分段组合式厌氧生物反应器工作性能的研究
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摘要
全球面临能源紧缺与环境污染的双重压力,将厌氧消化技术用于有机废水处理,可同时实现污染治理与能源生产,在“节能减排”中发挥重大作用。厌氧反应器是厌氧消化技术的核心载体,高效厌氧反应器的研发有力推动了厌氧消化技术的发展。
分段组合式厌氧反应器(Compartmentalized Anaerobic Reactor, CAR)是本课题研发的新型厌氧反应器。本论文系统研究了该反应器的运行性能、纵向分布特性、预警性能、流态特性和抗生素类制药废水及其厌氧消化中间产物的急性毒性,主要成果如下：
(1)探明了分段组合式厌氧反应器的运行性能。
①分段组合式厌氧反应器具有较高的容积效能。容积负荷可达100.46gCOD·L-1·d-1,容积去除率可达84.35gCOD·L-1·d-1,容积产气率可达57.00L·L-1·d-1,效能指标处于国内外文献报道值的前列。
②分段组合式厌氧反应器具有较大的反应动力。高负荷运行时,反应器平均出水COD浓度和出水挥发性脂肪酸(VFA)浓度分别为2447mg·L-1和1638mg·L-1,它们是反应器常负荷运行时相应值的18.49倍与37.52倍,可提供较大的反应推动力。
③高负荷厌氧反应器的运行稳定性低于常负荷厌氧反应器。在常负荷工况下,进水COD浓度的提升(平均相对标准偏差为23.92%)基本上与出水COD浓度(平均相对标准偏差为24.57%)和出水VFA浓度(平均相对标准偏差为23.03%)的增大同步,而在高负荷工况下,进水COD浓度的小幅提升(平均相对标准偏差为8.08%)可引起出水COD浓度(平均相对标准偏差为32.95%)和出水VFA浓度(平均相对标准偏差为40.46%)的大幅增加。
(2)探明了分段组合式厌氧反应器纵向特性及预警性能。
①分段组合式厌氧反应器具有显著的容积效能纵向分布特征。在高负荷工况下,区段Ⅰ、Ⅱ、Ⅲ的平均容积负荷和平均容积效能依次为327.6gCOD·L-1·d-1、221.2gCOD-L-1·d-1、153.3gCOD·L-1·d-1和106.4gCOD·L-1·d-1、67.9gCOD·L-1·d-1、32.0gCOD·L-1·d-1。与常负荷工况相比,高负荷工况下容积效能的纵向分布特征弱化,有利于均衡基质负荷、挖掘各区段的反应潜能。
②分段组合式厌氧反应器具有显著的基质浓度纵向分布特征。在高负荷工况下,区段Ⅰ、Ⅱ、Ⅲ的平均VFA浓度、平均COD浓度及两者之比依次为1267.7mg·L-1、1006.1mg·L-1、922.9mg·L-1,2867.8mg·L-1、1988.1mg-L-1、1573.5mg·L-1和0.44、0.51、0.58。与常负荷工况相比,高负荷工况下容积效能的纵向VFA和COD浓度分布特征弱化,区段Ⅱ、Ⅲ和出水的平均VFA浓度以及平均VFA浓度与平均COD浓度之比增大,需重视VFA对厌氧消化(特别是产甲烷)反应的抑制作用。
③高效厌氧反应器的负荷饱和度和VFA饱和度具有预警性。容积负荷饱和度和VFA饱和度分别低于0.89与0.40时(即常负荷工况),反应运行性能稳定；容积负荷饱和度和VFA饱和度趋近1时(即满负荷工况),反应运行性能波动增大；容积负荷饱和度和VFA饱和度超过1时(即超负荷工况),反应运行性能恶化。
(3)探明了分段组合式厌氧反应器流态特性。
①容积负荷可显著影响CAR的流态。在常负荷下该反应器的返混程度较小,流态偏向平推流,以轴向扩散模型表征的Pe准数为7.94与5.66,以多釜串联模型表征的串联釜数为4.55与3.44；在高负荷与超高负荷下该反应器的返混程度较大,流态偏向全混流,以轴向扩散模型表征的Pe准数为4.02、2.57与3.93、3.77,以多釜串联模型表征的串联釜数为2.66、2.00与2.62、2.51。
②沼气分段排出可显著改善CAR的性状。CAR的总死区平均值为33.58%,其中污泥死区的平均值为20%,水力死区的平均值为13.58%。水力死区Vh(%)与水力负荷L(m3·m-3·d-1)和产气速率G(m3·m-3·d-1)之间的相关关系为：Vh=3.75L+0.19G-9.47(相关系数R2=0.953)。在CAR中,容积产气速率对水力死区的影响小于容积水力负荷。
③产气速率和进水速率显著影响CAR的效能。不产沼气工况下反应器的水力效率高于产沼气工况下反应器的水力效率。高负荷(进水速率较大)下反应器的水力效率低于常负荷(进水速率较小)下反应器的水力效率。CAR采用分段排气方式可有效遏制返混作用,弱化所产沼气对反应器水力效率的影响。
(4)探明了抗生素类制药废水及其厌氧消化中间产物的急性毒性。
①制药废水所含抗生素金霉素、多粘菌素、氯霉素对发光杆菌发光强度的半抑制浓度IC50分别为12.06、6.24和429.90mg·L-1,其毒性大小顺序为：多粘菌素>金霉素>氯霉素。厌氧消化中间产物乙醇、乙酸、丙酸和丁酸对发光杆菌发光强度的半抑制浓度IC50分别为19.40、20.71、10.47和12.17g·L-1,其毒性大小顺序为：丙酸>丁酸>乙醇>乙酸。
②厌氧消化中间产物(4元混合物)、多粘菌素-厌氧消化中间产物(5元混合物)、氯霉素-厌氧消化中间产物(5元混合物)的联合毒性R值分别为0.779、1.684、2.384,对发光细菌的联合毒性呈相加作用。金霉素-厌氧消化中间产物(5元混合物)、3种抗生素-厌氧消化中间产物(7元混合物)的联合毒性R值分别为3.005与3.827,其对发光细菌发光强度的联合毒性呈协同作用。
Energy shortage and environmental pollution are two major survival pressures in the world, and the application of anaerobic digestion technology to organic wastewater treatment can eliminate pollutants as well as produce bioenergy, which will play a great role in energy-saving and emission-reduction. Anaerobic reactor is the core of digestion technology, the research of high-rate anaerobic reactor have forcefully promoted the development of anaerobic digestion technology.
Compartmentalized Anaerobic Reactor (CAR) is a novel high-rate anaerobic reactor designed by our laboratory.In this paper, the performance, vertical distribution, early warning and flow patterns of CAR were investigated and the toxicity of pharmaceutical wastewater containing antibiotics and its anaerobic digestion intermediates was assayed.The main acchievements were as follows.
(1)Having revealed the working performance of CAR.
①CAR could reach a high volumetric efficiency.The organic loading rate, volumetric COD removal rate and volumetric biogas production were100.46gCOD·L-1·d-1,84.35gCOD·L-1·d-1and57.00L·L-1·d-1respectively.
②CAR could provide a greater driving force for the anaerobic digestion reaction. The average concentrations of COD and volatile fatty acids (VFA) in a high-rate CAR were2447mg·L-1and1638mg·L-1respectively, which were18.49and37.52times as high as their counterparts in a common-rate CAR.
③The performance stability of CAR at high loading rate was worse than that at common loading rate. At normal loading rate, the fluctuation of effluent COD concentration and volatile fatty acids (VFA) concentration was synchronous with that of influent COD concentration. The average relative standard deviation of effluent COD concentration and VFA concentration was24.57%and23.03%respectively,while that of influent COD concentration was23.92%, neverthesless, the fluctuation of effluent COD concentration and VFA concentration was large as compared with regard to that of influent COD concentration at high loading rate,. The average relative standard deviation of effluent COD concentration and VFA concentration was32.95%and40.46%respectively, while that of influent COD concentration was8.08%.
(2) Having shown the vertical distribution and early-warning characteristics of CAR
①CAR showed an obvious vertical distribution of volumetric efficiency, e.g. the organic loading rate and volumetric COD removal rate of partⅠ,Ⅱ and Ⅲ (bottom, middle and top) at the high loading rate were327.6gCOD·L-1·d-1,221.2gCOD·L-1·d-1,153.3gCOD·L-1·d-1and106.4gCOD·L-1·d-1,67.9gCOD·L-1·d-1,32.0gCOD·L-1·d-1respectively. Compared with that at common loading rates, the vertical distribution of volumetric efficiency at high loading rates became less obvious, which was helpful to homogenize the organic loading rate along the reactor and exploit reaction potential of the whole reactor.
②CAR also showed an obvious vertical distribution of substrate concentration. The average concentrations of VFA and COD as well as the values of VFA to COD were1267.7mg·L-1,1006.1mg·L-1,922.9mg·L-1;2867.8mg·L-1,1988.1mg·L-1,1573.5mg·L-1and0.44、0.51、0.58respectively。The vertical concentration gradient of VFA and COD was smaller at high loading rates, and the ratios of VFA to COD in part Ⅰ, Ⅱ,Ⅲ increased significantly. More attention should be paid to the serious inhibition caused by VFA at high loading rates.
③The saturation of volumetric loading rate (SVLR) and VFA (SVFA) could be used to alarm the performance of anaerobic reactors. The working performance was good when the CAR was operated at normal OLR, in which SVLR and SVFA were below0.89and0.4respectively. The fluctuation of performance became larger when the CAR was operated at OLR near saturation, in which SVLR and SVFA were close to 1. The performance of CAR was deteriorated when the SVLR and SVFA were more than1.
(3) Having revealed the hydraulic characteristics and their effects on working performance of CAR
①The flow pattern of CAR was significantly influenced by volumetric organic loading rate. The back-mixing at normal loading rate was small and the flow pattern tended to plug-flow,Pe numbers of the axial dispersion (AD) model under the condition with or without biogas production were5.66and7.94respectively, N numbers of the tanks-in-series(TIS) model under the condition with or without biogas production were3.44and4.55respectively. The back-mixing at high or super-high loading rate was large and the flow pattern tended to complexly mixed flow, Pe numbers of the AD model under the condition with or without biogas production were2.57,4.02and3.77,3.93respectively, N numbers of the TIS model under the condition with or without biogas production were2.00,2.66and2.51,2.62respectively.
②The hydraulic characteristics of CAR were ameliorated by discharging biogas individually out of each compartment. The average total dead space of CAR was33.58%, of which the average hydraulic dead space was13.58%. The regression equation (Vh=3.75L+0.19G-9.47) was established among the hydraulic dead space (Vh), the volumetric hydraulic loading rate (L) and the volumetric biogas production rate(G), the influence of G on Vh was less than L in CAR.
③The efficiencies of CAR were significantly influenced by volumetric hydraulic loading rate and volumetric biogas production rate. The reactor hydraulic efficiency under the condition without biogas production was better than that with biogas production, and the hydraulic efficiencies at high or super-high loading rate were lower than that at normal loading rate. The mode of discharging biogas from each compartment could alleviate the back-mixing, weaken the influence of biogas production on volumetric efficiency and improve the reactor performance.
(4) Having assayed the acute toxicity of pharmaceutical wastewater containing antibiotics and its anaerobic digestion intermediates.
①The15min-IC5o of aureomycin, polymyxin and chloromycetin were12.06,6.24and429.90mg·L-1, the toxicity descended in the order of polymyxin, aureomycin and chloromycetin. The15min-IC50of ethanol,acetate, propionate and butyrate were19.40,20.71,10.47and12.17g·L-1respectively, the toxicity descended in the order of propionate, butyrate, ethanol and acetate.
②The R values of anaerobic digestion intermediates (quad mixtures), intermediates together with polymyxin (penta mixtures), intermediates together with chloromycetin (penta mixtures) were0.779,1.684,2.384respectively, their joint effects were all additive. The R values of intermediates together with aureomycin (penta mixtures),intermediates together with three antibiotics (hepta mixtures) were3.005,3.827respectively, their joint effect were synergistic.
分段组合式厌氧反应器(Compartmentalized Anaerobic Reactor, CAR)是本课题研发的新型厌氧反应器。本论文系统研究了该反应器的运行性能、纵向分布特性、预警性能、流态特性和抗生素类制药废水及其厌氧消化中间产物的急性毒性,主要成果如下：
(1)探明了分段组合式厌氧反应器的运行性能。
①分段组合式厌氧反应器具有较高的容积效能。容积负荷可达100.46gCOD·L-1·d-1,容积去除率可达84.35gCOD·L-1·d-1,容积产气率可达57.00L·L-1·d-1,效能指标处于国内外文献报道值的前列。
②分段组合式厌氧反应器具有较大的反应动力。高负荷运行时,反应器平均出水COD浓度和出水挥发性脂肪酸(VFA)浓度分别为2447mg·L-1和1638mg·L-1,它们是反应器常负荷运行时相应值的18.49倍与37.52倍,可提供较大的反应推动力。
③高负荷厌氧反应器的运行稳定性低于常负荷厌氧反应器。在常负荷工况下,进水COD浓度的提升(平均相对标准偏差为23.92%)基本上与出水COD浓度(平均相对标准偏差为24.57%)和出水VFA浓度(平均相对标准偏差为23.03%)的增大同步,而在高负荷工况下,进水COD浓度的小幅提升(平均相对标准偏差为8.08%)可引起出水COD浓度(平均相对标准偏差为32.95%)和出水VFA浓度(平均相对标准偏差为40.46%)的大幅增加。
(2)探明了分段组合式厌氧反应器纵向特性及预警性能。
①分段组合式厌氧反应器具有显著的容积效能纵向分布特征。在高负荷工况下,区段Ⅰ、Ⅱ、Ⅲ的平均容积负荷和平均容积效能依次为327.6gCOD·L-1·d-1、221.2gCOD-L-1·d-1、153.3gCOD·L-1·d-1和106.4gCOD·L-1·d-1、67.9gCOD·L-1·d-1、32.0gCOD·L-1·d-1。与常负荷工况相比,高负荷工况下容积效能的纵向分布特征弱化,有利于均衡基质负荷、挖掘各区段的反应潜能。
②分段组合式厌氧反应器具有显著的基质浓度纵向分布特征。在高负荷工况下,区段Ⅰ、Ⅱ、Ⅲ的平均VFA浓度、平均COD浓度及两者之比依次为1267.7mg·L-1、1006.1mg·L-1、922.9mg·L-1,2867.8mg·L-1、1988.1mg-L-1、1573.5mg·L-1和0.44、0.51、0.58。与常负荷工况相比,高负荷工况下容积效能的纵向VFA和COD浓度分布特征弱化,区段Ⅱ、Ⅲ和出水的平均VFA浓度以及平均VFA浓度与平均COD浓度之比增大,需重视VFA对厌氧消化(特别是产甲烷)反应的抑制作用。
③高效厌氧反应器的负荷饱和度和VFA饱和度具有预警性。容积负荷饱和度和VFA饱和度分别低于0.89与0.40时(即常负荷工况),反应运行性能稳定；容积负荷饱和度和VFA饱和度趋近1时(即满负荷工况),反应运行性能波动增大；容积负荷饱和度和VFA饱和度超过1时(即超负荷工况),反应运行性能恶化。
(3)探明了分段组合式厌氧反应器流态特性。
①容积负荷可显著影响CAR的流态。在常负荷下该反应器的返混程度较小,流态偏向平推流,以轴向扩散模型表征的Pe准数为7.94与5.66,以多釜串联模型表征的串联釜数为4.55与3.44；在高负荷与超高负荷下该反应器的返混程度较大,流态偏向全混流,以轴向扩散模型表征的Pe准数为4.02、2.57与3.93、3.77,以多釜串联模型表征的串联釜数为2.66、2.00与2.62、2.51。
②沼气分段排出可显著改善CAR的性状。CAR的总死区平均值为33.58%,其中污泥死区的平均值为20%,水力死区的平均值为13.58%。水力死区Vh(%)与水力负荷L(m3·m-3·d-1)和产气速率G(m3·m-3·d-1)之间的相关关系为：Vh=3.75L+0.19G-9.47(相关系数R2=0.953)。在CAR中,容积产气速率对水力死区的影响小于容积水力负荷。
③产气速率和进水速率显著影响CAR的效能。不产沼气工况下反应器的水力效率高于产沼气工况下反应器的水力效率。高负荷(进水速率较大)下反应器的水力效率低于常负荷(进水速率较小)下反应器的水力效率。CAR采用分段排气方式可有效遏制返混作用,弱化所产沼气对反应器水力效率的影响。
(4)探明了抗生素类制药废水及其厌氧消化中间产物的急性毒性。
①制药废水所含抗生素金霉素、多粘菌素、氯霉素对发光杆菌发光强度的半抑制浓度IC50分别为12.06、6.24和429.90mg·L-1,其毒性大小顺序为：多粘菌素>金霉素>氯霉素。厌氧消化中间产物乙醇、乙酸、丙酸和丁酸对发光杆菌发光强度的半抑制浓度IC50分别为19.40、20.71、10.47和12.17g·L-1,其毒性大小顺序为：丙酸>丁酸>乙醇>乙酸。
②厌氧消化中间产物(4元混合物)、多粘菌素-厌氧消化中间产物(5元混合物)、氯霉素-厌氧消化中间产物(5元混合物)的联合毒性R值分别为0.779、1.684、2.384,对发光细菌的联合毒性呈相加作用。金霉素-厌氧消化中间产物(5元混合物)、3种抗生素-厌氧消化中间产物(7元混合物)的联合毒性R值分别为3.005与3.827,其对发光细菌发光强度的联合毒性呈协同作用。
Energy shortage and environmental pollution are two major survival pressures in the world, and the application of anaerobic digestion technology to organic wastewater treatment can eliminate pollutants as well as produce bioenergy, which will play a great role in energy-saving and emission-reduction. Anaerobic reactor is the core of digestion technology, the research of high-rate anaerobic reactor have forcefully promoted the development of anaerobic digestion technology.
Compartmentalized Anaerobic Reactor (CAR) is a novel high-rate anaerobic reactor designed by our laboratory.In this paper, the performance, vertical distribution, early warning and flow patterns of CAR were investigated and the toxicity of pharmaceutical wastewater containing antibiotics and its anaerobic digestion intermediates was assayed.The main acchievements were as follows.
(1)Having revealed the working performance of CAR.
①CAR could reach a high volumetric efficiency.The organic loading rate, volumetric COD removal rate and volumetric biogas production were100.46gCOD·L-1·d-1,84.35gCOD·L-1·d-1and57.00L·L-1·d-1respectively.
②CAR could provide a greater driving force for the anaerobic digestion reaction. The average concentrations of COD and volatile fatty acids (VFA) in a high-rate CAR were2447mg·L-1and1638mg·L-1respectively, which were18.49and37.52times as high as their counterparts in a common-rate CAR.
③The performance stability of CAR at high loading rate was worse than that at common loading rate. At normal loading rate, the fluctuation of effluent COD concentration and volatile fatty acids (VFA) concentration was synchronous with that of influent COD concentration. The average relative standard deviation of effluent COD concentration and VFA concentration was24.57%and23.03%respectively,while that of influent COD concentration was23.92%, neverthesless, the fluctuation of effluent COD concentration and VFA concentration was large as compared with regard to that of influent COD concentration at high loading rate,. The average relative standard deviation of effluent COD concentration and VFA concentration was32.95%and40.46%respectively, while that of influent COD concentration was8.08%.
(2) Having shown the vertical distribution and early-warning characteristics of CAR
①CAR showed an obvious vertical distribution of volumetric efficiency, e.g. the organic loading rate and volumetric COD removal rate of partⅠ,Ⅱ and Ⅲ (bottom, middle and top) at the high loading rate were327.6gCOD·L-1·d-1,221.2gCOD·L-1·d-1,153.3gCOD·L-1·d-1and106.4gCOD·L-1·d-1,67.9gCOD·L-1·d-1,32.0gCOD·L-1·d-1respectively. Compared with that at common loading rates, the vertical distribution of volumetric efficiency at high loading rates became less obvious, which was helpful to homogenize the organic loading rate along the reactor and exploit reaction potential of the whole reactor.
②CAR also showed an obvious vertical distribution of substrate concentration. The average concentrations of VFA and COD as well as the values of VFA to COD were1267.7mg·L-1,1006.1mg·L-1,922.9mg·L-1;2867.8mg·L-1,1988.1mg·L-1,1573.5mg·L-1and0.44、0.51、0.58respectively。The vertical concentration gradient of VFA and COD was smaller at high loading rates, and the ratios of VFA to COD in part Ⅰ, Ⅱ,Ⅲ increased significantly. More attention should be paid to the serious inhibition caused by VFA at high loading rates.
③The saturation of volumetric loading rate (SVLR) and VFA (SVFA) could be used to alarm the performance of anaerobic reactors. The working performance was good when the CAR was operated at normal OLR, in which SVLR and SVFA were below0.89and0.4respectively. The fluctuation of performance became larger when the CAR was operated at OLR near saturation, in which SVLR and SVFA were close to 1. The performance of CAR was deteriorated when the SVLR and SVFA were more than1.
(3) Having revealed the hydraulic characteristics and their effects on working performance of CAR
①The flow pattern of CAR was significantly influenced by volumetric organic loading rate. The back-mixing at normal loading rate was small and the flow pattern tended to plug-flow,Pe numbers of the axial dispersion (AD) model under the condition with or without biogas production were5.66and7.94respectively, N numbers of the tanks-in-series(TIS) model under the condition with or without biogas production were3.44and4.55respectively. The back-mixing at high or super-high loading rate was large and the flow pattern tended to complexly mixed flow, Pe numbers of the AD model under the condition with or without biogas production were2.57,4.02and3.77,3.93respectively, N numbers of the TIS model under the condition with or without biogas production were2.00,2.66and2.51,2.62respectively.
②The hydraulic characteristics of CAR were ameliorated by discharging biogas individually out of each compartment. The average total dead space of CAR was33.58%, of which the average hydraulic dead space was13.58%. The regression equation (Vh=3.75L+0.19G-9.47) was established among the hydraulic dead space (Vh), the volumetric hydraulic loading rate (L) and the volumetric biogas production rate(G), the influence of G on Vh was less than L in CAR.
③The efficiencies of CAR were significantly influenced by volumetric hydraulic loading rate and volumetric biogas production rate. The reactor hydraulic efficiency under the condition without biogas production was better than that with biogas production, and the hydraulic efficiencies at high or super-high loading rate were lower than that at normal loading rate. The mode of discharging biogas from each compartment could alleviate the back-mixing, weaken the influence of biogas production on volumetric efficiency and improve the reactor performance.
(4) Having assayed the acute toxicity of pharmaceutical wastewater containing antibiotics and its anaerobic digestion intermediates.
①The15min-IC5o of aureomycin, polymyxin and chloromycetin were12.06,6.24and429.90mg·L-1, the toxicity descended in the order of polymyxin, aureomycin and chloromycetin. The15min-IC50of ethanol,acetate, propionate and butyrate were19.40,20.71,10.47and12.17g·L-1respectively, the toxicity descended in the order of propionate, butyrate, ethanol and acetate.
②The R values of anaerobic digestion intermediates (quad mixtures), intermediates together with polymyxin (penta mixtures), intermediates together with chloromycetin (penta mixtures) were0.779,1.684,2.384respectively, their joint effects were all additive. The R values of intermediates together with aureomycin (penta mixtures),intermediates together with three antibiotics (hepta mixtures) were3.005,3.827respectively, their joint effect were synergistic.
引文
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