同步脱硫反硝化工艺运行效能及关键影响因素研究
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摘要
本研究基于具有反硝化功能的自养硫氧化细菌可在厌氧条件下利用硫化物为电子供体、硝酸盐为电子受体进行代谢活动同时胞外生成单质硫的生理特性,利用定向驯化的活性污泥启动厌氧固定床生物膜——同步脱硫反硝化反应器,从而创造一个自养硫氧化/反硝化菌和异养反硝化菌共存的混养生态系统,通过二者的协同作用,实现对硫化物、硝酸盐和乙酸盐的同时去除以及单质硫的积累。
通过在不同条件下的连续流运行,考察了混养条件下同步脱硫反硝化工艺的可行性,探讨了工艺运行的关键影响因素如pH值和硫氮比,并在此基础上确定了本工艺系统的最大处理负荷。结果表明:①混养条件下可获得了良好的硫化物、硝酸盐和乙酸盐的同步去除以及单质硫生成的效果,硫化物的毒性对系统中微生物没有明显的抑制作用;②混养条件下自养反硝化菌和异养反硝化菌是共生的关系。异养反硝化菌通过利用自养反硝化菌的代谢中间产物亚硝酸根,促进自养反硝化活动的进行,同时保证了工艺过程中单质硫的大量积累;③较低的偏碱性pH值条件有利于同步脱硫反硝化过程的进行,在较高的pH值条件下,单质硫产率较低;④硫氮比对工艺的运行效能影响显著,硫氮比为5/6时可获得最佳的硫化物去除和单质硫生成的效果;⑤工艺的最大处理负荷为2.4 kgS2-/m3d,该负荷条件下可获得100%的硫化物去除率和略高于2.4 kgS/m3d的理论单质硫产率。更高的负荷条件下,工艺的运行效能大幅度降低。结合试验结果,对同步脱硫反硝化过程的机理进行了探讨,并推导了该过程的反应计量式。
混养同步脱硫反硝化工艺比单独自养时具有更佳的去除硝酸根的能力,是废水处理中一项经济高效的厌氧生物新技术。
In this study, a laboratory-scale anaerobic fixed-bed bio-reactor was used to investigate the treatment performance and key factors of simultaneous de-sulfurization and de-nitrification process. Activated sludge was domesticated directionally to cultivate autotrophic sulfur-oxidizing/denitrifying bacterium, which are capable to oxidize sulfide to elemental sulfur when nitrate was adopted as electron acceptor under anaerobic or anoxic conditions and accumulate elemental sulfur extracellularly. Acetate was also added to incubate heterotrophic denitrificans. Thus, autotrophs and heterotrophs coexisted in the ecosystem, and cooperated to remove sulfide, nitrate and acetate simultaneously with elemental sulfur accumulation.
The feasibility of simultaneous desulfurization and denitrification under mixotrophic condition was investigated via continuous-flow tests. Then key factors of the process, including pH value and sulfide/nitrate (S/N) ratio, were discussed. Under the optimum pH value and S/N ratio conditions, the volume loading rates were elevated until the treatment performance declined. The experimental results suggest:①The simultaneous removal of sulfide, nitrate and acetate as well as elemental sulfur accumulation could be achieved under mixotrophic condition. It was shown that the toxicity of sulfide had little inhibition on the functional microorganisms in this system.②The relation between autotrophic sulfur-oxidizing/denitrifying bacteria and heterotrophic denitrifiers was symbiotic. The heterotrophs could accelerate the autotrophic denitrification by utilizing its intermediate products, namely nitrite, which also ensured the accumulation of elemental sulfur.③Lower alkalescent pH condition was favorable to the SDD process. The theoretical S0 production rate was much lower under higher pH conditions.④S/N ratio had a remarkable influence on the treatment performance. The optimum S/N ratio to acquire the best efficiencies of both sulfide removal and elemental sulfur accumulation was supposed to be 5/6.⑤Complete sulfide removal and a theoretical elemental sulfur production rate of 2.4 kgS/m3d were achieved at a volume loading rate of 2.4 kgS2-/m3d. At higher loading rates, the efficiency deteriorated sharply. Based on these results, the
通过在不同条件下的连续流运行,考察了混养条件下同步脱硫反硝化工艺的可行性,探讨了工艺运行的关键影响因素如pH值和硫氮比,并在此基础上确定了本工艺系统的最大处理负荷。结果表明:①混养条件下可获得了良好的硫化物、硝酸盐和乙酸盐的同步去除以及单质硫生成的效果,硫化物的毒性对系统中微生物没有明显的抑制作用;②混养条件下自养反硝化菌和异养反硝化菌是共生的关系。异养反硝化菌通过利用自养反硝化菌的代谢中间产物亚硝酸根,促进自养反硝化活动的进行,同时保证了工艺过程中单质硫的大量积累;③较低的偏碱性pH值条件有利于同步脱硫反硝化过程的进行,在较高的pH值条件下,单质硫产率较低;④硫氮比对工艺的运行效能影响显著,硫氮比为5/6时可获得最佳的硫化物去除和单质硫生成的效果;⑤工艺的最大处理负荷为2.4 kgS2-/m3d,该负荷条件下可获得100%的硫化物去除率和略高于2.4 kgS/m3d的理论单质硫产率。更高的负荷条件下,工艺的运行效能大幅度降低。结合试验结果,对同步脱硫反硝化过程的机理进行了探讨,并推导了该过程的反应计量式。
混养同步脱硫反硝化工艺比单独自养时具有更佳的去除硝酸根的能力,是废水处理中一项经济高效的厌氧生物新技术。
In this study, a laboratory-scale anaerobic fixed-bed bio-reactor was used to investigate the treatment performance and key factors of simultaneous de-sulfurization and de-nitrification process. Activated sludge was domesticated directionally to cultivate autotrophic sulfur-oxidizing/denitrifying bacterium, which are capable to oxidize sulfide to elemental sulfur when nitrate was adopted as electron acceptor under anaerobic or anoxic conditions and accumulate elemental sulfur extracellularly. Acetate was also added to incubate heterotrophic denitrificans. Thus, autotrophs and heterotrophs coexisted in the ecosystem, and cooperated to remove sulfide, nitrate and acetate simultaneously with elemental sulfur accumulation.
The feasibility of simultaneous desulfurization and denitrification under mixotrophic condition was investigated via continuous-flow tests. Then key factors of the process, including pH value and sulfide/nitrate (S/N) ratio, were discussed. Under the optimum pH value and S/N ratio conditions, the volume loading rates were elevated until the treatment performance declined. The experimental results suggest:①The simultaneous removal of sulfide, nitrate and acetate as well as elemental sulfur accumulation could be achieved under mixotrophic condition. It was shown that the toxicity of sulfide had little inhibition on the functional microorganisms in this system.②The relation between autotrophic sulfur-oxidizing/denitrifying bacteria and heterotrophic denitrifiers was symbiotic. The heterotrophs could accelerate the autotrophic denitrification by utilizing its intermediate products, namely nitrite, which also ensured the accumulation of elemental sulfur.③Lower alkalescent pH condition was favorable to the SDD process. The theoretical S0 production rate was much lower under higher pH conditions.④S/N ratio had a remarkable influence on the treatment performance. The optimum S/N ratio to acquire the best efficiencies of both sulfide removal and elemental sulfur accumulation was supposed to be 5/6.⑤Complete sulfide removal and a theoretical elemental sulfur production rate of 2.4 kgS/m3d were achieved at a volume loading rate of 2.4 kgS2-/m3d. At higher loading rates, the efficiency deteriorated sharply. Based on these results, the
引文
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9 I. W. Koster. Sulfide inhibition of the methanogenic activity of granular sludge at various pH-levels. Water Res.. 1986, 20(12): 1561～1567
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2 Peter Fox and Venkatraghavan Venkatasubbiah. Coupled Anaerobic/Aerobic Treatment of High-sulfate Wastewater with Sulfate Reduction and Biological Sulfide Oxidation. Wat. Sci. Tech, 1996, 34:359-366
3 F. Cadena and R. W. Peters. Evaluation of Chemical Oxidizer for Hydrogen Sulfide Control. JWPCF, 1988, 60:1259-1263
4 P. H. Nielson. Biofilm Dynamics and Kinetics during High-rate Sulfate Reduction under Anaerobic Conditions. Appl. Environ. Microbiol.. 1987, 53: 27～32
5 E. Chio, J. M. Rim. Competition and Inhibition of Sulfate Reducers and Methane Producers in Anaerobic Treatment. Wat. Sci. Technol.. 1991, 23: 1259～1264
6 J. R. Postgate. The Sulfate Reducing Bacteria. UK. Cambridge University Press, 1984
7 A. W. Khan, T. M. Trottier. Effect of Sulfur Containing Compounds on Anaerobic Degradation of Cellulose to Methane by Mixed Cultures Obtained from Sewage Sludge. Appl. Environ. Microbiol.. 1978, 35: 1027～1034
8 M. A. M. Reise. Effect of Hydrogen Sulfide on Growth of Sulfate Reducing Bacteria. Biotech. Bioeng.. 1992, 40(5): 593～600
9 I. W. Koster. Sulfide inhibition of the methanogenic activity of granular sludge at various pH-levels. Water Res.. 1986, 20(12): 1561～1567
10 杨景亮,左剑恶. 两相厌氧工艺处理硫酸盐有机废水的研究. 环境科学. 1995,6(3):8～11
11 李亚新,苏冰琴. 硫酸盐还原菌和酸矿废水生物处理技术. 环境污染控制技术. 2000,1(5): 1～11
12 任南琪,王爱杰. 硫化物氧化及新工艺. 哈尔滨工业大学学报. 2003,35(3):265～268
13 C. J. Buisman. Biotechnological Sulfide Removal in Three Polyurethane Carrier Reactors: Stirred Reactor, Bio-rotor Reactor and Up flow Reactor .Wat. Res.. 1990, 24 (2): 245-251.
14 G. C. Stefess and J. G. Kuenen. Factors Influencing Elemental Sulfur Production from Sulfide or Thiosulfate by Autotrophic Thiobacilli . Forum Microbiology. 1989, 12: 92
15 Lee, K. L. Sublette. A New Biotechnological Process for Sulfide Removal with Sulfur Production [A]. Proc. of the 5th International Symp. of Anaerobic Digestion, Bologna, Italy, 1988: 19-22
16 C. J. Buisman. Optimization of Sulfur Production in a Biotechnological Sulfide-Removing Reactor Biotech. Bioeng. 1990, 35:50-56
17 C. J. Buisman. Kinetics of Chemical and Biological Sulfide Oxidation in Aqueous Solutions . Wat. Res. 1990, 24 (5): 667-671
18 C. J. Buisman and G. Lettinga. Sulfide from Anaerobic Waste Treatment Effluent of a Papermill . Wat. Res.. 1990, 24 (3): 313-319
19 C. J. N. Buisman. Biotechnological Sulfide Removal from Effluent. Wat. Sci. Tech. 1991, 24(3/4): 347-356
20 P. F. Henshaw. Biotechnological Removal of Hydrogen Sulfide from Refinery Wastewater and Conversion to Elemental Sulfur. Wat. Sci.& Tech.. 1992, 25(3): 265-267
21 P. Dezham. Digester Gas H2S Control Using Iron Salts . JWPCF. 1998, 60 (4): 514-517
22 F. J. Millero. Oxidation of H2S in Seawater as a Function of Temperature, pH, and Ionic Strength. Environ. Sci. & Technol.. 1987, 21(5): 439-443
23 Jackson Yu. An Advanced Method of Hydrogen Sulfide Removal from Biogas. Anaerobic Treatment of Industrial Wastewater. 1990: 98-101
24 林巯安等. 用改进萘醌法脱除沼气中硫化氢的研究. 中国沼气. 1985, 12(1): 15～20
25 J. P. Maree and W. F. Strydom. Biological Sulfate Removal from Industrial Effluent in an Up flow Packed Bed Reactor. Wat. Res.. 1987, 21(2): 141-146
26 D. Y. Sorokin and A. M. Lysenko. Characterization of Heterotrophic Bacteria from the Black Sea Able To Oxidize Sulfur Compounds to Sulfate. Mikrobiologiya. 1993, 62: 1018–1031
27 D. Y. Sorokin, A. M. Lysenko and L. L. Mityushina. Isolation and Characterization of Alkaliphilic Chemoorganoheterotrophic BacteriaOxidizing Reduced Inorganic Sulfur Compounds to Tetrathionate. Mikrobiologiya. 1996, 65: 370–383
28 D. Y. Sorokin. Oxidation of Inorganic Sulfur Compounds by Obligately Organotrophic Bacteria. Microbiology. 2003, 72(6): 641～653
29 S. W. Effler, C. M. Brooks, M. T. Auer, S. M. Doerr. Free Ammonia and Toxicity Criteria in a Polluted Urban Lake. J Water Pollut Control Fed 1990, 62: 771–779
30 C. P. L. Grady Jr., H.C. Lim, Biological Wastewater Treatment: Theory and Applications, Marcel Dekker, New York, 1980
31 S. S. Cheng, W. C. Chen. Organic Carbon Supplement Influencing Performance of Biological Nitritification in a Fluidized Bed Reactor. Wat. Sci. Technol.. 1994, 30(11): 131–142
32 E. Van, P. Arts, B. J. Wesselink, L. A. Robertson, J. G. Kuenen. Competition Between Heterotrophic and Autotrophic Nitrifiers for Ammonia in Chemostat Cultures. FEMS Microbiol Ecol.. 1993, 102:109–118
33 K. Hanaki, C. Wantawin, S. Ohgaki. Effects of the Activity of Heterotrophs on Nitrification in a Suspended-growth Reactor. Water Res.. 1990, 24: 289–296
34 S. K. Gupta, S. M. Raja. Simultaneous Nitrification Denitrification in a Rotating Biological Contactor. Envir. Tech.. 1994, 15(3): 145-153
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