高盐高碱环境下硝化反硝化过程及N_2O产生特征
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摘要
采用稳定运行在高盐高碱环境厌氧/好氧/缺氧(A_n/O/A)模式下的序批式生物膜反应器(SBBR),考察在不同碳氮比(C/N)条件下,硝化反硝化过程及N_2O产生特征.结果表明,在C/N为5、2和对照组(C/N=0)时,总氮去除率分别为(98. 17±0. 42)%、(65. 78±2. 47)%和(44. 08±0. 27)%; N_2O的产生量分别为(32. 07±2. 03)、(21. 81±0. 85)和(17. 32±0. 95) mg·L~(-1); N_2O转化率(N_2O产生量在去除总氮中的比例)分别为(29. 75±0. 93)%、(30. 04±2. 17)%和(41. 69±0. 80)%.高盐高碱条件下,亚硝酸盐氧化菌(NOB)受到很强的抑制作用,硝化过程基本停留在亚硝酸盐阶段.由于高盐高碱环境对N_2O还原酶活性的抑制,使得异养反硝化过程产生了大量N_2O,随着碳氮比的增大,有更多的碳源用于反硝化过程,因而总氮去除率和N_2O产生量均随之增加.随着碳氮比的增大,N_2O转化率随之降低,这可能是由于异养反硝化过程氮素还原酶对电子的竞争所形成的,碳氮比越高,电子竞争越弱.高通量测序表明:在SBBR中,氨氧化细菌(AOB)被富集,而几乎不存在NOB;优势异养反硝化菌属主要是Thauera、Azoarcus和Gemmobacter.
A sequencing biofilm batch reactor (SBBR) running continuously in an anaerobic/aerobic/anoxic( A_n/O/A) mode was adopted to study the characteristics of nitrification and denitrification process and nitrous oxide( N_2O) production under high saline and alkaline conditions. Different carbon and nitrogen ratios (C/N) were also investigated. An influent C/N ratio of 5,2,and 0( control),achieved the following results: TN removal efficiency was( 98. 17 ± 0. 42) %,( 65. 78 ± 2. 47) %,and( 44. 08 ±0. 27) %,respectively; total N_2O production was( 32. 07 ± 2. 03) mg·L~(-1),( 21. 81 ± 0. 85) mg·L~(-1),and( 17. 32 ± 0. 95) mg·L~(-1),respectively; and the N_2O conversion rate( i. e.,the ratio of total N_2O production to total nitrogen removal) was( 29. 75 ± 0. 93) %,( 30. 04 ± 2. 17) %,and( 41. 69 ± 0. 80) %,respectively. The nitrification process proceeded normally during the nitrite stage,and nitrite-oxidizing bacteria( NOB) were strongly inhibited under the high saline and alkaline conditions. Due to the inhibition of N_2O reductase under these conditions,N_2O production was higher during the heterotrophic denitrification process than during the ammonia oxidation process. With an increase in the carbon to nitrogen ratio,more carbon sources were available for denitrification meaning that the total nitrogen removal rate and N_2O production were both increased. As the ratio of carbon to nitrogen was increased,the N_2O conversion rate decreased,which may have been caused by electron competition among the nitrogen oxide reductases during the denitrification process; the higher the ratio of carbon to nitrogen,the weaker the electron competition. High-throughput sequencing indicated that ammonium-oxidizing bacteria( AOB) were enriched and NOB were almost entirely absent in the SBBR. Thauera,Azoarcus,and Gemmobacter were the dominant heterotrophic denitrifying bacteria identified in the system.
A sequencing biofilm batch reactor (SBBR) running continuously in an anaerobic/aerobic/anoxic( A_n/O/A) mode was adopted to study the characteristics of nitrification and denitrification process and nitrous oxide( N_2O) production under high saline and alkaline conditions. Different carbon and nitrogen ratios (C/N) were also investigated. An influent C/N ratio of 5,2,and 0( control),achieved the following results: TN removal efficiency was( 98. 17 ± 0. 42) %,( 65. 78 ± 2. 47) %,and( 44. 08 ±0. 27) %,respectively; total N_2O production was( 32. 07 ± 2. 03) mg·L~(-1),( 21. 81 ± 0. 85) mg·L~(-1),and( 17. 32 ± 0. 95) mg·L~(-1),respectively; and the N_2O conversion rate( i. e.,the ratio of total N_2O production to total nitrogen removal) was( 29. 75 ± 0. 93) %,( 30. 04 ± 2. 17) %,and( 41. 69 ± 0. 80) %,respectively. The nitrification process proceeded normally during the nitrite stage,and nitrite-oxidizing bacteria( NOB) were strongly inhibited under the high saline and alkaline conditions. Due to the inhibition of N_2O reductase under these conditions,N_2O production was higher during the heterotrophic denitrification process than during the ammonia oxidation process. With an increase in the carbon to nitrogen ratio,more carbon sources were available for denitrification meaning that the total nitrogen removal rate and N_2O production were both increased. As the ratio of carbon to nitrogen was increased,the N_2O conversion rate decreased,which may have been caused by electron competition among the nitrogen oxide reductases during the denitrification process; the higher the ratio of carbon to nitrogen,the weaker the electron competition. High-throughput sequencing indicated that ammonium-oxidizing bacteria( AOB) were enriched and NOB were almost entirely absent in the SBBR. Thauera,Azoarcus,and Gemmobacter were the dominant heterotrophic denitrifying bacteria identified in the system.
引文
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[16]王珊珊,梁红,高大文.盐度对好氧颗粒污泥硝化过程中N2O产生量的影响[J].环境科学,2014,35(11):4237-4243.Wang S S,Liang H,Gao D W.Effects of Salinity on N2Oproduction during nitrification using aerobic granular sludge[J].Environmental Science,2014,35(11):4237-4243.
[17]Zeng W,Li B X,Wang X D,et al.Integration of denitrifying phosphorus removal via nitrite pathway,simultaneous nitritationdenitritation and anammox treating carbon-limited municipal sewage[J].Bioresource Technology,2014,172:356-364.
[18]Rahimi Y,Torabian A,Mehrdadi N,et al.Simultaneous nitrification-denitrification and phosphorus removal in a fixed bed sequencing batch reactor(FBSBR)[J].Journal of Hazardous Materials,2011,185(2-3):852-857.
[19]Ma W W,Han Y X,Ma W C,et al.Enhanced nitrogen removal from coal gasification wastewater by simultaneous nitrification and denitrification(SND)in an oxygen-limited aeration sequencing batch biofilm reactor[J].Bioresource Technology,2017,244:84-91.
[20]Ge G H,Zhao J Q,Li X L,et al.Effects of influent COD/Nratios on nitrous oxide emission in a sequencing biofilm batch reactor for simultaneous nitrogen and phosphorus removal[J].Scientific Reports,2017,7(1):7417.
[21]葛光环.序批式生物膜反应器脱氮过程中N2O释放特征及其机理研究[D].西安:长安大学,2017.Ge G H.N2O emission characteristics and mechanisms during nitrogen removal in a sequencing batch biofilm reactor[D].Xi'an:Chang'an University,2017.
[22]Du R,Cao S B,Wang S Y,et al.Performance of partial denitrification(PD)-ANAMMOX process in simultaneously treating nitrate and low C/N domestic wastewater at low temperature[J].Bioresource Technology,2016,219:420-429.
[23]Gonzalez-Martinez A,Rodriguez-Sanchez A,Rodelas B,et al.454-pyrosequencing analysis of bacterial communities from autotrophic nitrogen removal bioreactors utilizing universal primers:effect of annealing temperature[J].BioMed Research International,2015,2015:892013.
[24]Hurek T,Handley L L,Reinhold-Hurek B,et al.Azoarcus grass endophytes contribute fixed nitrogen to the plant in an unculturable state[J].Molecular Plant-microbe Interactions:MPMI,2002,15(3):233-242.
[25]Zhao J G,Li Y H,Chen X R,et al.Effects of carbon sources on sludge performance and microbial community for 4-chlorophenol wastewater treatment in sequencing batch reactors[J].Bioresource Technology,2018,255:22-28.
[26]Liu J J,Yuan Y,Li B K,et al.Enhanced nitrogen and phosphorus removal from municipal wastewater in an anaerobicaerobic-anoxic sequencing batch reactor with sludge fermentation products as carbon source[J].Bioresource Technology,2017,244:1158-1165.
[2]Davidson E A.The contribution of manure and fertilizer nitrogen to atmospheric nitrous oxide since 1860[J].Nature Geoscience,2009,2(4):659-662.
[3]Ding X Q,Zhao J Q,Hu B,et al.Mathematical modeling of nitrous oxide production in an anaerobic/oxic/anoxic process[J].Bioresource Technology,2016,222:39-48.
[4]杨玉兵,杨庆,李洋,等.基于同位素技术的短程硝化过程N2O产生途径[J].环境科学,2018,39(11):5051-5057.Yang Y B,Yang Q,Li Y,et al.N2O Production pathways in partial nitrification based on isotope technology[J].Environmental Science,2018,39(11):5051-5057.
[5]Pan Y T,Ye L,Ni B J,et al.Effect of pH on N2O reduction and accumulation during denitrification by methanol utilizing denitrifiers[J].Water Research,2012,46(15):4832-4840.
[6]付昆明,王会芳,苏雪莹,等.初始p H值对序批式CANON工艺脱氮效果和N2O释放的影响[J].环境科学,2016,37(11):4261-4267.Fu K M,Wang H F,Su X Y,et al.Effect of initial pH on nitrogen removal performance and N2O emission of a sequencing batch CANON reactor[J].Environmental Science,2016,37(11):4261-4267.
[7]Reino C,van Loosdrecht M C M,Carrera J,et al.Effect of temperature on N2O emissions from a highly enriched nitrifying granular sludge performing partial nitritation of a low-strength wastewater[J].Chemosphere,2017,185:336-343.
[8]Peng L,Ni B J,Erler D,et al.The effect of dissolved oxygen on N2O production by ammonia-oxidizing bacteria in an enriched nitrifying sludge[J].Water Research,2014,66:12-21.
[9]Vendramel S,Dezotti M,Sant'Anna Jr G L.Nitrification of an industrial wastewater in a moving-bed biofilm reactor:effect of salt concentration[J].Environmental Technology,2011,32(8):837-846.
[10]Liu S T,Yang F L,Gong Z,et al.Assessment of the positive effect of salinity on the nitrogen removal performance and microbial composition during the start-up of CANON process[J].Applied Microbiology and Biotechnology,2008,80(2):339-348.
[11]She Z L,Zhao L T,Zhang X L,et al.Partial nitrification and denitrification in a sequencing batch reactor treating high-salinity wastewater[J].Chemical Engineering Journal,2016,288:207-215.
[12]邹高龙,李小明,李启武,等.盐度变化对SBBR和SBR中含氨氮废水的处理影响[J].环境科学,2009,30(9):2603-2608.Zou G L,Li X M,Li Q W,et al.Effects of salinity variation on the treatment wastewater containing ammonia in the SBBR and SBR[J].Environmental Science,2009,30(9):2603-2608.
[13]Wang J L,Gong B Z,Wang Y M,et al.The potential multiple mechanisms and microbial communities in simultaneous nitrification and denitrification process treating high carbon and nitrogen concentration saline wastewater[J].Bioresource Technology,2017,243:708-715.
[14]尚会来,彭永臻,张静蓉,等.盐度对污水硝化过程中N2O产量的影响[J].环境科学,2009,30(4):1079-1083.Shang H L,Peng Y Z,Zhang J R,et al.Effects of salinity concentration on N2O production during nitrification[J].Environmental Science,2009,30(4):1079-1083.
[15]刘甜甜,刘牡,王淑莹,等.盐度耦合FNA对短程反硝化过程中N2O还原的影响[J].中南大学学报(自然科学版),2013,44(8):3561-3568.Liu T T,Liu M,Wang S Y,et al.Impact of salinity coupling FNA on N2O reduction during denitrification via nitrite[J].Journal of Central South University(Science and Technology),2013,44(8):3561-3568.
[16]王珊珊,梁红,高大文.盐度对好氧颗粒污泥硝化过程中N2O产生量的影响[J].环境科学,2014,35(11):4237-4243.Wang S S,Liang H,Gao D W.Effects of Salinity on N2Oproduction during nitrification using aerobic granular sludge[J].Environmental Science,2014,35(11):4237-4243.
[17]Zeng W,Li B X,Wang X D,et al.Integration of denitrifying phosphorus removal via nitrite pathway,simultaneous nitritationdenitritation and anammox treating carbon-limited municipal sewage[J].Bioresource Technology,2014,172:356-364.
[18]Rahimi Y,Torabian A,Mehrdadi N,et al.Simultaneous nitrification-denitrification and phosphorus removal in a fixed bed sequencing batch reactor(FBSBR)[J].Journal of Hazardous Materials,2011,185(2-3):852-857.
[19]Ma W W,Han Y X,Ma W C,et al.Enhanced nitrogen removal from coal gasification wastewater by simultaneous nitrification and denitrification(SND)in an oxygen-limited aeration sequencing batch biofilm reactor[J].Bioresource Technology,2017,244:84-91.
[20]Ge G H,Zhao J Q,Li X L,et al.Effects of influent COD/Nratios on nitrous oxide emission in a sequencing biofilm batch reactor for simultaneous nitrogen and phosphorus removal[J].Scientific Reports,2017,7(1):7417.
[21]葛光环.序批式生物膜反应器脱氮过程中N2O释放特征及其机理研究[D].西安:长安大学,2017.Ge G H.N2O emission characteristics and mechanisms during nitrogen removal in a sequencing batch biofilm reactor[D].Xi'an:Chang'an University,2017.
[22]Du R,Cao S B,Wang S Y,et al.Performance of partial denitrification(PD)-ANAMMOX process in simultaneously treating nitrate and low C/N domestic wastewater at low temperature[J].Bioresource Technology,2016,219:420-429.
[23]Gonzalez-Martinez A,Rodriguez-Sanchez A,Rodelas B,et al.454-pyrosequencing analysis of bacterial communities from autotrophic nitrogen removal bioreactors utilizing universal primers:effect of annealing temperature[J].BioMed Research International,2015,2015:892013.
[24]Hurek T,Handley L L,Reinhold-Hurek B,et al.Azoarcus grass endophytes contribute fixed nitrogen to the plant in an unculturable state[J].Molecular Plant-microbe Interactions:MPMI,2002,15(3):233-242.
[25]Zhao J G,Li Y H,Chen X R,et al.Effects of carbon sources on sludge performance and microbial community for 4-chlorophenol wastewater treatment in sequencing batch reactors[J].Bioresource Technology,2018,255:22-28.
[26]Liu J J,Yuan Y,Li B K,et al.Enhanced nitrogen and phosphorus removal from municipal wastewater in an anaerobicaerobic-anoxic sequencing batch reactor with sludge fermentation products as carbon source[J].Bioresource Technology,2017,244:1158-1165.
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