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Isotope Signatures of N_2O in a Mixed Microbial Population System: Constraints on N_2O Producing Pathways in Wastewater Treatment

机译:混合微生物种群系统中N_2O的同位素特征:废水处理中N_2O产生途径的限制

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摘要

We present measurements of site preference (SP) and bulk ~(15)N/~(14)N ratios (δ~(15)N~(bulk)_(N2O)) of nitrous oxide (N_2O) by quantum cascade laser absorption spectroscopy (QCLAS) as a powerful tool to investigate N_2O production pathways in biological wastewater treatment. QCLAS enables high-precision N_2O isotopomer analysis in real time. This allowed us to trace short-term fluctuations in SP and δ~(15)N~(bulk)_(N2O) and, hence, microbial transformation pathways during individual batch experiments with activated sludge from a pilot-scale facility treating municipal wastewater. On the basis of previous work with microbial pure cultures, we demonstrate that N_2O emitted during ammonia (NH_4~+) oxidation with a SP of -5.8 to 5.6 ‰ derives mostly from nitrite (NO_2~-) reduction (e.g., nitrifier denitrification), with a minor contribution from hydroxylamine (NH_2OH) oxidation at the beginning of the experiments. SP of N_2O produced under anoxic conditions was always positive (1.2 to 26.1 ‰), and SP values at the high end of this spectrum (24.9 to 26.1 ‰) are indicative of N_2O reductase activity. The measured δ~(15)N~(bulk)_(N2O) at the initiation of the NH_4~+ oxidation experiments ranged between -42.3 and -57.6 ‰ (corresponding to a nitrogen isotope effect Δδ~(15)N = δ~(15)N_(substrate)- δ~(15)N~(bulk)_(N2O) of 43.5 to 58.8 ‰), which is considerably higher than under denitrifying conditions (δ~(15)N~(bulk)_(N2O) 2.4 to -17 ‰; Δδ~(15)N = 0.1 to 19.5 ‰). During the course of all NH_4~+ oxidation and nitrate (NO_3~-) reduction experiments, δ~(15)N~(bulk)_(N2O) increased significantly, indicating net ~(15)N enrichment in the dissolved inorganic nitrogen substrates (NH_4~+, NO_3~-) and transfer into the N_2O pool. The decrease in δ~(15)N~(bulk)_(N2O) during NO_2~- and NH_2OH oxidation experiments is best explained by inverse fractionation during the oxidation of NO_2~- to NO_3~-.
机译:我们通过量子级联激光吸收来测量一氧化二氮(N_2O)的位点偏爱(SP)和体积〜(15)N /〜(14)N比(δ〜(15)N〜(本体)_(N2O))的测量光谱法(QCLAS)作为研究生物废水处理中N_2O产生途径的有力工具。 QCLAS可以实时进行高精度的N_2O同位素分析。这使我们能够追踪SP和δ〜(15)N〜(大体积)_(N2O)的短期波动,从而追踪在处理城市污水的中试规模的活性污泥的单独批处理实验中的微生物转化途径。在先前对微生物纯培养物的研究基础上,我们证明了在氨(NH_4〜+)氧化过程中,SP值为-5.8至5.6‰释放的N_2O主要来自亚硝酸盐(NO_2〜-)的还原(例如硝化器反硝化),在实验开始时,羟胺(NH_2OH)氧化的贡献很小。在缺氧条件下产生的N_2O的SP始终为正值(1.2至26.1‰),该光谱的高端(24.9至26.1‰)的SP值指示N_2O还原酶活性。在NH_4〜+氧化实验开始时测得的δ〜(15)N〜(本体)_(N2O)在-42.3至-57.6‰之间(对应于氮同位素效应Δδ〜(15)N =δ〜 (15)N_(底物)-δ〜(15)N〜(本体)_(N2O)为43.5至58.8‰),大大高于反硝化条件下的δ〜(15)N〜(本体)_( N 2 O)为2.4至-17‰;Δδ〜(15)N = 0.1至19.5‰)。在所有NH_4〜+氧化和硝酸盐(NO_3〜-)还原实验过程中,δ〜(15)N〜(本体)_(N2O)均显着增加,表明溶解的无机氮基质中净〜(15)N富集(NH_4〜+,NO_3〜-)并转移到N_2O池中。在NO_2〜-和NH_2OH氧化实验中δ〜(15)N〜(本体)_(N2O)的减少最好用NO_2〜-氧化为NO_3〜-的反分馏来解释。

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  • 来源
    《Environmental Science & Technology》 |2013年第3期|1339-1348|共10页
  • 作者单位

    Eawag, Swiss Federal Institute of Aquatic Science and Technology, Ueberlandstrasse 133, P.O. Box 611, 8600 Duebendorf, Switzerland;

    Department of Environmental Science, Bernouilistrasse 30, University of Basel, 4054 Basel, Switzerland;

    Eawag, Swiss Federal Institute of Aquatic Science and Technology, Ueberlandstrasse 133, P.O. Box 611, 8600 Duebendorf, Switzerland;

    Empa, Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Air Pollution & Environmental Technology, Ueberlandstrasse 129, 8600 Duebendorf, Switzerland;

    Eawag, Swiss Federal Institute of Aquatic Science and Technology, Ueberlandstrasse 133, P.O. Box 611, 8600 Duebendorf, Switzerland;

    Empa, Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Air Pollution & Environmental Technology, Ueberlandstrasse 129, 8600 Duebendorf, Switzerland;

    Eawag, Swiss Federal Institute of Aquatic Science and Technology, Ueberlandstrasse 133, P.O. Box 611, 8600 Duebendorf, Switzerland,Empa, Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Air Pollution & Environmental Technology, Ueberlandstrasse 129, 8600 Duebendorf, Switzerland;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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