧预处理手段,在实际应用时也面临着处理效果较差的难题。而零价铁作为一种较好的还原剂,通过强化厌氧氛围来提高厌氧消化的处理效果在本课题中被相应研究。根据本课题的实验研究和理论分析,可以得出如下结论：
1、电场强化的内置零价铁厌氧反应器能够加快厌氧颗粒化进程。实验在三个平行的反应器中进行：电场强化的内置零价铁厌氧反应器(R1)、零价铁厌氧反应器(R2)以及普通的厌氧反应器(R3)。当1.4 V的电压作用于R1时,在接下来的4天里其COD去除率由60.3%上升到90.7%,同时38天内颗粒粒径由151.4μm增长到695.1μm。R2和R3中的COD去除率以及粒径的增加都要比R1小。电场使得零价铁的缓冲作用得到增强,并促使反应器内保持较低的氧化还原电位。除此之外,电场增加了二价铁离子的溶出和胞外聚合物的产量。这些都是有利于甲烷化以及颗粒化作用的。扫描电子显微镜照片表明R1中的颗粒污泥内外微生物分布不同。荧光原位杂交实验显示出R1中的产甲烷菌的相对丰度明显高于R2和R3反应器。以上的结果说明电场和零价铁的耦合作用能够有效地促进污泥颗粒化。
2、电场强化的内置零价铁厌氧反应器可以提高印染废水处理效果。实验在三个平行的反应器中进行：电场强化的内置零价铁厌氧反应器(R1)、零价铁厌氧反应器(R2)以及普通的厌氧反应器(R3)。电场强化的内置零价铁厌氧反应器R1具有最高的COD和色度去除率。提高施加电压可以增强R1的处理效果。扫描电子显微镜照片表明处理高浓度的染料废水后R1中的颗粒污泥仍然保持完整结实的结构,但是R3中的颗粒污泥则已经破碎。荧光原位杂交实验证明R1中的产甲烷菌丰度明显高于R2和R3。变形凝胶电泳显示电场和零价铁的耦合作用增加了微生物种群的结构,特别是对厌氧脱色起关键作用的菌群。
3、铁粉投加到水解酸化反应器从而强化该段作用被研究。结果表明,铁粉投加能明显提高水解酸化的效率。当水力停留时间从6 h降低到2 h时,在投加铁粉的水解酸化反应器(A1),COD去除率和酸化度分别较好地稳定在45%至56%和84%至91%之间,而参比反应器(A2)表现则分别明显地从45%下降到25%和从65%下降到30%。铁粉可以优化产酸类型,减少乙酸化较困难的丙酸的形成。铁粉的加入使水解酸化反应器A1中的丙酸占总挥发性脂肪酸的比例降低14%-20%,而乙酸和丁酸的含量则分别增加8%-11%和6%-9%。以上这些作用促进了反应器A1后续的甲烷化处理过程,而反应器A2后续的甲烷化过程中却发现了较高浓度的丙酸积累。铁粉使铁氧还蛋白的活性增加了17倍,这有助于加快产酸过程；荧光原位杂交实验证实,铁粉的加入使水解酸化反应器的产乙酸菌丰度明显提高,这与反应器中较高的乙酸含量的结果相一致。铁粉对水解酸化的强化效应,可对于降低后续处理负荷、形成更有利的有机酸形式起明显作用,有望在废水的预处理、两相厌氧发酵乃至污泥发酵中得到更有效的应用。
Anaerobic digestion (AD) of organic matters is a widely used technology in the efficient treatment of organic waste and the simultaneous generation of renewable energy source. With respect to Upflow anaerobic sludge blanket (UASB), the presence of granular sludge is a major characteristic of anaerobic reactor, which leads to high biodegradation efficiency. However, sludge granulation is a long-term process that generally takes three to eight months. Efforts need to enhance this process. Also, anaerobic reduction of azo linkages (-N=N-) present economical and environmentally friendly ways to remove dyes from wastewaters, but the performance gets worse under high azo dye concentrations. In addition, anaerobic pretreatment, i.e., acidification often presents low performance in practical process and needs to be enhanced. Therefore, zero valent iron (ZVI), a reducing agent, is used to enhancing these processes at the aim of helping create an enhanced anaerobic environment that may improve the performance of anaerobic digsetion due to its reductive property. According to the experimental study and theoretical analysis, we can draw the following conclusions:
1. A zero valent iron (ZVI) bed with a pair of electrodes was installed in an upflow anaerobic sludge blanket (UASB) reactor to create an enhanced condition to increase the rate of anaerobic granulation. The effects of an electric field and ZVI on granulation were investigated in three UASB reactors operated in parallel:an electric field enhanced ZVI-UASB reactor (reactor R1), a ZVI-UASB reactor (reactor R2) and a common UASB reactor (reactor R3). When a voltage of 1.4 V was supplied to reactor R1, COD removal dramatically increased from 60.3% to 90.7% over the following four days, while the mean granule size rapidly grew from 151.4μm to 695.1μm over the following 38 days. Comparatively, COD removal was lower and the increase in granule size was slower in the other two reactors (in the order:R1>R2>R3). The electric field caused the ZVI to more effectively buffer acidity and maintain a relatively low oxidation-reduction potential in the reactor. In addition, the electric field resulted in a significant increase in ferrous ion leaching and extracellular polymeric substances (EPS) production. These changes benefited methanogenesis and granulation. Scanning electron microscopy (SEM) images showed that different microorganisms were dominant in the external and internal layers of the reactor R1 granules. Additionally, fluorescence in situ hybridization (FISH) analysis indicated that the relative abundance of methanogens in reactor R1 was significantly greater than in the other two reactors. Taken together, these results suggested that the use of ZVI combined with an electric field in an UASB reactor could effectively enhance the sludge granulation.
2. A zero valent iron (ZVI) bed with a pair of electrodes was packed in an anaerobic reactor aiming at enhancing treatment of azo dye wastewater. The experiments were carried out in three reactors operated in parallel:an electric field enhanced ZVI-anaerobic reactor (R1), a ZVI-anaerobic reactor (R2) and a common anaerobic reactor (R3). R1 presented the highest performance in removal of COD and color. Raising voltage in R1 further improved its performance. Scanning electron microscopy images displayed that the structure of granular sludge from R1 was intact after being fed with the high dye concentration, while that of R3 was broken. Fluorescence in situ hybridization analysis indicated that the abundance of methanogens in R1 was significantly greater than that in the other two reactors. Denaturing gradient gel electrophoresis showed that the coupling of electric field and ZVI increased the diversity of microbial community and especially enhanced bacterial strains responsible for decolorization.
3. A novel strategy for enhancing anaerobic wastewater treatment via dosing Fe0 powder in acidification reactor was reported in this study. Experimental results showed that Fe0 powder dosed efficiently improved the acidification performance. Acidification reactor with Fe0 dosed (Al) presented higher and more stable performances in COD removal (ranging from 45% to 56%) and the degree of acidification (ranging from 84% to 91%) when lowering the HRT from 6 h to 2 h; however, those of the reference reactor without Fe0 (A2) significantly declined from 45% to 25% and 65% to 30%, respectively. Fe0 dosed could help optimize fermentation type, especially decreasing propionate which was lower in acetification as compared with butyrate. Reactor A1 presented 14%-20% less of propionate composition, but 8%-11% and 6%-9% more of acetate and butyrate composition respectively than reactor A2. Fe0 dosed improved 17-fold of the activity of pyruvate-ferredoxin oxidoreductase which is a crucial enzyme in the hydrolysis/fermentation, leading to an enhanced acidogenesis. Fuorescence in situ hybridization analysis indicated that Fe0 dosed increased the abundance of acidogens, and especially acetogens, coincident with higher acetate production. These effects facilitated the following methanogenic performance. Therefore, the Fe0 enhanced acidification is helpful to form the favorable fermentation type and low the subsequent treatment loading, which is expected to broadly apply in wastewater pretreatment, two-stage anaerobic digestion and even waste sludge fermentation.
1、电场强化的内置零价铁厌氧反应器能够加快厌氧颗粒化进程。实验在三个平行的反应器中进行：电场强化的内置零价铁厌氧反应器(R1)、零价铁厌氧反应器(R2)以及普通的厌氧反应器(R3)。当1.4 V的电压作用于R1时,在接下来的4天里其COD去除率由60.3%上升到90.7%,同时38天内颗粒粒径由151.4μm增长到695.1μm。R2和R3中的COD去除率以及粒径的增加都要比R1小。电场使得零价铁的缓冲作用得到增强,并促使反应器内保持较低的氧化还原电位。除此之外,电场增加了二价铁离子的溶出和胞外聚合物的产量。这些都是有利于甲烷化以及颗粒化作用的。扫描电子显微镜照片表明R1中的颗粒污泥内外微生物分布不同。荧光原位杂交实验显示出R1中的产甲烷菌的相对丰度明显高于R2和R3反应器。以上的结果说明电场和零价铁的耦合作用能够有效地促进污泥颗粒化。
2、电场强化的内置零价铁厌氧反应器可以提高印染废水处理效果。实验在三个平行的反应器中进行：电场强化的内置零价铁厌氧反应器(R1)、零价铁厌氧反应器(R2)以及普通的厌氧反应器(R3)。电场强化的内置零价铁厌氧反应器R1具有最高的COD和色度去除率。提高施加电压可以增强R1的处理效果。扫描电子显微镜照片表明处理高浓度的染料废水后R1中的颗粒污泥仍然保持完整结实的结构,但是R3中的颗粒污泥则已经破碎。荧光原位杂交实验证明R1中的产甲烷菌丰度明显高于R2和R3。变形凝胶电泳显示电场和零价铁的耦合作用增加了微生物种群的结构,特别是对厌氧脱色起关键作用的菌群。
3、铁粉投加到水解酸化反应器从而强化该段作用被研究。结果表明,铁粉投加能明显提高水解酸化的效率。当水力停留时间从6 h降低到2 h时,在投加铁粉的水解酸化反应器(A1),COD去除率和酸化度分别较好地稳定在45%至56%和84%至91%之间,而参比反应器(A2)表现则分别明显地从45%下降到25%和从65%下降到30%。铁粉可以优化产酸类型,减少乙酸化较困难的丙酸的形成。铁粉的加入使水解酸化反应器A1中的丙酸占总挥发性脂肪酸的比例降低14%-20%,而乙酸和丁酸的含量则分别增加8%-11%和6%-9%。以上这些作用促进了反应器A1后续的甲烷化处理过程,而反应器A2后续的甲烷化过程中却发现了较高浓度的丙酸积累。铁粉使铁氧还蛋白的活性增加了17倍,这有助于加快产酸过程；荧光原位杂交实验证实,铁粉的加入使水解酸化反应器的产乙酸菌丰度明显提高,这与反应器中较高的乙酸含量的结果相一致。铁粉对水解酸化的强化效应,可对于降低后续处理负荷、形成更有利的有机酸形式起明显作用,有望在废水的预处理、两相厌氧发酵乃至污泥发酵中得到更有效的应用。
Anaerobic digestion (AD) of organic matters is a widely used technology in the efficient treatment of organic waste and the simultaneous generation of renewable energy source. With respect to Upflow anaerobic sludge blanket (UASB), the presence of granular sludge is a major characteristic of anaerobic reactor, which leads to high biodegradation efficiency. However, sludge granulation is a long-term process that generally takes three to eight months. Efforts need to enhance this process. Also, anaerobic reduction of azo linkages (-N=N-) present economical and environmentally friendly ways to remove dyes from wastewaters, but the performance gets worse under high azo dye concentrations. In addition, anaerobic pretreatment, i.e., acidification often presents low performance in practical process and needs to be enhanced. Therefore, zero valent iron (ZVI), a reducing agent, is used to enhancing these processes at the aim of helping create an enhanced anaerobic environment that may improve the performance of anaerobic digsetion due to its reductive property. According to the experimental study and theoretical analysis, we can draw the following conclusions:
1. A zero valent iron (ZVI) bed with a pair of electrodes was installed in an upflow anaerobic sludge blanket (UASB) reactor to create an enhanced condition to increase the rate of anaerobic granulation. The effects of an electric field and ZVI on granulation were investigated in three UASB reactors operated in parallel:an electric field enhanced ZVI-UASB reactor (reactor R1), a ZVI-UASB reactor (reactor R2) and a common UASB reactor (reactor R3). When a voltage of 1.4 V was supplied to reactor R1, COD removal dramatically increased from 60.3% to 90.7% over the following four days, while the mean granule size rapidly grew from 151.4μm to 695.1μm over the following 38 days. Comparatively, COD removal was lower and the increase in granule size was slower in the other two reactors (in the order:R1>R2>R3). The electric field caused the ZVI to more effectively buffer acidity and maintain a relatively low oxidation-reduction potential in the reactor. In addition, the electric field resulted in a significant increase in ferrous ion leaching and extracellular polymeric substances (EPS) production. These changes benefited methanogenesis and granulation. Scanning electron microscopy (SEM) images showed that different microorganisms were dominant in the external and internal layers of the reactor R1 granules. Additionally, fluorescence in situ hybridization (FISH) analysis indicated that the relative abundance of methanogens in reactor R1 was significantly greater than in the other two reactors. Taken together, these results suggested that the use of ZVI combined with an electric field in an UASB reactor could effectively enhance the sludge granulation.
2. A zero valent iron (ZVI) bed with a pair of electrodes was packed in an anaerobic reactor aiming at enhancing treatment of azo dye wastewater. The experiments were carried out in three reactors operated in parallel:an electric field enhanced ZVI-anaerobic reactor (R1), a ZVI-anaerobic reactor (R2) and a common anaerobic reactor (R3). R1 presented the highest performance in removal of COD and color. Raising voltage in R1 further improved its performance. Scanning electron microscopy images displayed that the structure of granular sludge from R1 was intact after being fed with the high dye concentration, while that of R3 was broken. Fluorescence in situ hybridization analysis indicated that the abundance of methanogens in R1 was significantly greater than that in the other two reactors. Denaturing gradient gel electrophoresis showed that the coupling of electric field and ZVI increased the diversity of microbial community and especially enhanced bacterial strains responsible for decolorization.
3. A novel strategy for enhancing anaerobic wastewater treatment via dosing Fe0 powder in acidification reactor was reported in this study. Experimental results showed that Fe0 powder dosed efficiently improved the acidification performance. Acidification reactor with Fe0 dosed (Al) presented higher and more stable performances in COD removal (ranging from 45% to 56%) and the degree of acidification (ranging from 84% to 91%) when lowering the HRT from 6 h to 2 h; however, those of the reference reactor without Fe0 (A2) significantly declined from 45% to 25% and 65% to 30%, respectively. Fe0 dosed could help optimize fermentation type, especially decreasing propionate which was lower in acetification as compared with butyrate. Reactor A1 presented 14%-20% less of propionate composition, but 8%-11% and 6%-9% more of acetate and butyrate composition respectively than reactor A2. Fe0 dosed improved 17-fold of the activity of pyruvate-ferredoxin oxidoreductase which is a crucial enzyme in the hydrolysis/fermentation, leading to an enhanced acidogenesis. Fuorescence in situ hybridization analysis indicated that Fe0 dosed increased the abundance of acidogens, and especially acetogens, coincident with higher acetate production. These effects facilitated the following methanogenic performance. Therefore, the Fe0 enhanced acidification is helpful to form the favorable fermentation type and low the subsequent treatment loading, which is expected to broadly apply in wastewater pretreatment, two-stage anaerobic digestion and even waste sludge fermentation.
引文
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