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CLC number: Q939.99

On-line Access: 2019-01-07

Received: 2018-03-31

Revision Accepted: 2018-07-22

Crosschecked: 2019-01-02

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Citations:  Bibtex RefMan EndNote GB/T7714

 ORCID:

Man Zhang

https://orcid.org/0000-0003-0999-3769

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Journal of Zhejiang University SCIENCE B 2019 Vol.20 No.1 P.49-58

10.1631/jzus.B1800197


Factors influencing the accuracy of the denitrifier method for determining the oxygen isotopic composition of nitrate


Author(s):  Man Zhang, Jia-chun Shi, Lao-sheng Wu

Affiliation(s):  Institute of Soil and Water Resources and Environmental Science, College of Environmental and Resource Sciences, Zhejiang Provincial Key Laboratory of Agricultural and Environment, Zhejiang University, Hangzhou 310058, China; more

Corresponding email(s):   jcshi@zju.edu.cn

Key Words:  Denitrifier method, Nitrate, δ15N, δ18O, Dissolved oxygen, δ18O contraction


Man Zhang, Jia-chun Shi, Lao-sheng Wu. Factors influencing the accuracy of the denitrifier method for determining the oxygen isotopic composition of nitrate[J]. Journal of Zhejiang University Science B, 2019, 20(1): 49-58.

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DOI - 10.1631/jzus.B1800197


Abstract: 
The denitrifier method is widely used as a novel pretreatment method for the determination of nitrogen and oxygen isotope ratios as it can provide quantitative and high-sensitivity measurements. Nevertheless, the method is limited by relatively low measurement accuracy for δ18O. In this study, we analyzed the factors influencing the accuracy of δ18O determination, and then systematically investigated the effects of dissolved oxygen concentrations and nitrate sample sizes on estimates of the δ15N and δ18O of nitrate reference materials. The δ18O contraction ratio was used to represent the relationship between the measured difference and true difference between two reference materials. We obtained the following main results: (1) a gas-liquid ratio of 3:10 (v/v) in ordinary triangular flasks and a shaking speed of 120 r/min produced an optimal range (1.9 to 2.6 mg/L) in the concentration of dissolved oxygen for accurately determining δ18O, and (2) the δ18O contraction ratio decreased as nitrate sample size decreased within a certain range (1.0 to 0.1 μmol). Our results suggested that δ18O contraction is influenced mainly by dissolved oxygen concentrations in pure culture, and provided a model for improving the accuracy of oxygen isotope analysis.

影响细菌反硝化法测量硝酸盐氧同位素的因素分析

目的:针对硝酸盐氮氧同位素新型预处理方法--细菌反硝化法尚存在的氧同位素测试精度低和两种标准物质间的δ18O差值会收缩等问题进行优化试验和机理探究.
创新点:首次深入探究纯培养时的溶解氧浓度和硝酸盐进样量对同位素测试结果的影响及原因,可为氧同位素测试精度的提高提供方法和参考.
方法:通过控制培养瓶内的气液比(1:5、3:10、2:5和3:5)和摇床转速(60和120 r/min)来调节纯培养时的溶解氧浓度,并设计不同的硝酸盐进样量(0.05~1.00 µmol),由硝酸盐标准物质的测试结果判断适宜的溶解氧浓度和硝酸盐进样量.
结论:标准物质间的δ18O差值收缩主要受溶解氧浓度的影响.根据氧同位素测试结果的精度和δ18O差值收缩率的大小,得出以下结论:当普通三角瓶内的气液比为3:10,摇床转速为120 r/min时的溶解氧浓度最佳(1.9~2.6 mg/L),0.2~0.4 nmol的硝酸盐进样量最适宜.

关键词:细菌反硝化法;硝酸盐;δ15N;δ18O;溶解氧;δ18O收缩

Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article

Reference

[1]Böhlke JK, Coplen TB, 1995. Interlaboratory comparison of reference materials for nitrogen-isotope-ratio measurements. A Consultants Meeting on Reference and Intercomparison Materials for Stable Isotopes of Light Elements, p.51-66.

[2]Böhlke JK, Mroczkowski SJ, Coplen TB, 2003. Oxygen isotopes in nitrate: new reference materials for 18O:17O:16O measurements and observations on nitrate-water equilibration. Rapid Commun Mass Spectrom, 17(16):1835-1846.

[3]Bu F, Hu X, Li X, et al., 2015. Cassava stillage and its anaerobic fermentation liquid as external carbon sources in biological nutrient removal. J Zhejiang Univ-Sci B (Biomed & Biotechnol), 16(4):304-316.

[4]Casciotti KL, Sigman DM, Hastings MG, et al., 2002. Measurement of the oxygen isotopic composition of nitrate in seawater and freshwater using the denitrifier method. Anal Chem, 74(19):4905-4912.

[5]Christensen S, Tiedje JM, 1988. Sub-parts-per-billion nitrate method: use of an N2O-producing denitrifier to convert NO3 or 15NO3 to N2O. Appl Environ Microbiol, 54(6):1409-1413.

[6]Dahal B, Hastings MG, 2016. Technical considerations for the use of passive samplers to quantify the isotopic composition of NOx and NO2 using the denitrifier method. Atmos Environ, 143:60-66.

[7]Dai SH, Xie LH, Peng L, et al., 2017. Determination of nitrogen and oxygen isotopes in nitrates: a minireview. Anal Lett, 50(13):2045-2057.

[8]Deng K, 2010. Study on Denitrification and Character of Denitrifying Bacteria. MS Thesis, South China University of Technology, Guangzhou, China (in Chinese).

[9]Downes MT, 1988. Aquatic nitrogen transformations at low oxygen concentrations. Appl Environ Microbiol, 54(1):172-175.

[10]Galloway JN, Dentener FJ, Capone DG, et al., 2004. Nitrogen cycles: past, present, and future. Biogeochemistry, 70(2):153-226.

[11]Glockner AB, Jüngst A, Zumft WG, 1993. Copper-containing nitrite reductase from Pseudomonas aureofaciens is functional in a mutationally cytochrome cd1-free background (NirS) of Pseudomonas stutzeri. Arch Microbiol, 160(1):18-26.

[12]Granger J, Sigman DM, 2009. Removal of nitrite with sulfamic acid for nitrate N and O isotope analysis with the denitrifier method. Rapid Commun Mass Spectrom, 23(23):3753-3762.

[13]Hastings MG, Sigman DM, Lipschultz F, 2003. Isotopic evidence for source changes of nitrate in rain at Bermuda. J Geophys Res, 108(D24):4790.

[14]Hu X, Sobotka D, Czerwionka, K, et al., 2018. Effects of different external carbon sources and electron acceptors on interactions between denitrification and phosphorus removal in biological nutrient removal processes. J Zhejiang Univ-Sci B (Biomed & Biotechnol), 19(4):305-316.

[15]Huang XL, Xin MX, 2009. Microbiology. Higher Education Press, Beijing, China, p.193 (in Chinese).

[16]Koehler GD, Chipley D, Kyser TK, 1991. Measurement of the hydrogen and oxygen isotopic compositions of concentrated chloride brines and brines from fluid inclusions in halite. Chem Geol, 94(1):45-54.

[17]Kumar M, Lin JG, 2010. Co-existence of anammox and denitrification for simultaneous nitrogen and carbon removal— strategies and issues. J Hazard Mater, 178(1-3):1-9.

[18]Liu XY, Koba K, Takebayashi Y, et al., 2012. Preliminary insights into δ15N and δ18O of nitrate in natural mosses: a new application of the denitrifier method. Environ Pollut, 162:48-55.

[19]Matiatos I, 2016. Nitrate source identification in groundwater of multiple land-use areas by combining isotopes and multivariate statistical analysis: a case study of Asopos basin (Central Greece). Sci Total Environ, 541:802-814.

[20]McIlvin MR, Casciotti KL, 2011. Technical updates to the bacterial method for nitrate isotopic analyses. Anal Chem, 83(5):1850-1856.

[21]Mørkved PT, Dörsch P, Søvik AK, et al., 2007. Simplified preparation for the δ15N-analysis in soil NO3 by the denitrifier method. Soil Biol Biochem, 39(8):1907-1915.

[22]Morozkina EV, Zvyagilskaya RA, 2007. Nitrate reductases: structure, functions, and effect of stress factors. Biochemistry (Moscow), 72(10):1151-1160.

[23]Oelmann Y, Kreutziger Y, Bol R, et al., 2007. Nitrate leaching in soil: tracing the NO3 sources with the help of stable N and O isotopes. Soil Biol Biochem, 39(12):3024-3033.

[24]Popescu R, Mimmo T, Dinca OR, et al., 2015. Using stable isotopes in tracing contaminant sources in an industrial area: a case study on the hydrological basin of the Olt River, Romania. Sci Total Environ, 533:17-23.

[25]Qi HP, Coplen TB, Geilmann H, et al., 2003. Two new organic reference materials for δ13C and δ15N measurements and a new value for the δ13C of NBS 22 oil. Rapid Commun Mass Spectrom, 17(22):2483-2487.

[26]Rock L, Ellert BH, Mayer B, 2011. Tracing sources of soil nitrate using the dual isotopic composition of nitrate in 2 M KCl-extracts. Soil Biol Biochem, 43(12):2397-2405.

[27]Rogers KM, Nicolini E, Gauthier V, 2012. Identifying source and formation altitudes of nitrates in drinking water from Réunion Island, France, using a multi-isotopic approach. J Contam Hydrol, 138-139:93-103.

[28]Sigman DM, Casciotti KL, Andreani M, et al., 2001. A bacterial method for the nitrogen isotopic analysis of nitrate in seawater and freshwater. Anal Chem, 73(17):4145-4153.

[29]Silva SR, Kendall C, Wilkison DH, et al., 2000. A new method for collection of nitrate from fresh water and the analysis of nitrogen and oxygen isotope ratios. J Hydrol, 228(1-2):22-36.

[30]Stark JM, Hart SC, 1996. Diffusion technique for preparing salt solutions, Kjeldahl digests, and persulfate digests for nitrogen-15 analysis. Soil Sci Soc Am J, 60(6):1846-1855.

[31]Stevens RJ, Laughlin RJ, 1994. Determining nitrogen-15 in nitrite or nitrate by producing nitrous oxide. Soil Sci Soc Am J, 58(4):1108-1116.

[32]Tiedje JM, 1988. Ecology of denitrification and dissimilatory nitrate reduction to ammonium. In: Zehnder AJB (Ed.), Environmental Microbiology of Anaerobes. John Wiley and Sons, New York, p.179-224.

[33]Vicars WC, Morin S, Savarino J, et al., 2013. Spatial and diurnal variability in reactive nitrogen oxide chemistry as reflected in the isotopic composition of atmospheric nitrate: results from the CalNex 2010 field study. J Geophys Res: Atmos, 118(18):10567-10588.

[34]Wang HY, Ma F, Su JF, et al., 2007. Identification and characterization of a bacterial strain C3 capable of aerobic denitrification. Environ Sci, 28(7):1548-1552 (in Chinese).

[35]Ward EJ, Semmens BX, Schindler DE, 2010. Including source uncertainty and prior information in the analysis of stable isotope mixing models. Environ Sci Technol, 44(12):4645-4650.

[36]Weigand MA, Foriel J, Barnett B, et al., 2016. Updates to instrumentation and protocols for isotopic analysis of nitrate by the denitrifier method. Rapid Commun Mass Spectrom, 30(12):1365-1383.

[37]Widory D, Petelet-Giraud E, Négrel P, et al., 2005. Tracking the sources of nitrate in groundwater using coupled nitrogen and boron isotopes: a synthesis. Environ Sci Technol, 39(2):539-548.

[38]Xu CY, Li YZ, Hao WP, et al., 2012. Analysis of nitrogen isotopic composition of nitrate in water by denitrifier method and trace-gas/isotope ratio mass spectrometry. Chin J Anal Chem, 40(9):1360-1365 (in Chinese).

[39]Xue DM, de Baets B, Vermeulen J, et al., 2010. Error assessment of nitrogen and oxygen isotope ratios of nitrate as determined via the bacterial denitrification method. Rapid Commun Mass Spectrom, 24(14):1979-1984.

[40]Yang LP, Han JP, Xue JL, et al., 2013. Nitrate source apportionment in a subtropical watershed using Bayesian model. Sci Total Environ, 463-464:340-347.

[41]Ye RW, Toro-Suarez I, Tiedje JM, et al., 1991. H218O isotope exchange studies on the mechanism of reduction of nitric oxide and nitrite to nitrous oxide by denitrifying bacteria. Evidence for an electrophilic nitrosyl during reduction of nitric oxide. J Biol Chem, 266(20):12848-12851.

[42]Zhou Q, Takenaka S, Murakami S, et al., 2007. Screening and characterization of bacteria that can utilize ammonium and nitrate ions simultaneously under controlled cultural conditions. J Biosci Bioeng, 103(2):185-191.

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