基于化学法控制的亚硝化与厌氧氨氧化的耦合工艺研究
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摘要
针对低碳氮比废水中有机质含量不能满足正常反硝化除氮所需碳源的情况,近年来出现了短程硝化反硝化(SND)和厌氧氨氧化(ANAMMOX)新工艺,已在污泥厌氧消化液、垃圾渗沥液、养殖废水和味精废水等高氨氮废水的脱氮处理中得到了广泛应用。实现短程反硝化和厌氧氨氧化过程成功的关键,首要的是控制氨氮亚硝化步骤。尽管国内外对氨氮亚硝化进行了大量而卓有成效的研究工作,也取得了一些积极成果,如控制废水的温度、pH、碱度、水力停留时间(HRT)和溶解氧(DO)等工艺参数,但因受水质和有机负荷的波动以及环境条件变化的影响,仍然存在着过程控制复杂、亚硝化不稳定、效率不高等问题。因此研究一种经济、简便、易行的控制亚硝化的手段,具有重要的理论意义和应用价值。
论文首先研究了化学试剂法培养好氧亚硝化颗粒污泥,实现同时短程硝化反硝化脱氮工艺。通过添加NOB选择性抑制剂(氯酸钾或羟胺)培养亚硝化颗粒污泥。在SBR反应器内,进水中的有机质大部分得到去除,从而降低或消除了有机质对厌氧氨氧化菌的抑制作用,有利于实现厌氧氨氧化和异养反硝化协同脱氮作用。然后通过亚硝化颗粒污泥与厌氧氨氧化耦合技术,对低浓度、低碳氮比废水处理进行了系统的实验室研究。
在MBBR中试装置中,通过添羟胺快速启动了短程硝化,结合其他控制参数(游离氨、游离亚硝酸、低污泥龄和中温等),能够很好的控制出水NO2--N/NH4+-N比例,并将消化液中少量可降解有机质去除,为ANAMMOX中试装置提供合适的进水水质。
利用无纺布生物转盘进行了厌氧氨氧化反应快速启动的中试实验,并利用短程硝化/厌氧氨氧化耦合工艺进行污泥厌氧消化液的处理。
论文取得了一些创新性的研究成果,主要包括以下几点：
(1)通过间歇性添加5mM氯酸钾能够实现硝化颗粒污泥短程硝化反硝化脱氮。在添加1～10mM氯酸钾条件下,均能实现系统的亚硝酸积累,NOB受到不同强度的抑制,AOB并未受到明显的抑制。荧光原位杂交结果显示亚硝化颗粒污泥主要由AOB组成,NOB数量远远低于AOB。长期实验结果显示,在温度和溶解氧未加控制的条件下,当进水pH、NH4+-N和COD分别为7.8-8.2、100mg/L和400mg/L时,间歇地添加氯酸钾能使SBR内快速出现NO2--N积累,其积累率达到93%,NH4+-N和COD的去除率也分别达到99%和79%。同时90%以上的的氯酸钾被分解为无毒的氯离子,不会给生态环境带来二次污染。
(2)通过间歇地投加羟胺能够快速启动颗粒污泥系统的短程硝化反硝化,三周即可完成短程硝化中试装置启动。在常温条件下,当进水NH4+-N和COD浓度分别为100mg/L和400mg/L,pH控制在8.0左右时,投加10mg/L羟胺后SBR中快速呈现NO2--N积累现象,NO2--N的平均积累率达到99.8%,TN和COD的去除率分别为57%和79%。SEM结果显示亚硝化颗粒污泥结构致密,主要由短杆菌和球菌组成,且表面有很多利于传质作用的微孔。FISH结果显示亚硝化颗粒污泥主要有AOB组成,而NOB的量远远低于AOB的量。
(3)厌氧氨氧化和亚硝酸盐型反硝化耦合过程中,异养反硝化菌优于厌氧氨氧化菌竞争NO2--N,厌氧氨氧化/异养反硝化协同作用关系主要受COD/NO2--N比例的制约,当C/N≤1.9,NO2--N/NH4+-N为2:1时,反应器以ANAMMOX反应为主,NO2--N、NH4+-N、 COD和TN的去除率分别达到96%、93%、87%和94%。
(4)在室温(18-25℃)、接种少量ANAMMOX污泥(100mg/L)和pH为7.0的情况下,能够快速启动无纺布生物转盘中试装置。经过90多天的运行,ANAMMOX中试装置处理负荷达到1kg N m-3d-1, ANAMMOX细菌生物膜由黄色逐渐变成红色,生物量增加了20多倍。利用HZO和16S rRNA基因分别进行PCR扩增并构建DNA克隆文库,结果显示ANAMMOX细菌主要由Candidatus Jettenia和Candidatus Brocadia组成。利用本装置处理污泥消化液,表明该工艺处理高氨氮废水具有可行性。
At present, some new biological nitrogen removal methods, such as simultaneous nitritation and denitritation and anaerobic ammonium oxidation (ANAMMOX) are invented according to the treatment of low C/N wastewaters, which could not be well treated by conventional nitrification and denitrification. Partial nitritation/ANAMMOX has been successfully applied to treat sludge digester liquid, landfill leachate, livestock wastewater and monosodium glutamate wastewater. The key of nitritation and ANAMMOX is to control ammonia oxidation to nitrite but not nitrate. Some control parameters of nitritation, such as medium temperature, pH, alkalinity, HRT and DO, have been successfully used to inhibit ammonia oxidation to nitrite. However, it is difficult to operate through these control parameters, and the nitritation system is seriously influenced by the water quality, organic loading and environmental conditions. Therefore, it is necessary to find an economical, simple, and easy method for the nitritation process, which has important theoretical significance and application value.
This article attempts to cultivate nitrosifying granules by chemical method, and simultaneous nitritation and denitritation adjusted by chemical reagent is successfully in the aerobic granular system. Aerobic nitrosifying granules are cultured by dosing NOB-selective inhibitors (chlorate and hydroxylamine). In the SBR, most of the organic matters could be removed, reducing or eliminating the inhibitory effect of organic matters on the ANAMMOX bacteria. Thus, ANAMMOX bacteria and denitrifiers can coupled well for treating of low COD contained wastewaters. Then, a lab-scale nitrosifying granules/ANAMMOX experiment is conducted for the treatment of low ammonia and low C/N wastewaters.
In the pilot-scale MBBR, partial nitritation is quickly established with hydroxylamine addition. Then the NOB inhibitor is not added into the MBBR, but nitritation could be well maintained using the other control parameters, such as FA, FNA, SRT and temperature, etc. Most of the biodegradable organics are removed and the effluent nitrite/ammonia ratio is also suitable for the ANAMMOX.
Moreover, quick start-up of ANAMMOX is studied in a pilot-scale no-woven RBC, and then it is applied to treat sludge digester liquid. Some innovative findings have been made as follows:
(1)Partial nitrification was successfully achieved with addition of5mM chlorate in the aerobic granular system. Chlorate with concentrations ranged from1mM to10mM is beneficial for the nitrite accumulation. This chemical inhibitor selectively inhibited NOB over AOB. FISH analysis revealed that AOB became the dominant nitrifying bacteria, whereas NOB was detected only in low abundance. During stable partial nitrification, the influent pH was kept at7.8-8.2, while the DO and temperature were not controlled in the SBR. When the NH4+-N and COD levels were kept at100mg/l and400mg/1in the influent, the NH4+-N and COD removal efficiencies reached99%and79%, respectively. The NO2--N accounted for93%of the NOx--N (NO2--N+NO3--N) in the effluent. Furthermore, about90%of the chlorate was reduced to nontoxic chloride, thus it would not cause environmental problem.
(2)Simultaneous nitritation and denitritation was successfully achieved by hydroxylamine dosing, and it just took3weeks to start up a pilot nitritation reactor. Nitrite accumulation was quickly detected after10mg/L hydroxylamine addition, treating synthetic wastewater containing100mg/1NH4+-N and400mg/1COD under conditions of room temperature ad pH7.8-8.2. TN removal efficiency was57%with a NO2--N/NO-X-N ratio of99.8%. Meanwhile,79%COD was removed by aerobic granules. SEM detection showed that the main composition of aerobic granules was coccus and bacilli bacteria. FISH results indicated that AOB were the dominant bacteria of aerobic granules.
(3)Heterotrophic denitrifying bacteria were competitive with ANAMMOX bacteria for the NO2--N in the simultaneous ANAMMOX and denitritation. When the COD/NO2--N decreased to1.9, and NO2--N/NH4+-N was2:1, NO2--N, NH4+-N, COD and TN removal efficiencies reached93%,96%,87%and94%, respectively. ANAMMOX was the main reaction.
(4)Results shows ANAMMOX reaction was quickly detected with little ANAMMOX seed sludge in the non-woven rotating biological contactor (NRBC), under the conditions of temperature18～25℃, pH7.0. During the first90days, the TN removal rate reached about1kg·N·m-3·d-1. The color of ANAMMOX biofilm changed from pale yellow to dark red, with a biomass improvement of20folds. Clone library analysis of HZO gene and16S rRNA showed that ANAMMOX bacteria in the pilot RBC were mainly composed of Candidatus Jettenia, Candidatus Brocadia. Then the NRBC was applied to treat digester liquid, and the results demonstrated that it had feasibility to remove nitrogen from high-ammonia wastewater by ANAMMOX.
论文首先研究了化学试剂法培养好氧亚硝化颗粒污泥,实现同时短程硝化反硝化脱氮工艺。通过添加NOB选择性抑制剂(氯酸钾或羟胺)培养亚硝化颗粒污泥。在SBR反应器内,进水中的有机质大部分得到去除,从而降低或消除了有机质对厌氧氨氧化菌的抑制作用,有利于实现厌氧氨氧化和异养反硝化协同脱氮作用。然后通过亚硝化颗粒污泥与厌氧氨氧化耦合技术,对低浓度、低碳氮比废水处理进行了系统的实验室研究。
在MBBR中试装置中,通过添羟胺快速启动了短程硝化,结合其他控制参数(游离氨、游离亚硝酸、低污泥龄和中温等),能够很好的控制出水NO2--N/NH4+-N比例,并将消化液中少量可降解有机质去除,为ANAMMOX中试装置提供合适的进水水质。
利用无纺布生物转盘进行了厌氧氨氧化反应快速启动的中试实验,并利用短程硝化/厌氧氨氧化耦合工艺进行污泥厌氧消化液的处理。
论文取得了一些创新性的研究成果,主要包括以下几点：
(1)通过间歇性添加5mM氯酸钾能够实现硝化颗粒污泥短程硝化反硝化脱氮。在添加1～10mM氯酸钾条件下,均能实现系统的亚硝酸积累,NOB受到不同强度的抑制,AOB并未受到明显的抑制。荧光原位杂交结果显示亚硝化颗粒污泥主要由AOB组成,NOB数量远远低于AOB。长期实验结果显示,在温度和溶解氧未加控制的条件下,当进水pH、NH4+-N和COD分别为7.8-8.2、100mg/L和400mg/L时,间歇地添加氯酸钾能使SBR内快速出现NO2--N积累,其积累率达到93%,NH4+-N和COD的去除率也分别达到99%和79%。同时90%以上的的氯酸钾被分解为无毒的氯离子,不会给生态环境带来二次污染。
(2)通过间歇地投加羟胺能够快速启动颗粒污泥系统的短程硝化反硝化,三周即可完成短程硝化中试装置启动。在常温条件下,当进水NH4+-N和COD浓度分别为100mg/L和400mg/L,pH控制在8.0左右时,投加10mg/L羟胺后SBR中快速呈现NO2--N积累现象,NO2--N的平均积累率达到99.8%,TN和COD的去除率分别为57%和79%。SEM结果显示亚硝化颗粒污泥结构致密,主要由短杆菌和球菌组成,且表面有很多利于传质作用的微孔。FISH结果显示亚硝化颗粒污泥主要有AOB组成,而NOB的量远远低于AOB的量。
(3)厌氧氨氧化和亚硝酸盐型反硝化耦合过程中,异养反硝化菌优于厌氧氨氧化菌竞争NO2--N,厌氧氨氧化/异养反硝化协同作用关系主要受COD/NO2--N比例的制约,当C/N≤1.9,NO2--N/NH4+-N为2:1时,反应器以ANAMMOX反应为主,NO2--N、NH4+-N、 COD和TN的去除率分别达到96%、93%、87%和94%。
(4)在室温(18-25℃)、接种少量ANAMMOX污泥(100mg/L)和pH为7.0的情况下,能够快速启动无纺布生物转盘中试装置。经过90多天的运行,ANAMMOX中试装置处理负荷达到1kg N m-3d-1, ANAMMOX细菌生物膜由黄色逐渐变成红色,生物量增加了20多倍。利用HZO和16S rRNA基因分别进行PCR扩增并构建DNA克隆文库,结果显示ANAMMOX细菌主要由Candidatus Jettenia和Candidatus Brocadia组成。利用本装置处理污泥消化液,表明该工艺处理高氨氮废水具有可行性。
At present, some new biological nitrogen removal methods, such as simultaneous nitritation and denitritation and anaerobic ammonium oxidation (ANAMMOX) are invented according to the treatment of low C/N wastewaters, which could not be well treated by conventional nitrification and denitrification. Partial nitritation/ANAMMOX has been successfully applied to treat sludge digester liquid, landfill leachate, livestock wastewater and monosodium glutamate wastewater. The key of nitritation and ANAMMOX is to control ammonia oxidation to nitrite but not nitrate. Some control parameters of nitritation, such as medium temperature, pH, alkalinity, HRT and DO, have been successfully used to inhibit ammonia oxidation to nitrite. However, it is difficult to operate through these control parameters, and the nitritation system is seriously influenced by the water quality, organic loading and environmental conditions. Therefore, it is necessary to find an economical, simple, and easy method for the nitritation process, which has important theoretical significance and application value.
This article attempts to cultivate nitrosifying granules by chemical method, and simultaneous nitritation and denitritation adjusted by chemical reagent is successfully in the aerobic granular system. Aerobic nitrosifying granules are cultured by dosing NOB-selective inhibitors (chlorate and hydroxylamine). In the SBR, most of the organic matters could be removed, reducing or eliminating the inhibitory effect of organic matters on the ANAMMOX bacteria. Thus, ANAMMOX bacteria and denitrifiers can coupled well for treating of low COD contained wastewaters. Then, a lab-scale nitrosifying granules/ANAMMOX experiment is conducted for the treatment of low ammonia and low C/N wastewaters.
In the pilot-scale MBBR, partial nitritation is quickly established with hydroxylamine addition. Then the NOB inhibitor is not added into the MBBR, but nitritation could be well maintained using the other control parameters, such as FA, FNA, SRT and temperature, etc. Most of the biodegradable organics are removed and the effluent nitrite/ammonia ratio is also suitable for the ANAMMOX.
Moreover, quick start-up of ANAMMOX is studied in a pilot-scale no-woven RBC, and then it is applied to treat sludge digester liquid. Some innovative findings have been made as follows:
(1)Partial nitrification was successfully achieved with addition of5mM chlorate in the aerobic granular system. Chlorate with concentrations ranged from1mM to10mM is beneficial for the nitrite accumulation. This chemical inhibitor selectively inhibited NOB over AOB. FISH analysis revealed that AOB became the dominant nitrifying bacteria, whereas NOB was detected only in low abundance. During stable partial nitrification, the influent pH was kept at7.8-8.2, while the DO and temperature were not controlled in the SBR. When the NH4+-N and COD levels were kept at100mg/l and400mg/1in the influent, the NH4+-N and COD removal efficiencies reached99%and79%, respectively. The NO2--N accounted for93%of the NOx--N (NO2--N+NO3--N) in the effluent. Furthermore, about90%of the chlorate was reduced to nontoxic chloride, thus it would not cause environmental problem.
(2)Simultaneous nitritation and denitritation was successfully achieved by hydroxylamine dosing, and it just took3weeks to start up a pilot nitritation reactor. Nitrite accumulation was quickly detected after10mg/L hydroxylamine addition, treating synthetic wastewater containing100mg/1NH4+-N and400mg/1COD under conditions of room temperature ad pH7.8-8.2. TN removal efficiency was57%with a NO2--N/NO-X-N ratio of99.8%. Meanwhile,79%COD was removed by aerobic granules. SEM detection showed that the main composition of aerobic granules was coccus and bacilli bacteria. FISH results indicated that AOB were the dominant bacteria of aerobic granules.
(3)Heterotrophic denitrifying bacteria were competitive with ANAMMOX bacteria for the NO2--N in the simultaneous ANAMMOX and denitritation. When the COD/NO2--N decreased to1.9, and NO2--N/NH4+-N was2:1, NO2--N, NH4+-N, COD and TN removal efficiencies reached93%,96%,87%and94%, respectively. ANAMMOX was the main reaction.
(4)Results shows ANAMMOX reaction was quickly detected with little ANAMMOX seed sludge in the non-woven rotating biological contactor (NRBC), under the conditions of temperature18～25℃, pH7.0. During the first90days, the TN removal rate reached about1kg·N·m-3·d-1. The color of ANAMMOX biofilm changed from pale yellow to dark red, with a biomass improvement of20folds. Clone library analysis of HZO gene and16S rRNA showed that ANAMMOX bacteria in the pilot RBC were mainly composed of Candidatus Jettenia, Candidatus Brocadia. Then the NRBC was applied to treat digester liquid, and the results demonstrated that it had feasibility to remove nitrogen from high-ammonia wastewater by ANAMMOX.
引文
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