脱氮硫杆菌利用FeS自养反硝化过程研究
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摘要
以硫化亚铁(FeS)为电子供体的自养反硝化反应对水体中硝酸盐的去除有重要贡献.以菌株Thiobacillus(T.)denitrificans ATCC 25259为对象,首次研究了脱氮硫杆菌以FeS为底物的自养反硝化过程.结果表明,以FeS作为唯一电子供体时,T.denitrificans可以将NO~-_3-N(30 mg·L~(-1))彻底还原为N_2.同时,FeS中的硫元素经自养反硝化过程转化为SO■,而铁元素与培养基中PO■反应生成沉淀物Fe_3(PO_4)_2·8H_2O.通过对相关数据拟合发现自养反硝化过程遵循零级反应动力学(R~2>0.93),随着FeS加入量的增大,NO~-_3和NO~-_2的还原速率均增大,但NO~-_3的还原速率增大更多,使中间产物NO~-_2的累积量增大.
The autotrophic denitrification reaction with ferrous sulfide(FeS) as the electron donor plays a significant role in nitrate removal in water body. The strain Thiobacillus(T.) denitrificans ATCC 25259 is novelly applied to investigate the process of autotrophic denitrification with FeS as substrate. The results exhibit that NO~-_3-N(30 mg·L~(-1)) is finally reduced to N_2 by T. denitrificans utilizing FeS as the sole electron donor. The elemental sulphur in FeS is converted to SO■ via autotrophic denitrification, whereas the elemental iron is precipitated with PO■ as the form of Fe_3(PO_4)_2·8 H_2O. Besides, according to the fitted curves, this autotrophic denitrification process is demonstrated to accord with the zero-order kinetics(R~2>0. 93). As the rising amount of FeS, both the reduction rates of NO~-_2 and NO~-_3 increase. Additionally, the reduction rate of NO~-_3 grows even more sharply, which accounts for the improved accumulation concentration of NO~-_2 as intermediates.
The autotrophic denitrification reaction with ferrous sulfide(FeS) as the electron donor plays a significant role in nitrate removal in water body. The strain Thiobacillus(T.) denitrificans ATCC 25259 is novelly applied to investigate the process of autotrophic denitrification with FeS as substrate. The results exhibit that NO~-_3-N(30 mg·L~(-1)) is finally reduced to N_2 by T. denitrificans utilizing FeS as the sole electron donor. The elemental sulphur in FeS is converted to SO■ via autotrophic denitrification, whereas the elemental iron is precipitated with PO■ as the form of Fe_3(PO_4)_2·8 H_2O. Besides, according to the fitted curves, this autotrophic denitrification process is demonstrated to accord with the zero-order kinetics(R~2>0. 93). As the rising amount of FeS, both the reduction rates of NO~-_2 and NO~-_3 increase. Additionally, the reduction rate of NO~-_3 grows even more sharply, which accounts for the improved accumulation concentration of NO~-_2 as intermediates.
引文
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[23] LI Ruihua,NIU Jianmin,ZHAN Xinmin,et al.Simultaneous removal of nitrogen and phosphorus from wastewater by means of FeS-based autotrophic denitrification [J].Water Science and Technology,2013,67(12):2761-2767.
[24] 周彦卿,郝瑞霞,刘思远,等.新型硫铁复合填料强化再生水深度脱氮除磷 [J].环境科学,2017,38(10):4309-4315.ZHOU Yanqing,HAO Ruixia,LIU Siyuan,et al.Improving nitrogen and phosphorus removal from reclaimed water using a novel sulfur/iron composite filler [J].Environmental Science,2017,38(10):4309-4315.(in Chinese)
[25] JANZEN M P,NICHOLSON R V,SCHARER J M.Pyrrhotite reaction kinetics:reaction rates for oxidation by oxygen,ferric iron,and for nonoxidative dissolution [J].Geochimica et Cosmochimica Acta,2000,64(9):1511-1522.
[26] DUINEA M I,COSTAS A,BAIBARAC M A.Mechanism of the cathodic process coupled to the oxidation of iron monosulfide by dissolved oxygen [J].Journal of Colloid and Interface Science,2016,467:51-59.
[27] VACLAVKOVA S,JORGENSEN C J,JACOBSEN O S,et al.The importance of microbial iron sulfide oxidation for nitrate depletion in anoxic Danish sediments [J].Aquatic Geochemistry,2014,20(4):419-435.
[28] GLASS C,SILVERSTEIN J.Denitrification kinetics of high nitrate concentration water:pH effect on inhibition and nitrite accumulation [J].Water Research,1998,32(3):831-839.
[29] MIOT J,MACLELLAN K,BENZERARA K,et al.Preservation of protein globules and peptidoglycan in the mineralized cell wall of nitrate-reducing,iron(II)-oxidizing bacteria:a cryo-electron microscopy study [J].Geobiology,2011,9(6):459-470.
[2] DI CAPUA F,PIROZZI F,LENS P N.Electron donors for autotrophic denitrification [J].Chemical Engineering Journal,2019,362:922-937.
[3] JORGENSEN C J,JACOBSEN O S,ELBERLING B,et al.Microbial oxidation of pyrite coupled to nitrate reduction in anoxic groundwater sediment [J].Environmental Science & Technology,2009,43(13):4851-4857.
[4] HAAIJER S M,LAMERS L M,SMOLDERS A P,et al.Iron sulfide and pyrite as potential electron donors for microbial nitrate reduction in freshwater wetlands [J].Geomicrobiology Journal,2007,24(5):391-401.
[5] CHOPPALA G,BUSH R,MOON E,et al.Oxidative transformation of iron monosulfides and pyrite in estuarine sediments:Implications for trace metals mobilisation [J].Journal of Environmental Management,2017,186(2,SI):158-166.
[6] SCHIPPERS A,JORGENSEN B B.Biogeochemistry of pyrite and iron sulfide oxidation in marine sediments [J].Geochimica et Cosmochimica Acta,2002,66(1):85-92.
[7] LI Ruihua,MORRISON L,COLLINS G,et al.Simultaneous nitrate and phosphate removal from wastewater lacking organic matter through microbial oxidation of pyrrhotite coupled to nitrate reduction [J].Water Research,2016,96:32-41.
[8] 付炳炳,潘建新,马景德,等.采用含硫铁化学污泥作为反硝化电子供体进行焦化废水中总氮深度去除 [J].环境科学,2018,39(7):3262-3270.FU Bingbing,PAN Jianxin,MA Jingde,et al.Evaluation of advanced nitrogen removal from coking wastewater using sulfide iron-containing sludge as a denitrification electron donor [J].Environmental Science,2018,39(7):3262-3270.(in Chinese)
[9] STRAUB K L,BENZ M,SCHINK B,et al.Anaerobic,nitrate-dependent microbial oxidation of ferrous iron [J].Applied and Environmental Microbiology,1996,62(4):1458-1460.
[10] TROUVE C,CHAZAL P M,GUEROUX B,et al.Denitrification by new strains of Thiobacillus denitrificans under non-standard physicochemical conditions.Effect of temperature,pH,and sulphur source [J].Environmental Technology,1998,19(6):601-610.
[11] HAAIJER S C,VAN DER WELLE M E,SCHMID M C,et al.Evidence for the involvement of betaproteobacterial Thiobacilli in the nitrate-dependent oxidation of iron sulfide minerals [J].FEMS Microbiology Ecology,2006,58(3):439-448.
[12] BELLER H R.Anaerobic,nitrate-dependent oxidation of U(IV) oxide minerals by the chemolithoautotrophic bacterium Thiobacillus denitrificans [J].Applied and Environmental Microbiology,2005,71(4):2170-2174.
[13] 国家环境保护总局.水和废水监测分析方法 [M].4版.北京:中国环境科学出版社,2002.State Environmental Protection Administration.Monitoring and Analysis Method of Water and Waster Water [M].4th ed.Beijing:China Environmental Science Press,2002.(in Chinese)
[14] BRADFORD M M.A rapid and sensitive method for the quantitation of microgram quantities of protein utilizing the principle of protein-dye binding [J].Analytical Biochemistry,1976,72(1/2):248-254.
[15] PAN Yuting,NI Bingjie,BOND P L,et al.Electron competition among nitrogen oxides reduction during methanol-utilizing denitrification in wastewater treatment [J].Water Research,2013,47(10):3273-3281.
[16] LU Huijie,CHANDRAN K,STENSEL D.Microbial ecology of denitrification in biological wastewater treatment [J].Water Research,2014,64:237-254.
[17] TORRENTO C,CAMA J,URMENETA J,et al.Denitrification of groundwater with pyrite and Thiobacillus denitrificans [J].Chemical Geology,2010,278(1/2):80-91.
[18] GORDON A D,SMIRNOV A,SHUMLAS S L,et al.Reduction of nitrite and nitrate on nano-dimensioned FeS [J].Origins of Life and Evolution of Biospheres,2013,43(4/5):305-322.
[19] RIVETT M O,BUSS S R,MORGAN P,et al.Nitrate attenuation in groundwater:A review of biogeochemical controlling processes [J].Water Research,2008,42(16):4215-4232.
[20] WANG A J,DU D Z,REN N Q,et al.An innovative process of simultaneous desulfurization and denitrification by Thiobacillus denitrificans [J].Journal of Environmental Science and Health.Part A,Toxic/Hazardous Substances & Environmental Engineering,2005,40(10):1939-1949.
[21] TONG Shuang,RODRIGUEZ-GONZALEZ L C,FENG C A.Comparison of particulate pyrite autotrophic denitrification (PPAD) and sulfur oxidizing denitrification (SOD) for treatment of nitrified wastewater [J].Water Science and Technology,2017,75(1):239-246.
[22] ZHANG Yongwei,WEI Dongyang,MORRISON L,et al.Nutrient removal through pyrrhotite autotrophic denitrification:Implications for eutrophication control [J].Science of the Total Environment,2019,662:287-296.
[23] LI Ruihua,NIU Jianmin,ZHAN Xinmin,et al.Simultaneous removal of nitrogen and phosphorus from wastewater by means of FeS-based autotrophic denitrification [J].Water Science and Technology,2013,67(12):2761-2767.
[24] 周彦卿,郝瑞霞,刘思远,等.新型硫铁复合填料强化再生水深度脱氮除磷 [J].环境科学,2017,38(10):4309-4315.ZHOU Yanqing,HAO Ruixia,LIU Siyuan,et al.Improving nitrogen and phosphorus removal from reclaimed water using a novel sulfur/iron composite filler [J].Environmental Science,2017,38(10):4309-4315.(in Chinese)
[25] JANZEN M P,NICHOLSON R V,SCHARER J M.Pyrrhotite reaction kinetics:reaction rates for oxidation by oxygen,ferric iron,and for nonoxidative dissolution [J].Geochimica et Cosmochimica Acta,2000,64(9):1511-1522.
[26] DUINEA M I,COSTAS A,BAIBARAC M A.Mechanism of the cathodic process coupled to the oxidation of iron monosulfide by dissolved oxygen [J].Journal of Colloid and Interface Science,2016,467:51-59.
[27] VACLAVKOVA S,JORGENSEN C J,JACOBSEN O S,et al.The importance of microbial iron sulfide oxidation for nitrate depletion in anoxic Danish sediments [J].Aquatic Geochemistry,2014,20(4):419-435.
[28] GLASS C,SILVERSTEIN J.Denitrification kinetics of high nitrate concentration water:pH effect on inhibition and nitrite accumulation [J].Water Research,1998,32(3):831-839.
[29] MIOT J,MACLELLAN K,BENZERARA K,et al.Preservation of protein globules and peptidoglycan in the mineralized cell wall of nitrate-reducing,iron(II)-oxidizing bacteria:a cryo-electron microscopy study [J].Geobiology,2011,9(6):459-470.
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