UASB-MBR工艺短程硝化—同时甲烷化反硝化研究
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摘要
在能源紧缺,全球气候变暖的情况下,节能减碳和高效的污水治理技术已经成为研究的热点与重点。本研究采用UASB-MBR组合工艺系统试图在实现同时有机碳与氮去除的前提下,最大化保证厌氧产甲烷的功能,目的在于为新加坡新生水厂提供可靠的进水来源,同时也为低浓度市政污水处理开辟一条高质、高效、产能的新路径。
本研究中,MBR被选为UASB出水的后处理设施,在保障高效稳定的出水质量的前提下,实现污水中NH_4~+-N的氨氧化-硝化过程;而前置的UASB系统既要实现水体中反硝化的去除氮的功能,又要最大限度的保证UASB产甲烷的优势。鉴于甲烷化与反硝化是由两类相互独立的厌氧微生物完成,并且反硝化的底物以及中间产物对甲烷化有较大的抑制与毒害作用。因此,在组合系统操作前,首先采用批试验的方法研究反硝化对甲烷化的抑制作用和甲烷菌的适应能力。试验结果显示:当底物中的NO_2~--N浓度高于15mg/L时,能对有机碳的降解速率产生一定的抑制作用;而当以NO_3~--N为反硝化底物时,显著的抑制作用发生在底物浓度高于60 mg/L时;NO_2~--N比NO_3~--N对厌氧条件下有机碳的降解具有更强的抑制作用。但是以NO_2~--N为底物的反硝化过程具有较快的反应速率,相对抑制作用时间短,且对于环境pH和温度的适应范围更广。
为了进一步验证同时甲烷化/反硝化的长期稳定性与可行性,本试验中以不同浓度的反硝化底物NO_2~--N为代表,进行了长期抑制或适应性实验研究。结果显示:在较低的NO_2~--N浓度条件下,厌氧系统能够很好的实现有机碳与氮去除,并且甲烷的产生与回收利用仅受到较小的影响;而在较高NO_2~--N浓度条件下,尽管有机碳与氮的去除效率不变,但是产生的气体中以N_2为主,破坏了厌氧产能的功能。DGGE指纹图谱也证明高NO_2~--N浓度条件下,系统中菌群分布以及优势菌群发生了显著的变化。因此,要想在厌氧系统中实现反硝化的同时回收利用甲烷,就只能在相对较低的NO_2~--N浓度下进行,换言之,这种脱碳、脱氮、产能的一体化过程只适用于处理低氮负荷的废水。
因此,UASB-MBR组合工艺的操作适用于低浓度生活污水处理,不同运行条件的调查结果显示:随着循环比从50%增加到800%的过程中,TN的去除效率从48.1%增加到82.8%;在系统实现较高的有机碳与氮去除的同时,甲烷生成没有因为反硝化的引入而受到显著的影响,这主要是系统中实现了短程硝化反硝化的结果,在确保较低碳源竞争的同时,缩短了对甲烷菌的抑制时间;但当循环比从400%增加到800%时,TN的去除效率仅轻微增加,较大的上流速率和较高的DO条件却破坏了UASB系统运行的稳定性。因此建议根据进水中氮含量将循环比控制在200-400%之间能够达到比较满意的效果。同时,研究了MBR中曝气强度对系统运行的稳定性的影响:在较低的曝气速率条件下,能够维持系统中较高的甲烷产量,但是较低的硝化速率抑制了系统中TN的去除表现;在曝气速率高于2.5 L/min时,系统中TN去除能够达到80%,并且UASB中存在的部分好氧菌,对厌氧环境起到了一定的保护作用,使得甲烷的产生量随着DO浓度的升高仅轻微的降低。因此,在控制适当的循环比和曝气强度的条件下,这种技术在处理生活污水中是可行的,在完成有机碳与氮去除的同时实现了甲烷气的回收利用,并且系统污泥产量较低,后处理费用降低。
经过进一步的实验验证:这种伴随着甲烷产生的高氮去除过程主要是由于系统中实现了短程硝化反硝化。MBR中NO_2~--N的累积现象主要是由于活性污泥混合液在厌氧与好氧环境下的内循环模式,较高的pH值以及较低的C/N比加速了对硝酸盐氧化菌(NOB)的抑制和淘洗作用而实现的,从而使UASB-MBR组合工艺在处理低浓度生活污水中实现了高出水质量、高处理效率和较高的甲烷能源回收。
最后,针对本UASB-MBR组合工艺中MBR的膜污染形成过程、膜污染物主要成份以及膜污染控制方法进行了初步的研究与探讨,结果显示:该运行条件下MBR的膜污染速率较高,几乎呈线性增长趋势,胶体粒子和溶解性有机物,尤其是分子量与膜孔径相当的物质,比大的污泥絮体更容易沉积到膜表面,形成过滤凝胶层,加速膜污染进程;同时注意到当悬浮液中蛋白质为EPS主要成分时,多糖确是膜污染物中EPS的主要成分,尤其是在污染物形成的初期,多糖是构成污染物的主要物质。试验也同时证明了间歇运行模式和气体曝气剪切力模式都是有效的减缓膜污染的方法。间歇运行时,膜污染速率随着闲置时间的延长而降低,尤其是在高通量条件下,间歇运行对膜污染的改善更加明显;但当采用气体曝气模式时,存在最佳曝气强度。
The energy crisis and environment deterioration are two of the main problems the world is facing today.Hence,the simultaneous bio-energy production and nutrient removal has been given much attention in the wastewater treatment techniques during the last decade.The aim of this study is to establish a feasible method of treating municipal wastewater in an UASB coupled with an aerobic MBR.The pre-UASB was designed to retain a high carbon level for denitrification via nitrite and for methanogenesis and to proved the low C/N ratio effluent feeding to the MBR to perform the partial nitrification step while the MBR performed the nitrification step and improved the effluent quality.Therefore,the focus of this work was to investigate simultaneous carbon and nitrogen removal by shortcut nitrification and denitrification with a methane production process treating low strength synthetic wastewater in a combined UASB-MBR system.
Firstly,a series of experiments was carried out to find out the impact factors and feasibility on a simultaneous methanogenesis and shortcut/complete denitrification process using the adapted anaerobic mixed methanogenic culture.The results suggested that the obvious inhibition of NO_X~--N addition on carbon removal rate started to be observed when the initial NO_2~--N concentration was higher than 15 mg/L and the initial NO_3~--N concentration was higher than 60 mg/L.Whereas,the less carbon requirement for denitrification and faster denitrification rate via NO_2~--N than NO_3~--N still allowed methanogenesis to proceed in the same bioreactor treating wastewater with a lower NO_2~--N concentration,but with a higher TOC/TN ratio under the optimal temperature of 30-35℃and pH of 7.0-8.0.
Under the same optimal conditions,a long-term inhibition assay in an up-flow anaerobic sludge blanket(UASB) treating the synthetic NO_2~--N concentration wastewater indicated that the stable carbon and nitrogen removal efficiencies with an acceptable biogas production rate only could be obtained at the low NO_2~--N concentration although the varieties of dominant bacterial community composition were observed in the PCR-DGGE analysis results.At the high NO_2~--N concentration,the higher N_2,but lower CH_4 production was observed eventhough the carbon and nitrogen removal efficiencies maintaining at high level.It is indicated that the technique of simultaneous methane production and nitrogen removal only can be used to treat a low nitrogen strength wastewater.
Secondly,a combined bioenergy production and nitrogen removal system consisting of an UASB and MBR was developed to treat synthetic municipal wastewater.The results indicated that the simultaneous methanogenesis and denitrification for treating a low strength synthetic municipal wastewater was technically feasible with more than 98.0%total TOC removal,98.0%NH_4~+-N removal and 48.1-82.8%TN removal as the recycling ratio increased from 50%to 800%.In this combined UASB-MBR system,the methane production was not affected obviously by the denitrification process.A slight reduction in the methane percentage up to a recycling ratio of 400%was observed due to an increased nitrogen production.However,at the highest recycling ratio of 800%,a rapid decrease in the methane percentage occurred.It was probably due to high DO concentration was introduced into the UASB,which restrained the activity of methanogens and induced more organic substances being converted to CO_2 instead of methane according to the anoxic or aerobic biodegradation theories.Hence,the results indicated that the recycle ratio should be controlled at the range of 200-400%considering the nitrogen concentration and the discharged criterion.
At the same time,the effect of aeration rate in the MBR on the combined system performance was investigated.Optimal aeration rate range(2.5-5.0 L/min) was suggested based on the methane production and ratio as well as stable TOC(＞98%) and TN removal efficiencies(＞80%).At the low aeration rate,high methane production and ratio were achieved,but TN removal performance was restrained by the nitrification efficiencies.When the aeration rate was above 2.5 L/min,TN removal performance arrived to around 80%and could not be affected by the nitrification and denitrification efficiencies.However,the methane production decreased slightly follwong the increase in the DO concentration.
Hence,in the combined UASB-MBR system,simultaneous methane production and denitrification was technically feasible as an energy efficiently treating way to achieve high effluent quality,minimal biosolids generation,and optimal nitrogen removal efficiencies by controlling the recycling ratio and aeration rate.
Thirdly,the NO_2~--N accumulation was considered as the key factor to achieve simultaneous methanogenesis and denitrification using a combined UASB and MBR treating municipal wastewater.Based on analysis results,it was suggested that the internal recirculation pattern,higher pH and lower C/N ratio were the important factors leading to partial nitrification in the combined UASB-MBR.
Lastly,membrane fouling tendency,foultant composition,fouling mechanism and the fouling control methods were investigated and researched.The higher fouling rate present in the MBR treating anaerobic digestion effluent.The membrane foulants consisted of sludge flocs,colloidal particles and solutes,especially,the small particles in sludge suspension,those diameter are similar with the membrane pore size,had a strong deposit tendency on the membrane surface.At the same time,the polysaccharide was observed as the main EPS on the membrane surface while the protein is the main contain in the suspernant EPS.
Intermittent suction and air sparing were two kinds of effective cleaning strategies to decrease the membrane fouling rate.Under the intermittent suction mode,extending idle time benefited for reducing membrane fouling.This impact was more significant under higher flux. The results of air sparing on membrane fouling tendency showed that small or large aeration intensity had a negative influence on membrane permeability.Low aeration could not remove the membrane foulants from membrane surface effectively.However,the larger aeration intensity resulted in a severe breakup of sludge floes,and promoted the release of colloidal and soluble components from the microbial floes to the bulk solution due to microbial floc breakage,thus caused a rapid loss in membrane permeability.
本研究中,MBR被选为UASB出水的后处理设施,在保障高效稳定的出水质量的前提下,实现污水中NH_4~+-N的氨氧化-硝化过程;而前置的UASB系统既要实现水体中反硝化的去除氮的功能,又要最大限度的保证UASB产甲烷的优势。鉴于甲烷化与反硝化是由两类相互独立的厌氧微生物完成,并且反硝化的底物以及中间产物对甲烷化有较大的抑制与毒害作用。因此,在组合系统操作前,首先采用批试验的方法研究反硝化对甲烷化的抑制作用和甲烷菌的适应能力。试验结果显示:当底物中的NO_2~--N浓度高于15mg/L时,能对有机碳的降解速率产生一定的抑制作用;而当以NO_3~--N为反硝化底物时,显著的抑制作用发生在底物浓度高于60 mg/L时;NO_2~--N比NO_3~--N对厌氧条件下有机碳的降解具有更强的抑制作用。但是以NO_2~--N为底物的反硝化过程具有较快的反应速率,相对抑制作用时间短,且对于环境pH和温度的适应范围更广。
为了进一步验证同时甲烷化/反硝化的长期稳定性与可行性,本试验中以不同浓度的反硝化底物NO_2~--N为代表,进行了长期抑制或适应性实验研究。结果显示:在较低的NO_2~--N浓度条件下,厌氧系统能够很好的实现有机碳与氮去除,并且甲烷的产生与回收利用仅受到较小的影响;而在较高NO_2~--N浓度条件下,尽管有机碳与氮的去除效率不变,但是产生的气体中以N_2为主,破坏了厌氧产能的功能。DGGE指纹图谱也证明高NO_2~--N浓度条件下,系统中菌群分布以及优势菌群发生了显著的变化。因此,要想在厌氧系统中实现反硝化的同时回收利用甲烷,就只能在相对较低的NO_2~--N浓度下进行,换言之,这种脱碳、脱氮、产能的一体化过程只适用于处理低氮负荷的废水。
因此,UASB-MBR组合工艺的操作适用于低浓度生活污水处理,不同运行条件的调查结果显示:随着循环比从50%增加到800%的过程中,TN的去除效率从48.1%增加到82.8%;在系统实现较高的有机碳与氮去除的同时,甲烷生成没有因为反硝化的引入而受到显著的影响,这主要是系统中实现了短程硝化反硝化的结果,在确保较低碳源竞争的同时,缩短了对甲烷菌的抑制时间;但当循环比从400%增加到800%时,TN的去除效率仅轻微增加,较大的上流速率和较高的DO条件却破坏了UASB系统运行的稳定性。因此建议根据进水中氮含量将循环比控制在200-400%之间能够达到比较满意的效果。同时,研究了MBR中曝气强度对系统运行的稳定性的影响:在较低的曝气速率条件下,能够维持系统中较高的甲烷产量,但是较低的硝化速率抑制了系统中TN的去除表现;在曝气速率高于2.5 L/min时,系统中TN去除能够达到80%,并且UASB中存在的部分好氧菌,对厌氧环境起到了一定的保护作用,使得甲烷的产生量随着DO浓度的升高仅轻微的降低。因此,在控制适当的循环比和曝气强度的条件下,这种技术在处理生活污水中是可行的,在完成有机碳与氮去除的同时实现了甲烷气的回收利用,并且系统污泥产量较低,后处理费用降低。
经过进一步的实验验证:这种伴随着甲烷产生的高氮去除过程主要是由于系统中实现了短程硝化反硝化。MBR中NO_2~--N的累积现象主要是由于活性污泥混合液在厌氧与好氧环境下的内循环模式,较高的pH值以及较低的C/N比加速了对硝酸盐氧化菌(NOB)的抑制和淘洗作用而实现的,从而使UASB-MBR组合工艺在处理低浓度生活污水中实现了高出水质量、高处理效率和较高的甲烷能源回收。
最后,针对本UASB-MBR组合工艺中MBR的膜污染形成过程、膜污染物主要成份以及膜污染控制方法进行了初步的研究与探讨,结果显示:该运行条件下MBR的膜污染速率较高,几乎呈线性增长趋势,胶体粒子和溶解性有机物,尤其是分子量与膜孔径相当的物质,比大的污泥絮体更容易沉积到膜表面,形成过滤凝胶层,加速膜污染进程;同时注意到当悬浮液中蛋白质为EPS主要成分时,多糖确是膜污染物中EPS的主要成分,尤其是在污染物形成的初期,多糖是构成污染物的主要物质。试验也同时证明了间歇运行模式和气体曝气剪切力模式都是有效的减缓膜污染的方法。间歇运行时,膜污染速率随着闲置时间的延长而降低,尤其是在高通量条件下,间歇运行对膜污染的改善更加明显;但当采用气体曝气模式时,存在最佳曝气强度。
The energy crisis and environment deterioration are two of the main problems the world is facing today.Hence,the simultaneous bio-energy production and nutrient removal has been given much attention in the wastewater treatment techniques during the last decade.The aim of this study is to establish a feasible method of treating municipal wastewater in an UASB coupled with an aerobic MBR.The pre-UASB was designed to retain a high carbon level for denitrification via nitrite and for methanogenesis and to proved the low C/N ratio effluent feeding to the MBR to perform the partial nitrification step while the MBR performed the nitrification step and improved the effluent quality.Therefore,the focus of this work was to investigate simultaneous carbon and nitrogen removal by shortcut nitrification and denitrification with a methane production process treating low strength synthetic wastewater in a combined UASB-MBR system.
Firstly,a series of experiments was carried out to find out the impact factors and feasibility on a simultaneous methanogenesis and shortcut/complete denitrification process using the adapted anaerobic mixed methanogenic culture.The results suggested that the obvious inhibition of NO_X~--N addition on carbon removal rate started to be observed when the initial NO_2~--N concentration was higher than 15 mg/L and the initial NO_3~--N concentration was higher than 60 mg/L.Whereas,the less carbon requirement for denitrification and faster denitrification rate via NO_2~--N than NO_3~--N still allowed methanogenesis to proceed in the same bioreactor treating wastewater with a lower NO_2~--N concentration,but with a higher TOC/TN ratio under the optimal temperature of 30-35℃and pH of 7.0-8.0.
Under the same optimal conditions,a long-term inhibition assay in an up-flow anaerobic sludge blanket(UASB) treating the synthetic NO_2~--N concentration wastewater indicated that the stable carbon and nitrogen removal efficiencies with an acceptable biogas production rate only could be obtained at the low NO_2~--N concentration although the varieties of dominant bacterial community composition were observed in the PCR-DGGE analysis results.At the high NO_2~--N concentration,the higher N_2,but lower CH_4 production was observed eventhough the carbon and nitrogen removal efficiencies maintaining at high level.It is indicated that the technique of simultaneous methane production and nitrogen removal only can be used to treat a low nitrogen strength wastewater.
Secondly,a combined bioenergy production and nitrogen removal system consisting of an UASB and MBR was developed to treat synthetic municipal wastewater.The results indicated that the simultaneous methanogenesis and denitrification for treating a low strength synthetic municipal wastewater was technically feasible with more than 98.0%total TOC removal,98.0%NH_4~+-N removal and 48.1-82.8%TN removal as the recycling ratio increased from 50%to 800%.In this combined UASB-MBR system,the methane production was not affected obviously by the denitrification process.A slight reduction in the methane percentage up to a recycling ratio of 400%was observed due to an increased nitrogen production.However,at the highest recycling ratio of 800%,a rapid decrease in the methane percentage occurred.It was probably due to high DO concentration was introduced into the UASB,which restrained the activity of methanogens and induced more organic substances being converted to CO_2 instead of methane according to the anoxic or aerobic biodegradation theories.Hence,the results indicated that the recycle ratio should be controlled at the range of 200-400%considering the nitrogen concentration and the discharged criterion.
At the same time,the effect of aeration rate in the MBR on the combined system performance was investigated.Optimal aeration rate range(2.5-5.0 L/min) was suggested based on the methane production and ratio as well as stable TOC(＞98%) and TN removal efficiencies(＞80%).At the low aeration rate,high methane production and ratio were achieved,but TN removal performance was restrained by the nitrification efficiencies.When the aeration rate was above 2.5 L/min,TN removal performance arrived to around 80%and could not be affected by the nitrification and denitrification efficiencies.However,the methane production decreased slightly follwong the increase in the DO concentration.
Hence,in the combined UASB-MBR system,simultaneous methane production and denitrification was technically feasible as an energy efficiently treating way to achieve high effluent quality,minimal biosolids generation,and optimal nitrogen removal efficiencies by controlling the recycling ratio and aeration rate.
Thirdly,the NO_2~--N accumulation was considered as the key factor to achieve simultaneous methanogenesis and denitrification using a combined UASB and MBR treating municipal wastewater.Based on analysis results,it was suggested that the internal recirculation pattern,higher pH and lower C/N ratio were the important factors leading to partial nitrification in the combined UASB-MBR.
Lastly,membrane fouling tendency,foultant composition,fouling mechanism and the fouling control methods were investigated and researched.The higher fouling rate present in the MBR treating anaerobic digestion effluent.The membrane foulants consisted of sludge flocs,colloidal particles and solutes,especially,the small particles in sludge suspension,those diameter are similar with the membrane pore size,had a strong deposit tendency on the membrane surface.At the same time,the polysaccharide was observed as the main EPS on the membrane surface while the protein is the main contain in the suspernant EPS.
Intermittent suction and air sparing were two kinds of effective cleaning strategies to decrease the membrane fouling rate.Under the intermittent suction mode,extending idle time benefited for reducing membrane fouling.This impact was more significant under higher flux. The results of air sparing on membrane fouling tendency showed that small or large aeration intensity had a negative influence on membrane permeability.Low aeration could not remove the membrane foulants from membrane surface effectively.However,the larger aeration intensity resulted in a severe breakup of sludge floes,and promoted the release of colloidal and soluble components from the microbial floes to the bulk solution due to microbial floc breakage,thus caused a rapid loss in membrane permeability.
引文
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