部分亚硝化耦合厌氧氨氧化的工艺控制及其垃圾渗滤液脱氮特性
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摘要
垃圾渗滤液含有高浓度的氨氮和有机物,水质水量波动性大,若采用传统硝化反硝化脱氮技术处理则能耗大和成本高。部分亚硝化(partial nitritation, PN)-厌氧氨氧化(anaerobic ammonium oxidation, ANAMMOX)耦合工艺因其显著的经济性和高效性,有潜力成为替代传统硝化反硝化处理垃圾渗滤液的生物脱氮技术。但目前PN-ANAMMOX技术尚不成熟,存在的主要障碍是：氨氧化菌(ammonia oxidation bacteria,AOB)和厌氧氨氧化菌(ANAMMOX bacteria, AnAOB)生长速率缓慢,易受水质和运行条件影响,从而导致该工艺在实际废水处理中呈现启动缓慢、工艺组合协调困难、稳定性欠缺等问题。
为解决上述问题,本课题就PN-ANAMMOX技术在单级工艺的快速启动、负荷提高、工艺控制特点,串联运行的工艺衔接与控制规律及一步式耦合工艺的快速启动、工艺控制特性方面展开研究,取得如下成果。
(1)采用序批式反应器(Sequencing batch reactor, SBR)以常规的定时曝气方式运行,分别在间歇和连续曝气下实现了部分亚硝化联合反硝化对垃圾渗滤液进行脱氮除碳处理。在这两种运行方式中,通过调控总供气量(TAF)与进水负荷(ILR)的比值可有效抑制硝氮生成,出水pH可指示PN-SBR的出水NO2--N/NH4+-N摩尔比。间歇曝气运行方式由于形成的颗粒污泥数量较多,获得的脱氮除碳效果优于连续曝气运行方式的脱氮除碳效果。
(2)在PN-SBR絮状活性污泥系统中,也可实现部分亚硝化联合反硝化对垃圾渗滤液进行脱氮除碳处理。硝氮生成的抑制也可由调控TAF/ILR比值来实现,出水pH值也可指示出水NO2--N/NH4+-N摩尔比。SBR周期分析表明,反硝化在混合液中的脱氮除碳作用分别达28%和24%。同时硝化反硝化存在于SBR的第一个曝气阶段。
(3)采用终点pH控制法可在PN-SBR长期运行中稳定实现部分亚硝化联合反硝化处理垃圾渗滤液。曝气量在0.8、1.2和1.6m3/h时对出水NO2--N/NH4+-N摩尔比几无影响。反应温度在30℃、33℃和36℃时对出水NO2--N/NH4+-N摩尔比也几无影响。每周期进水量的改变也并不明显影响出水NO2--N/NH4+-N摩尔比。
(4)通过接种PN-SBR的活性污泥和少量低活性的ANAMMOX污泥,可快速启动ANAMMOX-UASB。pH、电导率和出水硝氮浓度可作为ANAMMOX脱氮效能的指示参数。进水基质比例和pH值均会明显影响ANAMMOX脱氮效率。因而在两步式PN-ANAMMOX单元之间应设置基质比例和pH调整单元,将基质比例调节为1.25-1.35,而pH调节为7.0-7.5。
(5)以垃圾渗滤液原水为配水的低有机COD条件下,因渗滤液水质多变以及有机物的抑制作用,可使ANAMMOX脱氮效果波动,难以实现高效脱氮。而以PN单元的稀释出水作为进水时,则可实现高效高负荷脱氮和培养出红褐色的ANAMMOX颗粒污泥。在有机COD约为200mg/L的进水条件下,反应器仍能以高负荷稳定运行,最高脱氮负荷率达8.9kg N/m3/d,远高于同类其它研究的脱氮效果。其中pH、电导率和出水硝氮浓度仍可作为有机条件下ANAMMOX脱氮的指示参数,而电导率为最有效最精确的指示参数。
(6) PN-SBR与ANAMMOX-UASB的串联运行试验表明,通过动态调整终点pH值可使PN-SBR获得稳定的部分亚硝化效果,ANAMMOX-UASB处理100%的PN单元出水时可获得高效和高负荷脱氮。但由于受高进水pH抑制后,其脱氮效果波动较大,难以在100%的PN出水下以高负荷稳定地运行。随后ANAMMOX-UASB可在100%的PN出水下以低负荷稳定运行。PN-SBR活性污泥中的功能菌AOB较为多样,其中一个OTU与Nitrosomonas sp. IWT514相似度高达99%；另一OTU与Nitrosomonas eutropha(NR_027566)相似度为96%;还有两个OTU和Nitrosomonas eutropha (CP000450)相似度为96%。未检测出NOB,检出其它多种不可培养的微生物。PN-SBR的活性污泥中AOB只占总细菌的0.24%,还存在少量(0.04%)的AnAOB。 ANAMMOX-UASB颗粒污泥的主要脱氮功能菌为Kuenenia stuttgartiensis (CT573071)。ANAMMOX-UASB颗粒污泥中AnAOB占总细菌的8.34%,不存在NOB,存在少量(0.1%)的AOB。
(7)采用絮状AOB污泥和颗粒状AnAOB污泥作为CANON反应器的接种污泥,并于试验前45d在进水中添加少量亚硝氮,可实现CANON反应器的快速启动。随后逐步提高垃圾渗滤液在配水中的比例直至添加100%的垃圾渗滤液(C/N比为0.80-0.95),CANON反应器脱氮负荷也能稳步上升。至第101d,反应器的NRR达1.32kg N/m3/d,脱氮效率为81%。CANON活性污泥细菌中,AOB仅占总细菌的1%-3%,而AnAOB含量更低,低于0.3%,还存在其它多种多样的微生物。
Leachate generated from landfill contains high concentrations of ammonium and organic compounds, varies significantly in composition and flow rate, thus making its treatment energy-gobbling and highly expensive when using conventional nitrification and denitrification processes. Due to the high cost-effectiveness and efficiency, combined partial nitritation (PN)-anaerobic ammonium oxidation (ANAMMOX) process, is a promising alternative to conventional nitrification and denitrification for nitrogen removal from landfill leachate. However, the PN-ANAMMOX technology has not yet been fully investigated; there have still been some barriers remained to be solved. Both ammonia oxidation bacteria (AOB) and ANAMMOX bacteria (AnAOB) are slow growers, and are susceptible to the variation in wastewater compositions and operational conditions, thus resulting in a slow reactor startup and a difficult process control and a frequent instability in operation.
The overarching goal of this research was to solve the above issues:to investigate the fast startup, loading enhancement and process control of the PN and ANAMMOX units, to examine the rules of the process control on combining PN-ANAMMOX by means of two-stage and one-stage modes. The results are listed as follows.
(1) By using conventional fixed-time control in a sequencing batch reactor (SBR), partial nitritation of landfill leachate was achieved under both intermittent and continuous aeration modes. The adjustment of total air flux (TAF)/influent loading rate (ILR) ratio was observed to be effective to inhibiting nitrate formation. The effluent pH was found to be an indicator for effluent NO2--N/NH4+-N molar ratio. Due to more granules formed in the reactor operated under intermittent aeration mode, the nitrogen and COD removal performance were superior to those observed in continuous aeration mode.
(2) During the PN experiment in an SBR with a10times bigger volume (50L), combiantion of partial nitritation and denitrification was achieved by using flocculent activated sludge. Inhibition of nitrate formation can also be achieved by adjusting the TAF/ILR ratio; effluent pH was also observed as an effective indicator for effluent NO2--N/NH4+-N molar ratio. The analysis of the state in an SBR cycle showed that simultaneous nitrification and denitrification occurred in the first aeration stage.
(3) Endpoint pH control technique was used in the PN-SBR system for landfill leachate treatment by combination of partial nitritation and denitrification, resulting in a stable performance during long-term operation. Dynamically setting a suitable endpoint pH was the key to achieving optimal effluent NO2--N/NH4+-N molar ratio. Air flow rates at0.8,1.2and 1.6m3/h had unnoticeable effect on effluent NO2--N/NH4+-N molar ratio. Reaction temperatures at30℃,33℃and36℃had also unnoticeable effect on effluent NO2--N/NH4+-N molar ratio. Influent flow rate had no obvious effect on effluent NO2--N/NH4+-N molar ratio as well.
(4) By using the activated sludge in the PN-SBR and a small amount of ANAMMOX sludge from a UASB, fast startup of ANAMMOX reactor with NRR of6.2kg N/m3/d on day91was achieved. The pH, conductivity and effluent nitrate concentration can be the performance indicators of ANAMMOX reactor. Influent pH and NO2--N/NH4+-N molar ratio were found to significantly affect the ANAMMOX performance. Therefore, it is necessary to impose an equalization tank between the PN and ANAMMOX units for two-stage PN-ANAMMOX process. The optimal influent pH was7.0-7.5and NO2--N/NH4+-N molar ratio was1.25-1.35.
(5) The effect of organic compounds on AnAOB was investigated by adding raw landfill leachate as organic compounds in the ANAMMOX feed. The results showed that ANAMMOX performance was fluctuated and it was unable to achieve high rate nitrogen removal owing to the inhibition of organic compounds in the leachate. In contrast, it is successful to attain high rate nitrogen removal from the diluted PN-treated leachate, leading to development of reddish ANAMMOX granules. When the organic COD in the influent was around200mg/L, the NRR reached8.9kg N/m3/d, which is much higher than that reported in other related studies. Moreover, pH, conductivity and effluent nitrate can be used as indicators of performance of ANAMMOX reactor fed with diluted PN-treated leachate.
(6) Two-stage PN-SBR and ANAMMOX-UASB process was able to achieve efficient nitrogen removal from landfill leachate. Despite the significant variation in composition of landfill leachate, stable PN performance was witnessed in the PN-SBR using dynamic endpoint pH control technique. During the treatment of100%of PN-treated leachate in the ANAMMOX-UASB, high rate nitrogen removal can be achieved. Later on, after shock of high influent pH due to lack in reactor operation, the reactor performance is fluctuated and unstable during treatment of100%of PN effluent. Finally,85±1%of nitrogen removal and0.75±0.12kg N/m3/d of NRR were achieved when the ANAMMOX-UASB was operated under lower nitrogen load. Cloning analysis of the activated sludge in the PN-SBR indicated that one operational taxa unit (OTU) was99%related to the AOB species of Nitrosomonas sp. IWT514, one OTU was96%related to Nitrosomonas eutropha (NR_027566) and two OTUs were96%related to Nitrosomonas eutropha (CP000450). A variety of uncultured bacteria, however, no nitrobacter were found in the PN-SBR. AOB only accounted for0.24%of the total bacteria, surprisingly, AnAOB accounted for0.04%of the total bacteria, but no nitrobacter were found. The AnAOB in the ANAMMOX-UASB were highly related to Kuenenia stuttgartiensis (CT573071), and accounted for8.34%of total bacteria, while AOB accounted for0.1%of total bacteria, no nitrobacter were observed.
(7) By using floc-like AOB and granular AnAOB as seeds for the completely autotrophic nitrogen removal over nitrite (CANON) reactor, and adding a small amount of nitrite in the feed during the first45days, fast startup of CANON reactor was achieved. Proportion of addition of landfill leachate in the feed was then gradually increased till100%of raw leachate (C/N ratio of0.80-0.95); the nitrogen removal performance was stepwise improved. On day101, NRR reached1.32kg N/m3/d, and the nitrogen removal efficiency was81%. The qPCR analysis showed that AOB accounted for only1%-3%of the total bacteria in the CANON system, AnAOB accounted for a lower proportion (0.3%) of total bacteria. There were a variety of other bacteria in the CANON sludge, indicating the great bacterial diversity in the system.
为解决上述问题,本课题就PN-ANAMMOX技术在单级工艺的快速启动、负荷提高、工艺控制特点,串联运行的工艺衔接与控制规律及一步式耦合工艺的快速启动、工艺控制特性方面展开研究,取得如下成果。
(1)采用序批式反应器(Sequencing batch reactor, SBR)以常规的定时曝气方式运行,分别在间歇和连续曝气下实现了部分亚硝化联合反硝化对垃圾渗滤液进行脱氮除碳处理。在这两种运行方式中,通过调控总供气量(TAF)与进水负荷(ILR)的比值可有效抑制硝氮生成,出水pH可指示PN-SBR的出水NO2--N/NH4+-N摩尔比。间歇曝气运行方式由于形成的颗粒污泥数量较多,获得的脱氮除碳效果优于连续曝气运行方式的脱氮除碳效果。
(2)在PN-SBR絮状活性污泥系统中,也可实现部分亚硝化联合反硝化对垃圾渗滤液进行脱氮除碳处理。硝氮生成的抑制也可由调控TAF/ILR比值来实现,出水pH值也可指示出水NO2--N/NH4+-N摩尔比。SBR周期分析表明,反硝化在混合液中的脱氮除碳作用分别达28%和24%。同时硝化反硝化存在于SBR的第一个曝气阶段。
(3)采用终点pH控制法可在PN-SBR长期运行中稳定实现部分亚硝化联合反硝化处理垃圾渗滤液。曝气量在0.8、1.2和1.6m3/h时对出水NO2--N/NH4+-N摩尔比几无影响。反应温度在30℃、33℃和36℃时对出水NO2--N/NH4+-N摩尔比也几无影响。每周期进水量的改变也并不明显影响出水NO2--N/NH4+-N摩尔比。
(4)通过接种PN-SBR的活性污泥和少量低活性的ANAMMOX污泥,可快速启动ANAMMOX-UASB。pH、电导率和出水硝氮浓度可作为ANAMMOX脱氮效能的指示参数。进水基质比例和pH值均会明显影响ANAMMOX脱氮效率。因而在两步式PN-ANAMMOX单元之间应设置基质比例和pH调整单元,将基质比例调节为1.25-1.35,而pH调节为7.0-7.5。
(5)以垃圾渗滤液原水为配水的低有机COD条件下,因渗滤液水质多变以及有机物的抑制作用,可使ANAMMOX脱氮效果波动,难以实现高效脱氮。而以PN单元的稀释出水作为进水时,则可实现高效高负荷脱氮和培养出红褐色的ANAMMOX颗粒污泥。在有机COD约为200mg/L的进水条件下,反应器仍能以高负荷稳定运行,最高脱氮负荷率达8.9kg N/m3/d,远高于同类其它研究的脱氮效果。其中pH、电导率和出水硝氮浓度仍可作为有机条件下ANAMMOX脱氮的指示参数,而电导率为最有效最精确的指示参数。
(6) PN-SBR与ANAMMOX-UASB的串联运行试验表明,通过动态调整终点pH值可使PN-SBR获得稳定的部分亚硝化效果,ANAMMOX-UASB处理100%的PN单元出水时可获得高效和高负荷脱氮。但由于受高进水pH抑制后,其脱氮效果波动较大,难以在100%的PN出水下以高负荷稳定地运行。随后ANAMMOX-UASB可在100%的PN出水下以低负荷稳定运行。PN-SBR活性污泥中的功能菌AOB较为多样,其中一个OTU与Nitrosomonas sp. IWT514相似度高达99%；另一OTU与Nitrosomonas eutropha(NR_027566)相似度为96%;还有两个OTU和Nitrosomonas eutropha (CP000450)相似度为96%。未检测出NOB,检出其它多种不可培养的微生物。PN-SBR的活性污泥中AOB只占总细菌的0.24%,还存在少量(0.04%)的AnAOB。 ANAMMOX-UASB颗粒污泥的主要脱氮功能菌为Kuenenia stuttgartiensis (CT573071)。ANAMMOX-UASB颗粒污泥中AnAOB占总细菌的8.34%,不存在NOB,存在少量(0.1%)的AOB。
(7)采用絮状AOB污泥和颗粒状AnAOB污泥作为CANON反应器的接种污泥,并于试验前45d在进水中添加少量亚硝氮,可实现CANON反应器的快速启动。随后逐步提高垃圾渗滤液在配水中的比例直至添加100%的垃圾渗滤液(C/N比为0.80-0.95),CANON反应器脱氮负荷也能稳步上升。至第101d,反应器的NRR达1.32kg N/m3/d,脱氮效率为81%。CANON活性污泥细菌中,AOB仅占总细菌的1%-3%,而AnAOB含量更低,低于0.3%,还存在其它多种多样的微生物。
Leachate generated from landfill contains high concentrations of ammonium and organic compounds, varies significantly in composition and flow rate, thus making its treatment energy-gobbling and highly expensive when using conventional nitrification and denitrification processes. Due to the high cost-effectiveness and efficiency, combined partial nitritation (PN)-anaerobic ammonium oxidation (ANAMMOX) process, is a promising alternative to conventional nitrification and denitrification for nitrogen removal from landfill leachate. However, the PN-ANAMMOX technology has not yet been fully investigated; there have still been some barriers remained to be solved. Both ammonia oxidation bacteria (AOB) and ANAMMOX bacteria (AnAOB) are slow growers, and are susceptible to the variation in wastewater compositions and operational conditions, thus resulting in a slow reactor startup and a difficult process control and a frequent instability in operation.
The overarching goal of this research was to solve the above issues:to investigate the fast startup, loading enhancement and process control of the PN and ANAMMOX units, to examine the rules of the process control on combining PN-ANAMMOX by means of two-stage and one-stage modes. The results are listed as follows.
(1) By using conventional fixed-time control in a sequencing batch reactor (SBR), partial nitritation of landfill leachate was achieved under both intermittent and continuous aeration modes. The adjustment of total air flux (TAF)/influent loading rate (ILR) ratio was observed to be effective to inhibiting nitrate formation. The effluent pH was found to be an indicator for effluent NO2--N/NH4+-N molar ratio. Due to more granules formed in the reactor operated under intermittent aeration mode, the nitrogen and COD removal performance were superior to those observed in continuous aeration mode.
(2) During the PN experiment in an SBR with a10times bigger volume (50L), combiantion of partial nitritation and denitrification was achieved by using flocculent activated sludge. Inhibition of nitrate formation can also be achieved by adjusting the TAF/ILR ratio; effluent pH was also observed as an effective indicator for effluent NO2--N/NH4+-N molar ratio. The analysis of the state in an SBR cycle showed that simultaneous nitrification and denitrification occurred in the first aeration stage.
(3) Endpoint pH control technique was used in the PN-SBR system for landfill leachate treatment by combination of partial nitritation and denitrification, resulting in a stable performance during long-term operation. Dynamically setting a suitable endpoint pH was the key to achieving optimal effluent NO2--N/NH4+-N molar ratio. Air flow rates at0.8,1.2and 1.6m3/h had unnoticeable effect on effluent NO2--N/NH4+-N molar ratio. Reaction temperatures at30℃,33℃and36℃had also unnoticeable effect on effluent NO2--N/NH4+-N molar ratio. Influent flow rate had no obvious effect on effluent NO2--N/NH4+-N molar ratio as well.
(4) By using the activated sludge in the PN-SBR and a small amount of ANAMMOX sludge from a UASB, fast startup of ANAMMOX reactor with NRR of6.2kg N/m3/d on day91was achieved. The pH, conductivity and effluent nitrate concentration can be the performance indicators of ANAMMOX reactor. Influent pH and NO2--N/NH4+-N molar ratio were found to significantly affect the ANAMMOX performance. Therefore, it is necessary to impose an equalization tank between the PN and ANAMMOX units for two-stage PN-ANAMMOX process. The optimal influent pH was7.0-7.5and NO2--N/NH4+-N molar ratio was1.25-1.35.
(5) The effect of organic compounds on AnAOB was investigated by adding raw landfill leachate as organic compounds in the ANAMMOX feed. The results showed that ANAMMOX performance was fluctuated and it was unable to achieve high rate nitrogen removal owing to the inhibition of organic compounds in the leachate. In contrast, it is successful to attain high rate nitrogen removal from the diluted PN-treated leachate, leading to development of reddish ANAMMOX granules. When the organic COD in the influent was around200mg/L, the NRR reached8.9kg N/m3/d, which is much higher than that reported in other related studies. Moreover, pH, conductivity and effluent nitrate can be used as indicators of performance of ANAMMOX reactor fed with diluted PN-treated leachate.
(6) Two-stage PN-SBR and ANAMMOX-UASB process was able to achieve efficient nitrogen removal from landfill leachate. Despite the significant variation in composition of landfill leachate, stable PN performance was witnessed in the PN-SBR using dynamic endpoint pH control technique. During the treatment of100%of PN-treated leachate in the ANAMMOX-UASB, high rate nitrogen removal can be achieved. Later on, after shock of high influent pH due to lack in reactor operation, the reactor performance is fluctuated and unstable during treatment of100%of PN effluent. Finally,85±1%of nitrogen removal and0.75±0.12kg N/m3/d of NRR were achieved when the ANAMMOX-UASB was operated under lower nitrogen load. Cloning analysis of the activated sludge in the PN-SBR indicated that one operational taxa unit (OTU) was99%related to the AOB species of Nitrosomonas sp. IWT514, one OTU was96%related to Nitrosomonas eutropha (NR_027566) and two OTUs were96%related to Nitrosomonas eutropha (CP000450). A variety of uncultured bacteria, however, no nitrobacter were found in the PN-SBR. AOB only accounted for0.24%of the total bacteria, surprisingly, AnAOB accounted for0.04%of the total bacteria, but no nitrobacter were found. The AnAOB in the ANAMMOX-UASB were highly related to Kuenenia stuttgartiensis (CT573071), and accounted for8.34%of total bacteria, while AOB accounted for0.1%of total bacteria, no nitrobacter were observed.
(7) By using floc-like AOB and granular AnAOB as seeds for the completely autotrophic nitrogen removal over nitrite (CANON) reactor, and adding a small amount of nitrite in the feed during the first45days, fast startup of CANON reactor was achieved. Proportion of addition of landfill leachate in the feed was then gradually increased till100%of raw leachate (C/N ratio of0.80-0.95); the nitrogen removal performance was stepwise improved. On day101, NRR reached1.32kg N/m3/d, and the nitrogen removal efficiency was81%. The qPCR analysis showed that AOB accounted for only1%-3%of the total bacteria in the CANON system, AnAOB accounted for a lower proportion (0.3%) of total bacteria. There were a variety of other bacteria in the CANON sludge, indicating the great bacterial diversity in the system.
引文
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