厌氧颗粒污泥对活性黑KN-B染料的生物降解脱色研究
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摘要
论文研究了以葡萄糖为共基质条件下常温升流式厌氧污泥床(UASB)反应器中活性黑KN-B染料的脱色效果;并进行了生物吸附及降解的静态批式试验,探讨了染料脱色的机理。通过考察厌氧条件下活性黑KN-B的生物降解过程,初步分析了活性黑KN-B染料的降解动力学;又考察了碳源浓度、染料浓度、pH值、温度、盐度对活性黑KN-B染料厌氧生物降解脱色的影响;采用紫外-可见光谱、红外光谱对染料的降解途径进行分析,初步得出了染料的降解途径和降解产物。
首先研究了以葡萄糖为共基质及在不同硫酸盐浓度条件下,常温UASB反应器中活性黑KN-B的脱色效果,结果表明:当HRT=24h,进水COD_(Cr)浓度为800～1300mg/L,染料浓度10～40mg/L时,COD_(Cr)去除率、染料的脱色率分别在54.2%、72%以上,此时反应器出水挥发酸(VFA)在200mg乙酸/L以下,出水碱度在508～668mgCaCO_3/L之间。适量的硫酸盐(<500 mg/L)对反应器的COD_(Cr)去除率、染料的脱色率影响不大;但高浓度的硫酸盐(>800 mg/L)会导致COD_(Cr)去除率、染料的脱色率逐渐下降。当硫酸盐浓度为1500 mg/L时,COD_(Cr)去除率、染料脱色率仅为38.3%、65.8%,出水VFA的浓度接近400乙酸mg/L,碱度降至200mgCaCO_3/L以下,反应器有酸化的危险。反应器中厌氧颗粒污泥粒径大小为0.5～5mm,其微生物以丝状菌为主,另有少量球状菌和竹节状杆菌。
然后通过生物吸附及降解的静态批式试验,分析了染料生物降解脱色的机理。由吸附试验得出,厌氧颗粒污泥对活性黑KN-B的吸附均符合Freundlich模型和Langmuir模型,但吸附量较小。对活性黑KN-B的吸附机理研究发现,污泥菌体中的负电性会对在溶液中以阴离子形式存在的活性黑KN-B染料产生一定的排斥作用,因而导致厌氧颗粒污泥对其吸附能力低;通过吸附试验,24h后染料的吸附率仅为14.3%,并且600nm处染料的最大吸收波长并没有发生改变;而通过降解试验,24h后染料的脱色率为80.1%,且600nm处的吸收峰几乎消失,说明厌氧颗粒污泥对活性黑KN-B染料的脱色作用主要是生物降解,而不是吸附作用。
在厌氧生物降解静态试验的基础上,又考察了活性黑KN-B染料的生物降解过程,初步探讨了活性黑KN-B染料的降解动力学。结果表明:厌氧颗粒污泥可以单独降解活性黑KN-B(以活性黑为单一碳源时,活性黑KN-B的24h脱色率为43.1%),也可以在以葡萄糖为共基质条件下降解活性黑KN-B;以活性黑KN-B为单一碳源时其降解过程符合一级反应动力学方程,而以葡萄糖为共基质时其降解过程符合二级反应动力学方程。
进一步通过厌氧生物降解静态试验,本文还考察了碳源浓度、染料浓度、pH值、温度、盐度对活性黑KN-B染料厌氧生物降解脱色的影响。通过正交试验,得出了厌氧颗粒污泥对活性黑KN-B染料废水的最佳脱色条件为:染料浓度为50mg/L、温度为50℃、pH值为8、含盐量为500mg/L,此时染料的脱色率可达87.5%。
最后,对降解前和降解后染料的降解液采用UV-可见光谱、红外光谱分析,讨论了活性黑KN-B染料的降解途径以及初步的降解产物。用UV-可见光谱发现活性黑KN-B在可见光区600nm处的吸收峰已消失,并且紫外区309nm处的吸收峰减弱,但255nm处的吸收峰增强,说明活性黑KN-B染料中的偶氮键断裂后生成芳香胺类化合物,这些中间产物一部分可在厌氧条件下进行矿化,一部分需后续进一步好氧处理才能降解。用红外光谱分析,其结果与UV-可见光谱分析一致。
The decolourization efficiencies of reactive black KN-B were researched by up-flow anaerobic sludge blanket reactor (UASB) using glucose as co-substrate by pilot-scale experiments, the mechanism of dye decolourization were also analyzed by batch adsorption and degradation tests. The degradation kinetics was then discussed by further degradation decolorization tests. The influence of carbon source concentration, dye concentration, pH, temperature, salinity on biodegradation decolorization of KN-B was also investigated. Furthermore, the degradation process of reactive black KN-B and preliminary degradation products were achieved by UV-Vis and IR spectrum.
The decolourization of reactive black KN-B was investigated by the UASB reactor using glucose as co-substrate and at various sulfate concentrations. The results showed that the average removal of COD_(Cr) and color higher than 60% and 72% were achieved, respectively, when COD_(Cr) and dye concentration of influent was 800-1300mg·L~(-1) and 10-40 mg·L~(-1), respectively, the conditions were: the tempreture was 20-29°C, hydraulic retention time (HRT) was 24h, the effluent VFA was lower than 200 mg·L~(-1), alkalinity was 508-668mgCaCO_3·L~(-1). The concentration of sulfate lower than 500 mg·L~(-1) had no effect on COD_(Cr) and dye removal efficiencies, but sulfate concentration higher than 800 mg·L~(-1) would result in COD_(Cr) and color removal efficiencies gradually reducing. When sulfate concentration reached 1500 mg·L~(-1), COD_(Cr) and color removal efficiencies were only 38.3%, 65.8%, respectively; the effluent VFA approached to 400 mg·L~(-1), alkalinity was lower than 200mgCaCO_3/L, the reactor was badly affected. Diameter of anaerobic granular sludge was 0.5-5mm in the UASB reactor, microbe was not only dominated by filamentous bacteria, but also some cocci and bacilli.
The mechanism of dye decolourization was also reseached by the adsorption and degradation tests. Adsorption of the dye by anaerobic granular sludge fitted well both Freundlich model (R~2 =0.9824) and Langmuir model (R~2 =0.9460), however, the adsorption amount of reactive black KN-B was low. By discussing the adsorption mechanism of reactive black KN-B, it indicated that the negatively charged sludge would have certain repulsive interaction to reactive black KN-B existing in form of anionic in solutions, which resulted in the low adsorption amount. The adsorption rate was only 14.3%, and the absorption peak at 600 nm didn't change during the adsorption tests, while the color removal rate was 80.1% and the maximum absorption wavelength almost vanished during degradation, so the decolorization of reactive black was due mainly to degradation, rather than adsorption.
Furthermore, the degradation experiment of reactive black KN-B in keeping with time was performed, and degradation kinetics was analyzed at the same time. The conclusion demonstrated that anaerobic granular sludge could decompose reactive black KN-B with or without glucose as a co-substrate (reactive black KN-B was reduced by 43.1% through 24 hours' anaerobic treatment with dye as sole carbon source). The degradation of reactive black KN-B with or without the presence of glucose conformed to the first order reaction and the second order reaction, respectively.
The degradation decolorization of reactive black KN-B wastewater by anaerobic granular sludge was then carried out by treating compounding simulated wastewater in the 250mL flasks reactor. The effect of carbon source concentration, dye concentration, pH, temperature, salinity on biodegradation decolorization of KN-B was investigated. Through the orthogonal experiment, the optimal conditions for reactive black KN-B wastewater decolorization were obtained: dye concentration 50 mg·L~(-1), temperature 50℃, pH=8, salinity 500 mg·L~(-1). The decolorization rate of dye was up to 87.5%.
From the UV-Vis and IR spectrum of dye before and after degradation, the absorption peak at 600 nm in the visible region, at 309nm and at 255nm in the ultraviolet region vanished, decreased and increased, respectively. It proved that aromatic amines produced after the cleavage of the azo linkage, most of them could not be metabolized anaerobically, which need be degraded by further aerobic treatment. The results were in accordance with IR spectrum'.
首先研究了以葡萄糖为共基质及在不同硫酸盐浓度条件下,常温UASB反应器中活性黑KN-B的脱色效果,结果表明:当HRT=24h,进水COD_(Cr)浓度为800～1300mg/L,染料浓度10～40mg/L时,COD_(Cr)去除率、染料的脱色率分别在54.2%、72%以上,此时反应器出水挥发酸(VFA)在200mg乙酸/L以下,出水碱度在508～668mgCaCO_3/L之间。适量的硫酸盐(<500 mg/L)对反应器的COD_(Cr)去除率、染料的脱色率影响不大;但高浓度的硫酸盐(>800 mg/L)会导致COD_(Cr)去除率、染料的脱色率逐渐下降。当硫酸盐浓度为1500 mg/L时,COD_(Cr)去除率、染料脱色率仅为38.3%、65.8%,出水VFA的浓度接近400乙酸mg/L,碱度降至200mgCaCO_3/L以下,反应器有酸化的危险。反应器中厌氧颗粒污泥粒径大小为0.5～5mm,其微生物以丝状菌为主,另有少量球状菌和竹节状杆菌。
然后通过生物吸附及降解的静态批式试验,分析了染料生物降解脱色的机理。由吸附试验得出,厌氧颗粒污泥对活性黑KN-B的吸附均符合Freundlich模型和Langmuir模型,但吸附量较小。对活性黑KN-B的吸附机理研究发现,污泥菌体中的负电性会对在溶液中以阴离子形式存在的活性黑KN-B染料产生一定的排斥作用,因而导致厌氧颗粒污泥对其吸附能力低;通过吸附试验,24h后染料的吸附率仅为14.3%,并且600nm处染料的最大吸收波长并没有发生改变;而通过降解试验,24h后染料的脱色率为80.1%,且600nm处的吸收峰几乎消失,说明厌氧颗粒污泥对活性黑KN-B染料的脱色作用主要是生物降解,而不是吸附作用。
在厌氧生物降解静态试验的基础上,又考察了活性黑KN-B染料的生物降解过程,初步探讨了活性黑KN-B染料的降解动力学。结果表明:厌氧颗粒污泥可以单独降解活性黑KN-B(以活性黑为单一碳源时,活性黑KN-B的24h脱色率为43.1%),也可以在以葡萄糖为共基质条件下降解活性黑KN-B;以活性黑KN-B为单一碳源时其降解过程符合一级反应动力学方程,而以葡萄糖为共基质时其降解过程符合二级反应动力学方程。
进一步通过厌氧生物降解静态试验,本文还考察了碳源浓度、染料浓度、pH值、温度、盐度对活性黑KN-B染料厌氧生物降解脱色的影响。通过正交试验,得出了厌氧颗粒污泥对活性黑KN-B染料废水的最佳脱色条件为:染料浓度为50mg/L、温度为50℃、pH值为8、含盐量为500mg/L,此时染料的脱色率可达87.5%。
最后,对降解前和降解后染料的降解液采用UV-可见光谱、红外光谱分析,讨论了活性黑KN-B染料的降解途径以及初步的降解产物。用UV-可见光谱发现活性黑KN-B在可见光区600nm处的吸收峰已消失,并且紫外区309nm处的吸收峰减弱,但255nm处的吸收峰增强,说明活性黑KN-B染料中的偶氮键断裂后生成芳香胺类化合物,这些中间产物一部分可在厌氧条件下进行矿化,一部分需后续进一步好氧处理才能降解。用红外光谱分析,其结果与UV-可见光谱分析一致。
The decolourization efficiencies of reactive black KN-B were researched by up-flow anaerobic sludge blanket reactor (UASB) using glucose as co-substrate by pilot-scale experiments, the mechanism of dye decolourization were also analyzed by batch adsorption and degradation tests. The degradation kinetics was then discussed by further degradation decolorization tests. The influence of carbon source concentration, dye concentration, pH, temperature, salinity on biodegradation decolorization of KN-B was also investigated. Furthermore, the degradation process of reactive black KN-B and preliminary degradation products were achieved by UV-Vis and IR spectrum.
The decolourization of reactive black KN-B was investigated by the UASB reactor using glucose as co-substrate and at various sulfate concentrations. The results showed that the average removal of COD_(Cr) and color higher than 60% and 72% were achieved, respectively, when COD_(Cr) and dye concentration of influent was 800-1300mg·L~(-1) and 10-40 mg·L~(-1), respectively, the conditions were: the tempreture was 20-29°C, hydraulic retention time (HRT) was 24h, the effluent VFA was lower than 200 mg·L~(-1), alkalinity was 508-668mgCaCO_3·L~(-1). The concentration of sulfate lower than 500 mg·L~(-1) had no effect on COD_(Cr) and dye removal efficiencies, but sulfate concentration higher than 800 mg·L~(-1) would result in COD_(Cr) and color removal efficiencies gradually reducing. When sulfate concentration reached 1500 mg·L~(-1), COD_(Cr) and color removal efficiencies were only 38.3%, 65.8%, respectively; the effluent VFA approached to 400 mg·L~(-1), alkalinity was lower than 200mgCaCO_3/L, the reactor was badly affected. Diameter of anaerobic granular sludge was 0.5-5mm in the UASB reactor, microbe was not only dominated by filamentous bacteria, but also some cocci and bacilli.
The mechanism of dye decolourization was also reseached by the adsorption and degradation tests. Adsorption of the dye by anaerobic granular sludge fitted well both Freundlich model (R~2 =0.9824) and Langmuir model (R~2 =0.9460), however, the adsorption amount of reactive black KN-B was low. By discussing the adsorption mechanism of reactive black KN-B, it indicated that the negatively charged sludge would have certain repulsive interaction to reactive black KN-B existing in form of anionic in solutions, which resulted in the low adsorption amount. The adsorption rate was only 14.3%, and the absorption peak at 600 nm didn't change during the adsorption tests, while the color removal rate was 80.1% and the maximum absorption wavelength almost vanished during degradation, so the decolorization of reactive black was due mainly to degradation, rather than adsorption.
Furthermore, the degradation experiment of reactive black KN-B in keeping with time was performed, and degradation kinetics was analyzed at the same time. The conclusion demonstrated that anaerobic granular sludge could decompose reactive black KN-B with or without glucose as a co-substrate (reactive black KN-B was reduced by 43.1% through 24 hours' anaerobic treatment with dye as sole carbon source). The degradation of reactive black KN-B with or without the presence of glucose conformed to the first order reaction and the second order reaction, respectively.
The degradation decolorization of reactive black KN-B wastewater by anaerobic granular sludge was then carried out by treating compounding simulated wastewater in the 250mL flasks reactor. The effect of carbon source concentration, dye concentration, pH, temperature, salinity on biodegradation decolorization of KN-B was investigated. Through the orthogonal experiment, the optimal conditions for reactive black KN-B wastewater decolorization were obtained: dye concentration 50 mg·L~(-1), temperature 50℃, pH=8, salinity 500 mg·L~(-1). The decolorization rate of dye was up to 87.5%.
From the UV-Vis and IR spectrum of dye before and after degradation, the absorption peak at 600 nm in the visible region, at 309nm and at 255nm in the ultraviolet region vanished, decreased and increased, respectively. It proved that aromatic amines produced after the cleavage of the azo linkage, most of them could not be metabolized anaerobically, which need be degraded by further aerobic treatment. The results were in accordance with IR spectrum'.
引文
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