Environmental Science and Pollution Research

, Volume 25, Issue 24, pp 24348–24361 | Cite as

The sources and dispersal of nitrate in multiple waters, constrained by multiple isotopes, in the Wudalianchi region, northeast China

  • Haiyan Zhang
  • Yuesuo Yang
  • Junyu Zou
  • Yujuan Wen
  • Cuiping Gao
Research Article


The Wudalianchi scenic area in NE China has been named an UNESCO “Global Geopark” and “Biosphere Reserve.” During this investigation, the sources of nitrate and the hydrologic system through which it is dispersed were assessed using geochemical data and a multiple isotopic approach. The cold waters from the south and north springs originated from the deep subsurface. Isotopically, these waters exhibited relatively negative δD and δ18O values and nitrate in the water was substantially depleted 15N, suggesting that the mineral water was primarily derived from depth. Lakes within the Wudalianchi region were primarily composed of water from these deep mineral springs and precipitation. Chemical fertilizers were the primary source of nitrate to the Wudalianchi lakes. Groundwater was found in shallow mineral springs and wells plotted above the local meteoric water line, implying that shallow groundwater was primarily derived from precipitation. Elevated concentrations of nitrate in shallow mineral springs and well waters during the summer, autumn, and winter suggest that shallow groundwater within the Yaoquan volcanic area was also polluted by nitrate from human activities. Denitrification of shallow groundwater is slow, reducing the potential for “self-remediation”. The concentration data are supported by nitrogen (N) isotope data; wells and springs exhibited N isotopic ratios between − 5‰ and + 5‰ (typical of fertilizers and precipitation) and exhibited higher oxygen (O) isotope values than water in the Wudalianchi lakes. These relationships suggest that nitrate in shallow mineral springs, wells, and lakes near the Yaoquan volcano was derived from the mixing of chemical fertilizers with local summer rainfall.


Wudalianchi Nitrate pollution Nitrogen isotopes Hydrogen and oxygen tracers Lakes and groundwater 



We gratefully acknowledge Prof. Philippe Garrigues and two anonymous reviewers for their thoughtful and constructive comments.

Funding information

This work was supported financially by National Natural Science Foundation of China (Grant No. 41472237), Jilin University Postdoctoral Research Start-up Funds (801171050425), Liaoning Innovation Team Project (No. LT2015017) and Research Programs of Heilongjiang Land and Resources Department.


  1. Andersson KK, Hooper AB (1983) O2 and H2O are each the source of one O in NO2 produced from NH3 by Nitrosomonas: 15N−NMR evidence. FEBS Lett 164:236–240.
  2. Aravena R, Evans ML, Cherry JA (2010) Stable isotopes of oxygen and nitrogen in source identification of nitrate from septic systems. Ground Water 31:180–186. CrossRefGoogle Scholar
  3. Böhlke JK, Denver JM (1995) Combined use of groundwater dating, chemical and isotopic analyses to resolve the history and fate nitrate contamination in two agricultural watersheds, Atlantic Coastal Plain, Maryland. Water Resour Res 31(9):2319–2339. CrossRefGoogle Scholar
  4. Böttcher J, Strebel O, Voerkelius S, Schmidt HL (1990) Using isotope fractionation of nitrate nitrogen and nitrate oxygen for evaluation of denitrification in a sandy aquifer. J Hydrol 114:413–424. CrossRefGoogle Scholar
  5. Burns DA, Kendall C (2002) Analysis of δ15N and δ18O to differentiate NO3 - sources in runoff at two watersheds in the Catskill Mountains of New York. Water Resour Res 38:9-1–9-11.
  6. Clark ID, Fritz P (1997) Environmental isotopes in hydrogeology. Lewis Publishers, New YorkGoogle Scholar
  7. Craig H (1961) Isotopic variation in meteoric waters. Science 133:1702–1703CrossRefGoogle Scholar
  8. Dansgaard W (1964) Stable isotopes in precipitation. Tellus 16:436–468CrossRefGoogle Scholar
  9. Du JG, Li SQ, Zhao Y et al (1999) Geochemical characteristics of gases from the Wudalianchi volcanic area, Northeastern China. Acta Geol Sin (English Edition) 73:225–229. CrossRefGoogle Scholar
  10. Finlay JC, Sterner RW, Kumar S (2007) Isotopic evidence for in-lake production of accumulating nitrate in Lake Superior. Ecol Appl 17:2323–2332. CrossRefGoogle Scholar
  11. Guo W, Huo S, Xi B, Zhang J, Wu F (2015) Heavy metal contamination in sediments from typical lakes in the five geographic regions of China: distribution, bioavailability, and risk. Ecol Eng 81:243–255. CrossRefGoogle Scholar
  12. Gui Z, Xue B, Yao S, Zhang F, Yi S (2012) Catchment erosion and trophic status changes over the past century as recorded in sediments from Wudalianchi Lake, the northernmost volcanic lake in China. Quatern Int 282:163–170. CrossRefGoogle Scholar
  13. Han G, Lv P, Tang Y, Song Z (2017) Spatial and temporal variation of H and O isotopic compositions of the Xijiang River system, Southwest China. Isot Environ Health Stud 1:137–146. CrossRefGoogle Scholar
  14. Hiscock KM, Lloyd JW, Lerner DN (1991) Review of natural and artificial denitrification of groundwater. Water Res 25(9):1099–1111. CrossRefGoogle Scholar
  15. Kang P, Xu S (2016) The impact of mariculture on nutrient dynamics and identification of the nitrate sources in coastal waters. Environ Sci Pollut R 23(2):1300–1311. CrossRefGoogle Scholar
  16. Kellman L, Hillaire-Marcel C (1998) Nitrate cycling in streams: using natural abundances of NO3 15N to measure in-situ denitrification. Biogeochemistry 43:273–292. CrossRefGoogle Scholar
  17. Kendall C, Elliott EM, Wankel SD (2007) Tracing anthropogenic inputs of nitrogen to ecosystems. Stable isotopes in ecology and environmental science, Second Edition 375–449.
  18. Kendall C, McDonell JJ e (1998) Isotope tracers in catchment hydrology. Elsevier Science, AmsterdamGoogle Scholar
  19. Kendall C (1998) Tracing nitrogen courses and cycling in catchments. Isotope Tracers in Catchment Hydrology Chapter 16.
  20. Kool DM, Wrage N, Oenema O, van Kessel C, van Groenigen JW (2011) Oxygen exchange with water alters the oxygen isotopic signature of nitrate in soil ecosystems. Soil Biol Biochem 43:1180–1185. CrossRefGoogle Scholar
  21. Lake JL, McKinney RA, Osterman FA, Pruell RJ, Kiddon J, Ryba SA, Libby AD (2001) Stable nitrogen isotopes as indicators of anthropogenic activities in small freshwater systems. Can J Fish Aquat Sci 58:870–878CrossRefGoogle Scholar
  22. Li SL, Liu CQ, Li J, Liu X, Chetelat B, Wang B, Wang F (2010) Assessment of the sources of nitrate in the Changjiang River, China using a nitrogen and oxygen isotopic approach. Environ Sci Technol 44:1573–1578. CrossRefGoogle Scholar
  23. Li SL, Liu CQ, Li J, Xue Z, Guan J, Lang Y, Ding H, Li L (2013) Evaluation of nitrate source in surface water of southwestern China; based on stable isotopes. Environ Earth Sci 68:219–228. CrossRefGoogle Scholar
  24. Li SL, Yue FJ, Liu CQ et al (2015) The O and H isotope characteristics of water from major rivers in China. Chin J Geochem 34:28–37. CrossRefGoogle Scholar
  25. Liang LE, Li C, Shi XH et al (2017) Characteristics of hydrogen and oxygen isotopes of surface and groundwater and the analysis of source of lake water in Hulun Lake Basin, Inner Mongolia. Wetland Sci-China 15(3):385–390 (in Chinese with an English abstract)Google Scholar
  26. Liang XJ, Xiao CL, Sheng HX et al (2007) Migration and transformation of ammonia-nitrite-nitrates in groundwater in the City of Jilin. J Jilin University (Earth Science Edition) 37(2):335–345 (in Chinese with an English abstract)Google Scholar
  27. Liu CQ, Li SL, Lang YC, Xiao HY (2006) Using δ15N- and δ18O-values to identify nitrate sources in karst ground water, Guiyang, Southwest China. Environ Sci Technol 40:6928–6933. CrossRefGoogle Scholar
  28. Mcilvin MR, Altabet MA (2005) Chemical conversion of nitrate and nitrite to nitrous oxide for nitrogen and oxygen isotopic analysis in freshwater and seawater. Anal Chem 77:5589–5595. CrossRefGoogle Scholar
  29. Mengis M, Walther U, Bernasconi SM, Wehrli B (2001) Limitations of using delta 18O for the source identification of nitrate in agricultural soils. Environ Sci Technol 35:1840–1844. CrossRefGoogle Scholar
  30. Nestler A, Berglund M, Accoe F, Duta S, Xue D, Boeckx P, Taylor P (2011) Isotopes for improved management of nitrate pollution in aqueous resources: review of surface water field studies. Environ Sci Pollut R. 18(4):519–533. CrossRefGoogle Scholar
  31. Nikolenko O, Jurado A, Borges AV et al (2017) Isotopic composition of nitrogen species in groundwater under agricultural areas: a review. Sci Total Environ.
  32. Pardo LH, Kendall C, Pett-Ridge J, Chang CCY (2004) Evaluating the source of streamwater nitrate using δ15N and δ18O in nitrate in two watersheds in New Hampshire, USA. Hydrol Process 18:2699–2712. CrossRefGoogle Scholar
  33. Rozanski K, Araguas-Araguas L, Gonfiantini R (1993) Isotope patterns in modern global precipitation. In: Swart PK et al (eds) Climate change in continental isotope records, geophysical monograph series, vol 78. AGU, Washington, pp 1–36Google Scholar
  34. Sun RB, Du JG (1998) The hydro-geochemical background of the Wudalianchi volcanic area. Bulletin mineral. Petrol Geochem 17(3):150–155 (in China with an English abstract)Google Scholar
  35. Wang XZ (2001a) The new explanation of the cause of Wudalianchi mineral water. Heilongjiang Geol 1:27–39 (in Chinese with an English abstract)Google Scholar
  36. Wang YP (2001b) Evaluation and discussion on the primary mineral water resources of Yaoquanshan in Wudalianchi. Heilongjiang Geol 4:95–107 (in Chinese with an English abstract)Google Scholar
  37. Xiao HY, Liu CQ (2002) Sources of nitrogen and sulfur in wet deposition at Guiyang, southwest China. Atmos Environ 36:5121–5130. CrossRefGoogle Scholar
  38. Xiao K, Shen LC, Wang P (2014) Hydrogen and oxygen isotopes of lake water and geothermal spring water in arid area of south Tibet. Environ Sci 35(8):2952 (in China with an English abstract)Google Scholar
  39. Xing G, Cao Y, Shi S et al (2001) N pollution sources and denitrification in waterbodies in Taihu Lake region. Sci China Ser B 44:304–314. CrossRefGoogle Scholar
  40. Xue D, Botte J, De Baets B, Accoe F, Nestler A, Taylor P, Van Cleemput O, Berglund M, Boeckx P (2009) Present limitations and future prospects of stable isotope methods for nitrate source identification in surface and groundwater. Water Res 43:1159–1170. CrossRefGoogle Scholar
  41. Yan L, Hu H, Zhang S, Chen P, Wang W, Li H (2017) Arsenic tolerance and bioleaching from realgar based on response surface methodology by Acidithiobacillus ferrooxidans, isolated from Wudalianchi volcanic lake, northeast China. Electron J Biotechnol 25(C):50–57. CrossRefGoogle Scholar
  42. Yue FJ, Li SL, Liu CQ, Zhao ZQ, Hu J (2013) Using dual isotopes to evaluate sources and transformation of nitrogen in the Liao River, northeast China. Appl Geochem 36:1–9. CrossRefGoogle Scholar
  43. Yue FJ, Liu CQ, Li SL, Zhao ZQ, Liu XL, Ding H, Liu BJ, Zhong J (2014) Analysis of δ15N and δ18O to identify nitrate sources and transformations in Songhua River, Northeast China. J Hydrol 519:329–339. CrossRefGoogle Scholar
  44. Yue FJ, Li SL, Liu CQ, Lang YC, Ding H (2015) Sources and transport of nitrate constrained by the isotopic technique in a karst catchment: an example from southwest China. Hydrol Process 29:1883–1893. CrossRefGoogle Scholar
  45. Yue FJ, Li SL, Liu CQ, Zhao ZQ, Ding H (2017) Tracing nitrate sources with dual isotopes and long term monitoring of nitrogen species in the Yellow River, China. Sci Rep-UK 7(1):8537. CrossRefGoogle Scholar
  46. Zeng Y, Yang C, Wang XY et al (2017) Application of principal component analysis to parse the source of heavy metals in surface sediments of volcano dammed lake in Wudalianchi. Environ Dev 42:168–170 (in Chinese with an English abstract)Google Scholar
  47. Zhang YD, Wang YP, Li JZ et al (1988) Genesis study of mineral water in Yaoquan Mountain in Wudalianchi. Hydrogeol Eng 4:28–31 (in Chinese)Google Scholar
  48. Zheng MF, Hu WJ, Qiu YS et al (2017) N2O preconcentration device upgraded for Gasbench || -IRMS analyzing N and O isotopes of seawater nitrate. J Appl Oceanography 36:135–142 (in Chinese with an English abstract)Google Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  • Haiyan Zhang
    • 1
    • 2
  • Yuesuo Yang
    • 1
    • 3
  • Junyu Zou
    • 1
  • Yujuan Wen
    • 3
  • Cuiping Gao
    • 3
  1. 1.Key Lab of Groundwater Environment & Resources (Jilin University)Ministry of EducationChangchunChina
  2. 2.Hydrogeology and Engineering Geology Survey of Heilongjiang ProvinceHaerbinChina
  3. 3.Key Lab of Eco-Restoration of Regional Polluted Environment (Shenyang University)Ministry of EducationShengyangChina

Personalised recommendations