利用双污泥反硝化除磷工艺降低污水处理过程中N_2O的产生
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摘要
近年来随着城市化和工业化进程的不断提高,低碳氮比(C/N)污水日益增多。然而,传统生物脱氮除磷工艺由于存在反硝化菌和聚磷菌对碳源竞争的问题,难以实现低C/N污水的达标处理。反硝化除磷作为一种新型脱氮除磷技术能“一碳两用”,可有效处理低C/N污水,达到高效脱氮除磷的目的。然而,反硝化除磷过程可产生大量温室气体N20,因此研究其N20的产生机理和控制方法,为推广反硝化除磷工艺的应用具有重要意义。
本论文构建了双污泥反硝化除磷系统,研究了其处理低C/N城市污水过程中N20的产生特征,明确了系统中N20的主要产生阶段；探讨了双污泥系统曝气硝化阶段以及缺氧反硝化除磷阶段N20产生的机理和影响因素,确定了曝气和缺氧阶段的最佳运行条件；提出了双污泥系统处理低C/N城市污水过程中N20产生的减量化控制措施,并对减排效果进行了评价。主要研究内容及结果如下：
(1)阐明了双污泥系统中氮、磷的去除效果和N2O的产生特征。双污泥系统对低C/N城市污水具有较高的处理效果,总氮和总磷的去除效率高达92.13%和95.18%。双污泥处理低C/N城市污水过程中有大量N20的产生,每周期N20产生量占总氮去除的比例高达1.47%；其中曝气阶段、缺氧反硝化除磷阶段以及后曝气阶段N20产生量占总氮去除的比例分别为0.86%、0.41%以及0.20%。
(2)明确了双污泥系统曝气硝化过程中N2O产生的来源,确定了曝气硝化阶段的最佳DO浓度。双污泥系统曝气阶段N2O产生主要来源于自养菌的硝化作用,其对N2O产生的贡献率高达97.1%,而异养菌的反硝化作用对N20的产生几乎没有贡献。DO浓度对曝气阶段N20的产生具有重要的影响,当DO浓度为2.5mg/L时,N20的产生量最低,其周期产生量只有0.20mg/L。
(3)揭示了双污泥系统缺氧反硝化除磷过程中N20产生的机理,确定了可减少缺氧反硝化除磷阶段N20产生的运行方式。反硝化除磷过程中N20产生的主要原因是,反硝化聚磷菌以胞内聚合物(PHA)为碳源进行反硝化,导致反硝化酶对电子形成竞争,使氧化亚氮还原酶无法获得足够的电子将N20还原,并引起亚硝酸盐的积累。连续的硝酸盐投加方式、以丙酸为碳源,均可明显减少反硝化除磷过程中亚硝酸盐的积累,降低N20的产生。
(4)研究了碳源类型对反硝化除磷过程N20产生的影响机制,揭示了以丙酸为碳源时反硝化除磷过程N20产生量低的原因。碳源类型明显影响了反硝化除磷过程中N20的产生,以乙酸为碳源时,N20的产生量最高,占总氮去除的16.32%；而以混合酸(乙酸和丙酸)和丙酸为碳源时,N20的产生量仅占总氮去除的1.92%和0.43%。丙酸系统N20产生量低的主要原因是,以丙酸为单一碳源,反硝化除磷系统中不存在反硝化酶对电子的竞争作用,亚硝酸盐和氧化亚氮还原酶的活性不会受到抑制,不会导致亚硝酸盐的积累。
(5)建立了可有效提高氮磷去除效果、降低N20产生的双污泥系统及其优化控制方案。控制曝气阶段DO条件以及采用丙酸作为碳源,能有效降低双污泥系统N20的产生,并可实现氮磷的高效去除。构建的双污泥系统出水中的总氮和总磷浓度分别只有3.16mg/L和0.39mg/L,去除率都达到90%以上；其N20产生量只占总氮去除的0.75%,远低于常规污水处理工艺(1.72%)和文献中报告的其他工艺的产生量。
In recent years, with the improvement of urbanization and industrialization, wastewater with low C/N ratio is increasing. However, due to both denitrifiers and phosphate accumulating orgasims (PAOs) require carbon source, the effluent could not reach the discharge standards when conventional biological nutrient removal (BNR) was used to treat the wastewater with low C/N ratio. Denitrifying phosphorus removal which could remove nitrogen and phosphorus simultaneously using the same carbon source is a new prominent biological wastewater treatment technique, and it is particularly suitable for treating low COD/N wastewater. However, several studies have reported that denitrifying phosphorus removal process could produce a lot of nitrous oxide (N2O). Therefore, effective control of N2O emission from denitrifying phosphorus removal process is of great importance and attracts increasingly more attention.
In this study, the denitrifying phosphorus removal was achieved in a two-sludge system which was used to treat municipal sewage with low C/N ratio, and the N2O production characteristics during this system were systemically studied, and the main N2O production phase was clear; the mechanism and influence factors of N2O production during the aerobic nitrification stage and anoxic denitrifying phosphorus removal stage in two-sludge system was investigated, and the best operating conditions during aerobic and anoxic stages was clear; feasible N2O reduction strategies in two-sludge system were proposed, and the reduction effects of the proposed strategies were evaluated. The main research conclusions are as follows:
(1) The nitrogen and phosphorous removal rates and N2O production characteristics in two-sludge system was clear. It was found that the TN and TP removal rates in two-sludge system reached92.13%and95.18%respectively. A lot of N2O was produced in two-sludge system, N2O production during one cycle accounted for1.47%of the total nitrogen removal, and the production amounts during aerobic, anoxic and post-aerobic stages were0.86%,0.41%and0.20%of the TN removal.
(2) The sources of N2O production and the best DO concentrations in aerobic stage of two-sludge system were clear. Autotrophic nitrification which accounted for97.1%of the N2O production was the main source due to no heterotrophic denitrification occurred in aerobic stage of two-sludge system. DO concentrations significantly affected N2O production in aerobic stage. When DO concentration was2.5mg/L, the N2O production was lowest, and the amount during one cycle was only0.20mg/L.
(3) The mechanism of N2O production and the best operating conditions which could decrease N2O production during anoxic denitrifying phosphorus removal stage were clear. The main reason for N2O production during denitrifying phosphorus removal process was that denitrifying phosphorous accumulating organisms DPAOs used poly-β-hydroxyalkanoates (PHA) as carbon source for denitrification, and the limited electrons provided by PHA could not satisfy the requirement of denitrifying enzymes, and this resulted high nitrite accumulation. Accordingly, the reduction of N2O production was successfully achieved via two control measures:the use of continuous nitrate addition and the use of propionate as the carbon source.
(4) The mechanisms of carbon sources affected N2O production during denitrifying phosphorous removal process were studied, and the causes of low N2O production when using propionate as carbon source was clear. Carbon sources significantly affected N2O production during denitrifying phosphorous removal process. When using acetate as the sole carbon source, the N2O production amount was up to16.3%of the TN removal; whereas, when using the mixture of acetate and propionate or propionate as carbon source, the N2O production amount were1.92%and0.43%of the TN removal. The main reason for nearly no N2O production in propionate system was that:when using propionate as the sole carbon source, the electrons provided by PHA could satisfy the requirement of denitrifying enzymes, and the nitrite and N2O reductase activities were not inhibited, as a result, no nitrite was accumulated.
(5) The two-sludge system and optimization strategies which could improve nitrogen and phosphorous removal ratio and decrease N2O production were established. When using propionate as the sole carbon source and the DO concentrations were controlled at2.5mg/L, not only low N2O production but also high nitrogen and phosphorous removal were achieved in two-sludge system. The TN and TP concentrations in effluent were only3.16and0.39mg/L, respectively. N2O production amount during one cycle was only0.75%of TN removal, which was much lower than the conventional wastewater treatment (1.72%) and other processes reported in the literatures.
本论文构建了双污泥反硝化除磷系统,研究了其处理低C/N城市污水过程中N20的产生特征,明确了系统中N20的主要产生阶段；探讨了双污泥系统曝气硝化阶段以及缺氧反硝化除磷阶段N20产生的机理和影响因素,确定了曝气和缺氧阶段的最佳运行条件；提出了双污泥系统处理低C/N城市污水过程中N20产生的减量化控制措施,并对减排效果进行了评价。主要研究内容及结果如下：
(1)阐明了双污泥系统中氮、磷的去除效果和N2O的产生特征。双污泥系统对低C/N城市污水具有较高的处理效果,总氮和总磷的去除效率高达92.13%和95.18%。双污泥处理低C/N城市污水过程中有大量N20的产生,每周期N20产生量占总氮去除的比例高达1.47%；其中曝气阶段、缺氧反硝化除磷阶段以及后曝气阶段N20产生量占总氮去除的比例分别为0.86%、0.41%以及0.20%。
(2)明确了双污泥系统曝气硝化过程中N2O产生的来源,确定了曝气硝化阶段的最佳DO浓度。双污泥系统曝气阶段N2O产生主要来源于自养菌的硝化作用,其对N2O产生的贡献率高达97.1%,而异养菌的反硝化作用对N20的产生几乎没有贡献。DO浓度对曝气阶段N20的产生具有重要的影响,当DO浓度为2.5mg/L时,N20的产生量最低,其周期产生量只有0.20mg/L。
(3)揭示了双污泥系统缺氧反硝化除磷过程中N20产生的机理,确定了可减少缺氧反硝化除磷阶段N20产生的运行方式。反硝化除磷过程中N20产生的主要原因是,反硝化聚磷菌以胞内聚合物(PHA)为碳源进行反硝化,导致反硝化酶对电子形成竞争,使氧化亚氮还原酶无法获得足够的电子将N20还原,并引起亚硝酸盐的积累。连续的硝酸盐投加方式、以丙酸为碳源,均可明显减少反硝化除磷过程中亚硝酸盐的积累,降低N20的产生。
(4)研究了碳源类型对反硝化除磷过程N20产生的影响机制,揭示了以丙酸为碳源时反硝化除磷过程N20产生量低的原因。碳源类型明显影响了反硝化除磷过程中N20的产生,以乙酸为碳源时,N20的产生量最高,占总氮去除的16.32%；而以混合酸(乙酸和丙酸)和丙酸为碳源时,N20的产生量仅占总氮去除的1.92%和0.43%。丙酸系统N20产生量低的主要原因是,以丙酸为单一碳源,反硝化除磷系统中不存在反硝化酶对电子的竞争作用,亚硝酸盐和氧化亚氮还原酶的活性不会受到抑制,不会导致亚硝酸盐的积累。
(5)建立了可有效提高氮磷去除效果、降低N20产生的双污泥系统及其优化控制方案。控制曝气阶段DO条件以及采用丙酸作为碳源,能有效降低双污泥系统N20的产生,并可实现氮磷的高效去除。构建的双污泥系统出水中的总氮和总磷浓度分别只有3.16mg/L和0.39mg/L,去除率都达到90%以上；其N20产生量只占总氮去除的0.75%,远低于常规污水处理工艺(1.72%)和文献中报告的其他工艺的产生量。
In recent years, with the improvement of urbanization and industrialization, wastewater with low C/N ratio is increasing. However, due to both denitrifiers and phosphate accumulating orgasims (PAOs) require carbon source, the effluent could not reach the discharge standards when conventional biological nutrient removal (BNR) was used to treat the wastewater with low C/N ratio. Denitrifying phosphorus removal which could remove nitrogen and phosphorus simultaneously using the same carbon source is a new prominent biological wastewater treatment technique, and it is particularly suitable for treating low COD/N wastewater. However, several studies have reported that denitrifying phosphorus removal process could produce a lot of nitrous oxide (N2O). Therefore, effective control of N2O emission from denitrifying phosphorus removal process is of great importance and attracts increasingly more attention.
In this study, the denitrifying phosphorus removal was achieved in a two-sludge system which was used to treat municipal sewage with low C/N ratio, and the N2O production characteristics during this system were systemically studied, and the main N2O production phase was clear; the mechanism and influence factors of N2O production during the aerobic nitrification stage and anoxic denitrifying phosphorus removal stage in two-sludge system was investigated, and the best operating conditions during aerobic and anoxic stages was clear; feasible N2O reduction strategies in two-sludge system were proposed, and the reduction effects of the proposed strategies were evaluated. The main research conclusions are as follows:
(1) The nitrogen and phosphorous removal rates and N2O production characteristics in two-sludge system was clear. It was found that the TN and TP removal rates in two-sludge system reached92.13%and95.18%respectively. A lot of N2O was produced in two-sludge system, N2O production during one cycle accounted for1.47%of the total nitrogen removal, and the production amounts during aerobic, anoxic and post-aerobic stages were0.86%,0.41%and0.20%of the TN removal.
(2) The sources of N2O production and the best DO concentrations in aerobic stage of two-sludge system were clear. Autotrophic nitrification which accounted for97.1%of the N2O production was the main source due to no heterotrophic denitrification occurred in aerobic stage of two-sludge system. DO concentrations significantly affected N2O production in aerobic stage. When DO concentration was2.5mg/L, the N2O production was lowest, and the amount during one cycle was only0.20mg/L.
(3) The mechanism of N2O production and the best operating conditions which could decrease N2O production during anoxic denitrifying phosphorus removal stage were clear. The main reason for N2O production during denitrifying phosphorus removal process was that denitrifying phosphorous accumulating organisms DPAOs used poly-β-hydroxyalkanoates (PHA) as carbon source for denitrification, and the limited electrons provided by PHA could not satisfy the requirement of denitrifying enzymes, and this resulted high nitrite accumulation. Accordingly, the reduction of N2O production was successfully achieved via two control measures:the use of continuous nitrate addition and the use of propionate as the carbon source.
(4) The mechanisms of carbon sources affected N2O production during denitrifying phosphorous removal process were studied, and the causes of low N2O production when using propionate as carbon source was clear. Carbon sources significantly affected N2O production during denitrifying phosphorous removal process. When using acetate as the sole carbon source, the N2O production amount was up to16.3%of the TN removal; whereas, when using the mixture of acetate and propionate or propionate as carbon source, the N2O production amount were1.92%and0.43%of the TN removal. The main reason for nearly no N2O production in propionate system was that:when using propionate as the sole carbon source, the electrons provided by PHA could satisfy the requirement of denitrifying enzymes, and the nitrite and N2O reductase activities were not inhibited, as a result, no nitrite was accumulated.
(5) The two-sludge system and optimization strategies which could improve nitrogen and phosphorous removal ratio and decrease N2O production were established. When using propionate as the sole carbon source and the DO concentrations were controlled at2.5mg/L, not only low N2O production but also high nitrogen and phosphorous removal were achieved in two-sludge system. The TN and TP concentrations in effluent were only3.16and0.39mg/L, respectively. N2O production amount during one cycle was only0.75%of TN removal, which was much lower than the conventional wastewater treatment (1.72%) and other processes reported in the literatures.
引文
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