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Determining the origin and fate of nitrate in the Nanyang Basin, Central China, using environmental isotopes and the Bayesian mixing model

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Abstract

Identifying sources of nitrate contamination has been a long-term challenge in areas with different land uses. We investigated the biogeochemical processes and quantified the contribution of potential nitrate sources in the Nanyang Basin, the source area of the South to North Water Diversion Project in China. Hydrogeochemical characteristics, the dual-isotope method (δ15N-NO3 and δ18O-NO3), and the Bayesian mixing model (SIAR) were combined. The results for 160 samples indicated that mean nitrate concentrations of residential area (162.83 mg L−1) and farmland (75.71 mg L−1) were higher compared with those of surface water (16.15 mg L−1) and forest (36.25 mg L−1). Hydrochemical facies and molar ratios of major ions indicated that the natural environment was greatly impacted by anthropogenic activities. Nitrification, ammonium volatilization, and mixing effects were the dominant processes in nitrogen transformation. The contributions of different sources to nitrate contamination were 45.41%, 35.81%, 17.87%, and 0.91% for sewage and manure, soil organic nitrogen, synthetic fertilizer, and atmospheric deposition, respectively. Undeveloped infrastructure and sewage disposal in rural areas were the main causes of nitrate contamination. Our results provide a theoretical basis for the development of measures to guarantee long-term water supply of the South to North Water Diversion Project.

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References

  • Aeschbach W, Gleeson T (2012) Regional strategies for the accelerating global problem of groundwater depletion. Nat Geosci 5:853–861

    Article  CAS  Google Scholar 

  • Arce MI, von Schiller D, Gómez R (2014) Variation in nitrate uptake and denitrification rates across a salinity gradient in Mediterranean semiarid streams. Aquat Sci 76:295–311

    Article  CAS  Google Scholar 

  • Archana A, Thibodeau B, Geeraert N, Xu MN, Kao S-J, Baker DM (2018) Nitrogen sources and cycling revealed by dual isotopes of nitrate in a complex urbanized environment. Water Res 142:459–470

    Article  CAS  Google Scholar 

  • Atekwana EA, Geyer CJ (2018) Spatial and temporal variations in the geochemistry of shallow groundwater contaminated with nitrate at a residential site. Environ Sci Pollut Res 25:27155–27172

    Article  CAS  Google Scholar 

  • Bakeer S (2016) Effect of ammonium nitrate fertilizer and calcium chloride foliar spray on fruit cracking and sunburn of manfalouty pomegranate trees. Sci Hortic 209:300–308

    Article  CAS  Google Scholar 

  • Buccianti A, Nisi B, Martín-Fernández JA, Palarea-Albaladejo J (2014) Methods to investigate the geochemistry of groundwaters with values for nitrogen compounds below the detection limit. J Geochem Explor 141:78–88

    Article  CAS  Google Scholar 

  • Burkart MR, Kolpin DW (1993) Hydrologic and land-use factors associated with herbicides and nitrate in near-surface aquifers. J Environ Qual 22:646–656

    Article  CAS  Google Scholar 

  • Camacho-Cruz KA, Ortiz-Hernández MC, Sánchez A, Carrillo L, de Jesús Navarrete A (2020) Water quality in the eastern karst region of the Yucatan Peninsula: nutrients and stable nitrogen isotopes in turtle grass, Thalassia testudinum. Environ Sci Pollut Res 27:15967–15983

    Article  CAS  Google Scholar 

  • Chaudhuri Sriroop, Srinivasulu Ale, Delaune Paul, et al. (2012). Spatio-temporal variability of groundwater nitrate concentration in Texas: 1960 to 2010', 41: 1806-17.

  • Chen ZX, Yu L, Liu WG, Lam MHW, Liu G-J, Yin X-B (2014) Nitrogen and oxygen isotopic compositions of water-soluble nitrate in Taihu Lake water system, China: implication for nitrate sources and biogeochemical process. Environ Earth Sci 71:217–223

    Article  CAS  Google Scholar 

  • ChenMin-hua, X., Ling, M.-H., Zhou, Q., Zhang, Z.-C., Cheng, Q.-B., 2011. Numerical modeling the role of rubber dams on groundwater recharge and phreatic evaporation loss in riparian zones. Environmental Earth Sciences - ENVIRON EARTH SCI 65.

  • Clagnan, Elisa, Thornton Steven, Rolfe Stephen, et al. 2017. 'Influence of artificial drainage system design on the nitrogen attenuation potential of gley soils: evidence from hydrochemical and isotope studies under field-scale conditions', Journal of Environmental Management, 206.

  • Dan-Hassan, MA, Olasehinde PI, Amadi AN, et al. 2012. 'Spatial and temporal distribution of nitrate pollution in groundwater of Abuja, Nigeria', Spatial and Temporal Distribution of Nitrate Pollution in Groundwater of Abuja, Nigeria.

  • Deng X, Sun Y, Lei X et al (1996) Illite/smectite diagenesis in the NanXiang, Yitong, and North China Permian-Carboniferous Basins: application to petroleum exploration in China1. AAPG Bull 80:157–172

    CAS  Google Scholar 

  • Deutsch B, Mewes M, Liskow I, Voss M (2006) Quantification of diffuse nitrate inputs into a small river system using stable isotopes of oxygen and nitrogen in nitrate. Org Geochem 37:1333–1342

    Article  CAS  Google Scholar 

  • Ding J, Xi B, Xu Q, Su J, Huo S, Liu H, Yu Y, Zhang Y (2015) Assessment of the sources and transformations of nitrogen in a plain river network region using a stable isotope approach. J Environ Sci 30:198–206

    Article  CAS  Google Scholar 

  • Du Y, Ma T, Deng Y et al (2017) Sources and fate of high levels of ammonium in surface water and shallow groundwater of the Jianghan Plain, Central China. Environ Sci Process Impacts 19:161–172

    Article  CAS  Google Scholar 

  • Elisante, Eliapenda, and Muzuka Alfred. 2015. 'Occurrence of nitrate in Tanzanian groundwater aquifers: a review', Applied Water Science.

  • FAO. 2020. World Food and Agriculture - Statistical Yearbook 2020 (FAO: Rome, Italy).

  • Feth JH, Gibbs RJ (1971) Mechanisms controlling world water chemistry: evaporation-crystallization process. Science 172:870–872

    Article  CAS  Google Scholar 

  • Gautam S, Iqbal MZ (2010) Using stable isotopes of nitrogen to study its source and transformation in a heavily farmed watershed. Environ Earth Sci 60:11–20

    Article  CAS  Google Scholar 

  • Gibrilla A, Fianko JR, Ganyaglo S, Adomako D, Anornu G, Zakaria N (2020) Nitrate contamination and source apportionment in surface and groundwater in Ghana using dual isotopes (15N and 18O-NO3) and a Bayesian isotope mixing model. J Contam Hydrol 233:103658

    Article  CAS  Google Scholar 

  • Granger, Julie, and Wankel Scott. 2016. 'Isotopic overprinting of nitrification on denitrification as a ubiquitous and unifying feature of environmental nitrogen cycling', Proceedings of the National Academy of Sciences, 113.

  • Guo Z, Yan C, Wang Z, Xu F, Yang F (2020) Quantitative identification of nitrate sources in a coastal peri-urban watershed using hydrogeochemical indicators and dual isotopes together with the statistical approaches. Chemosphere 243:125364

    Article  CAS  Google Scholar 

  • Hinshaw SE, Zhang T, John A. Harrison, et al. (2020) Excess N2 and denitrification in hyporheic porewaters and groundwaters of the San Joaquin River, California. Water Res 168:115161

    Article  CAS  Google Scholar 

  • Huizenga A, Bailey R, Gates T (2017) Stream-aquifer and in-stream processes affecting nitrogen along a major river and contributing tributary. J Contam Hydrol 199:24–35

    Article  CAS  Google Scholar 

  • Jin Z, Zheng Q, Zhu C, Wang Y, Cen J, Li F (2018) Contribution of nitrate sources in surface water in multiple land use areas by combining isotopes and a Bayesian isotope mixing model Applied Geochemistry:93

  • Ju XT, Kou CL, Zhang FS, Christie P (2006) Nitrogen balance and groundwater nitrate contamination: Comparison among three intensive cropping systems on the North China Plain. Environ Pollut 143:117–125

    Article  CAS  Google Scholar 

  • Kaushal SS, Groffman PM, Band LE, Elliott EM, Shields CA, Kendall C (2011) Tracking nonpoint source nitrogen pollution in human-impacted watersheds. Environ Sci Technol 45:8225–8232

    Article  CAS  Google Scholar 

  • Kendall C, Ramón A, Cook PG et al (2000) Nitrate isotopes in groundwater systems. Environmental tracers in subsurface hydrology:261–298

  • Kendall Carol, Elliott M. Emily, Wankel D. Scott. 2007. Tracing anthropogenic inputs of nitrogen to ecosystems.' in K. Lajtha R. Michener (ed.), Stable isotopes in ecology and environmental science.

  • Kendall, Carol, Elliott Emily, and Wankel Scott. 2008. 'Tracing anthropogenic inputs of nitrogen to ecosystems.' in.

  • Kim K-H, Yun S-T, Choi B-Y, Chae G-T, Joo Y, Kim K, Kim H-S (2009) Hydrochemical and multivariate statistical interpretations of spatial controls of nitrate concentrations in a shallow alluvial aquifer around oxbow lakes (Osong area, central Korea). J Contam Hydrol 107:114–127

    Article  CAS  Google Scholar 

  • Kim KH, Yun ST, Mayer B, Lee J-H, Kim T-S, Kim H-K (2015) Quantification of nitrate sources in groundwater using hydrochemical and dual isotopic data combined with a Bayesian mixing model. Agric Ecosyst Environ 199:369–381

    Article  CAS  Google Scholar 

  • Kim H, Kaown D, Mayer B, Lee JY, Lee KK (2018) Combining pyrosequencing and isotopic approaches to assess denitrification in a hyporheic zone. Sci Total Environ 631-632:755–764

    Article  CAS  Google Scholar 

  • Knobeloch L, Salna B, Hogan A, Postle J, Anderson H (2000) Blue babies and nitrate-contaminated well water. Environ Health Perspect 108:675–678

    Article  CAS  Google Scholar 

  • Lasagna M, De Luca DA (2019) Evaluation of sources and fate of nitrates in the western Po plain groundwater (Italy) using nitrogen and boron isotopes. Environ Sci Pollut Res 26:2089–2104

    Article  CAS  Google Scholar 

  • Li Y, Yan W, Wang F, Lv S, Li Q, Yu Q (2019) Nitrogen pollution and sources in an aquatic system at an agricultural coastal area of Eastern China based on a dual-isotope approach. Environ Sci Pollut Res 26:23807–23823

    Article  CAS  Google Scholar 

  • Liu M, Seyf-Laye ASM, Ibrahim T et al (2014) Tracking sources of groundwater nitrate contamination using nitrogen and oxygen stable isotopes at Beijing area, China. Environ Earth Sci 72:707–715

    Article  CAS  Google Scholar 

  • Lu L, Cheng H, Pu X, Liu X, Cheng Q (2015) Nitrate behaviors and source apportionment in an aquatic system from a watershed with intensive agricultural activities. Environ Sci Process Impacts 17:131–144

    Article  CAS  Google Scholar 

  • Lunau M, Voss M, Erickson M et al (2012) Excess nitrate loads to coastal waters reduces nitrate removal efficiency: mechanism and implications for coastal eutrophication. Environ Microbiol 15

  • Ma Z, Yang Y, Lian X et al (2016) Identification of nitrate sources in groundwater using a stable isotope and 3DEEM in a landfill in Northeast China. Science of the Total Environment, s 563–564:593–599

    Article  CAS  Google Scholar 

  • Ma P, Liu S, Yu Q, Li X, Han X (2019) Sources and transformations of anthropogenic nitrogen in the highly disturbed Huai River Basin, Eastern China. Environ Sci Pollut Res 26:11153–11169

    Article  CAS  Google Scholar 

  • 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

    Article  CAS  Google Scholar 

  • Mayer B, Bollwerk SM, Mansfeldt T, Hütter B, Veizer J (2001) The oxygen isotope composition of nitrate generated by nitrification in acid forest floors. Geochim Cosmochim Acta 65:2743–2756

    Article  CAS  Google Scholar 

  • Meghdadi A, Javar N (2018a) Evaluation of nitrate sources and the percent contribution of bacterial denitrification in hyporheic zone using isotope fractionation technique and multi-linear regression analysis. J Environ Manag 222:54–65

    Article  CAS  Google Scholar 

  • Meghdadi A, Javar N (2018b) Quantification of spatial and seasonal variations in the proportional contribution of nitrate sources using a multi-isotope approach and Bayesian isotope mixing model. Environ Pollut 235:207–222

    Article  CAS  Google Scholar 

  • Menció A, Mas-Pla J, Otero N, Regàs O, Boy-Roura M, Puig R, Bach J, Domènech C, Zamorano M, Brusi D, Folch A (2016) Nitrate pollution of groundwater; all right…, but nothing else? Sci Total Environ 539:241–251

    Article  CAS  Google Scholar 

  • Mengis M, Walther U, Bernasconi S et al (2001) Limitations of using ?? 18 O for the source identification of nitrate in agricultural soils. Environ Sci Technol 35:1840–1844

    Article  CAS  Google Scholar 

  • Meybeck M (1982) Carbon, nitrogen, and phosphorus transport by world rivers. Am J Sci 282:401–450

    Article  CAS  Google Scholar 

  • Minet E, Coxon C, Goodhue R et al (2012) Evaluating the utility of N-15 and O-18 isotope abundance analyses to identify nitrate sources: a soil zone study. Water Res 46:3723–3736

    Article  CAS  Google Scholar 

  • Minet, EP, Goodhue R, Meier-Augenstein W, et al. 2017. 'Combining stable isotopes with contamination indicators: a method for improved investigation of nitrate sources and dynamics in aquifers with mixed nitrogen inputs', 124: 85,

  • Murgulet D, Tick GR (2013) Understanding the sources and fate of nitrate in a highly developed aquifer system. J Contam Hydrol 155:69–81

    Article  CAS  Google Scholar 

  • Nanyang Municipal Government. (2019). Nanyang Statistical Yearbook (in Chinese) (China Statistics Yearbook: Nanyang, China).

  • Oberhelman, Andrew, and Peterson Eric. 2020. 'Chloride source delineation in an urban-agricultural watershed: deicing agents versus agricultural contributions', Hydrological Processes.

  • Parnell AC, Inger R, Bearhop S, Jackson AL (2010) Source partitioning using stable isotopes: coping with too much variation. PLoS One 5:e9672

    Article  CAS  Google Scholar 

  • Pasten-Zapata E, Ledesma R, Harter T, Ramirez A, Mahlknecht J (2014) Assessment of sources and fate of nitrate in shallow groundwater of an agricultural area by using a multi-tracer approach. Sci Total Environ 470-471:855–864

    Article  CAS  Google Scholar 

  • Piske J, Peterson E (2020) The role of corn and soybean cultivation on nitrate export from Midwestern US agricultural watersheds. Environ Earth Sci 79

  • Rahmati O, Melesse A (2016) Application of Dempster–Shafer theory, spatial analysis and remote sensing for groundwater potentiality and nitrate pollution analysis in the semi-arid region of Khuzestan, Iran. Sci Total Environ 568:1110–1123

    Article  CAS  Google Scholar 

  • Roadcap, George, Keith Hackley, and Hue-Hwa Hwang. 2002. 'Application of nitrogen and oxygen isotopes to identify sources of nitrate'.

    Google Scholar 

  • Roy S, Gaillardet J, Allègre CJ (1999) Geochemistry of dissolved and suspended loads of the Seine River, France: anthropogenic impact, carbonate and silicate weathering. Geochim Cosmochim Acta 63:1277–1292

    Article  CAS  Google Scholar 

  • Sheikhy NT, Aris AZ, Sefie A et al (2017) Detecting and predicting the impact of land use changes on groundwater quality, a case study in Northern Kelantan, Malaysia. Sci Total Environ 599-600:844–853

    Article  CAS  Google Scholar 

  • Shi X, Dong W, Li M, Zhang Y (2012) Evaluation of groundwater renewability in the Henan Plains, China. Geochem J 46:107–115

    Article  CAS  Google Scholar 

  • Sigman D, Casciotti K, Andreani M et al (2001) A bacterial method for the nitrogen isotopic analysis of nitrate in seawater and freshwater. Anal Chem 73:4145–4153

    Article  CAS  Google Scholar 

  • Soto DX, Koehler G, Leonard I. Wassenaar, et al. (2019) Spatio-temporal variation of nitrate sources to Lake Winnipeg using N and O isotope (δ15N, δ18O) analyses. Sci Total Environ 647:486–493

    Article  CAS  Google Scholar 

  • Spalding R, Hirsh AJ, Exner ME et al (2018a) 'Applicability of the dual isotopes δ15N and δ18O to identify nitrate in groundwater beneath irrigated cropland. J Contam Hydrol:220

  • Spalding R, Hirsh A, Exner M et al (2018b) 'Integrated deep soil n and groundwater isotope investigation of n sources captured by municipal wells. Groundwater Monitoring & Remediation:39

  • Su X, Wang H, Zhang Y (2013) Health risk assessment of nitrate contamination in groundwater: a case study of an agricultural area in northeast China. Water Resour Manag 27:3025–3034

    Article  Google Scholar 

  • Taufiq A, Effendi AJ, Iskandar I, Hosono T, Hutasoit LM (2019) Controlling factors and driving mechanisms of nitrate contamination in groundwater system of Bandung Basin, Indonesia, deduced by combined use of stable isotope ratios, CFC age dating, and socioeconomic parameters. Water Res 148:292–305

    Article  CAS  Google Scholar 

  • Torres-Martínez JA, Mora A, Mahlknecht J, Daesslé LW, Cervantes-Avilés PA, Ledesma-Ruiz R (2021) Estimation of nitrate pollution sources and transformations in groundwater of an intensive livestock-agricultural area (Comarca Lagunera), combining major ions, stable isotopes and MixSIAR model. Environ Pollut 269:115445

    Article  CAS  Google Scholar 

  • Wang S, Tang C, Song X, Yuan R, Wang Q, Zhang Y (2013) Using major ions and δ15N-NO3- to identify nitrate sources and fate in an alluvial aquifer of the Baiyangdian lake watershed, North China Plain. Environ Sci Process Impacts 15:1430–1443

    Article  CAS  Google Scholar 

  • Wang Z-h, Miao Y-f, Li S-x (2015) Effect of ammonium and nitrate nitrogen fertilizers on wheat yield in relation to accumulated nitrate at different depths of soil in drylands of China. Field Crop Res 183:211–224

    Article  Google Scholar 

  • Wang S, Zheng W, Currell M et al (2017) Relationship between land-use and sources and fate of nitrate in groundwater in a typical recharge area of the North China. Plain 609:607–620

    CAS  Google Scholar 

  • Wick K, Heumesser C, Schmid E (2011) Groundwater nitrate contamination: factors and indicators. J Environ Manag 111:178–186

    Article  CAS  Google Scholar 

  • Widory D, Petelet-Giraud E, Négrel P, Ladouche B (2005) Tracking the sources of nitrate in groundwater using coupled nitrogen and boron isotopes: a synthesis. Environ Sci Technol 39:539–548

    Article  CAS  Google Scholar 

  • World Health Organization. 2003. "Nitrate and nitrite in drinking-water: background document for development of WHO guidelines for drinking-water quality." In. Geneva: World Health Organization.

  • Wu, Fengchang, Feng Weiying, Guo Wenjing, et al. 2018. 'Using dual isotopes and a Bayesian isotope mixing model to evaluate sources of nitrate of Tai Lake, China', Environmental Science and Pollution Research, 25.

  • Xue D, Botte J, De Baets B et al (2009) Present limitations and future prospects of stable isotope methods for nitrate source identification in surface and groundwater. Water Res 43:1159–1170

    Article  CAS  Google Scholar 

  • Xue D, De Baets B, Van Cleemput O et al (2012) Use of a Bayesian isotope mixing model to estimate proportional contributions of multiple nitrate sources in surface water. Environ Pollut 161:43–49

    Article  CAS  Google Scholar 

  • Yang L, Han J, Xue J et al (2013) Nitrate source apportionment in a subtropical watershed using Bayesian model. Sci Total Environ 463:340–347

    Article  CAS  Google Scholar 

  • Zhang Q, Wang H, Wang L (2018a) Tracing nitrate pollution sources and transformations in the over-exploited groundwater region of north China using stable isotopes. J Contam Hydrol 218:1–9

    Article  CAS  Google Scholar 

  • Zhang Y, Shi P, Li F, Wei A, Song J, Ma J (2018b) Quantification of nitrate sources and fates in rivers in an irrigated agricultural area using environmental isotopes and a Bayesian isotope mixing model. Chemosphere:208

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Acknowledgements

We thank Ling Junhong and Zeng Chaoyan from the Chinese Research Academy of Environmental Sciences for their collaboration in sample processing.

Availability of data and materials

This study included the analysis of major ions concentration and isotopic composition of nitrate and water. Supplementary data associated with this article can be found in the excel file we provided, named Supplemental Material1204. We agree to make it available online if this article could be accepted by your journal.

Funding

This study was supported by the China Geological Survey Program (DD20160322, DD20190303) and the Scientific Major Project of Water Pollution Control and Treatment (2018ZX07109-004).

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Contributions

Shengwei Cao: investigation, formal analysis, data curation, original draft

Yuhong Fei: supervision

Xia Tian: investigation, formal analysis

Xiangxiang Cui: investigation

Xueqiang Zhang: investigation

Ruoxi Yuan: investigation

Yasong Li*: supervision, funding acquisition, writing–review and editing

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Correspondence to Yasong Li.

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Highlights

1. We investigated the impacts of diverse land uses and anthropogenic activities on nitrate in groundwater.

2. Dual-isotope composition illustrated that sewage and manure were the main pollution source.

3. Nitrification and ammonium volatilization were the dominant factors causing variations in isotopic composition.

4. Limitations of the dual-isotope method mask the potential sources of nitrate contamination.

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Cao, S., Fei, Y., Tian, X. et al. Determining the origin and fate of nitrate in the Nanyang Basin, Central China, using environmental isotopes and the Bayesian mixing model. Environ Sci Pollut Res 28, 48343–48361 (2021). https://doi.org/10.1007/s11356-021-14083-2

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