Distribution and Source of Nitrate in Groundwater in the Hilly-Plain Transition Area of Jianghan Plain Using Dual N and O Isotopes of Nitrate

Abstract

Nitrogen contamination of groundwater in the Jianghan Plain (JHP) in the middle reaches of the Yangtze River is widespread, but the sources and fate of nitrate (NO₃⁻) in the transitional area between plains and hills are poorly understood. This paper characterized the distribution, sources and transformation processes of NO₃⁻ in groundwater in the hilly-plain transition area of JHP through hydrogeochemistry and dual isotopes (δ¹⁵N and δ¹⁸O-NO₃⁻). The hydrogeochemical results showed that the NO₃⁻ in the plain and hilly areas is heterogeneous and controlled by topography. From plain to hilly areas in summer, NO₃⁻ in groundwater has a general trend of decreasing with the direction of groundwater flow. The groundwater in the plain area is strongly affected by anthropogenic activities, and the NO₃⁻ in the multi-level aquifer gradually decreases with increasing depth. Changes in redox conditions caused by river erosion may be responsible for higher NO₃⁻ in groundwater along the eroded banks. The isotopic results showed that NO₃⁻ in the hilly area mainly comes from soil organic nitrogen, which is a natural source. While, groundwater NO₃⁻ in the plain area is strongly affected by livestock manure and domestic sewage, which may be owing to the high density of residents and the impact of anthropogenic activities.

Keywords

Jianghan Plain / groundwater / nitrate / isotope / underground water / hydrogeology

References

[1] Aeschbach-Hertig W, Gleeson T. Regional Strategies for the Accelerating Global Problem of Groundwater Depletion. Nature Geoscience, 2012, 5(12): 853-861

[2] Bhatnagar A, Sillanpää M. A Review of Emerging Adsorbents for Nitrate Removal from Water. Chemical Engineering Journal, 2011, 168(2): 493-504

[3] Böttcher J, Strebel O, Voerkelius S, et al. . Using Isotope Fractionation of Nitrate-Nitrogen and Nitrate-Oxygen for Evaluation of Microbial Denitrification in a Sandy Aquifer. Journal of Hydrology, 1990, 114(3/4): 413-424

[4] Burkart M R, Kolpin D W. Hydrologic and Land-Use Factors Associated with Herbicides and Nitrate in Near-Surface Aquifers. Journal of Environmental Quality, 1993, 22(4): 646-656

[5] Burow K R, Nolan B T, Rupert M G, et al. . Nitrate in Groundwater of the United States, 1991–2003. Environmental Science & Technology, 2010, 44(13): 4988-4997

[6] Burt T P, Matchett L S, Goulding K W T, et al. . Denitrification in Riparian Buffer Zones: The Role of Floodplain Hydrology. Hydrological Processes, 1999, 13(10): 1451-1463

[7] Carrey R, Ballesté E, Blanch A R, et al. . Combining Multi-Isotopic and Molecular Source Tracking Methods to Identify Nitrate Pollution Sources in Surface and Groundwater. Water Research, 2021, 188: 116537

[8] Chen D J Z, MacQuarrie K T B. Correlation of δ¹⁵N and δ¹⁸O in NO₃⁻ during Denitrification in Groundwater. Journal of Environmental Engineering and Science, 2005, 4(3): 221-226

[9] Chen Z M, Ding W X, Xu Y H, et al. . Importance of Heterotrophic Nitrification and Dissimilatory Nitrate Reduction to Ammonium in a Cropland Soil: Evidences from a ¹⁵N Tracing Study to Literature Synthesis. Soil Biology and Biochemistry, 2015, 91: 65-75

[10] Craig H. Standard for Reporting Concentrations of Deuterium and Oxygen-18 in Natural Waters. Science, 1961, 133(3467): 1833-1834

[11] Dalai T K, Krishnaswami S, Sarin M M. Major Ion Chemistry in the Headwaters of the Yamuna River System. Geochimica et Cosmochimica Acta, 2002, 66(19): 3397-3416

[12] Du Y, Deng Y M, Ma T, et al. . Hydrogeochemical Evidences for Targeting Sources of Safe Groundwater Supply in Arsenic-Affected Multi-Level Aquifer Systems. Science of the Total Environment, 2018, 645: 1159-1171

[13] Ernesto P Z, Rogelio L R, Harter T, et al. . Assessment of Sources and Fate of Nitrate in Shallow Groundwater of an Agricultural Area by Using a Multi-Tracer Approach. Science of the Total Environment, 2014, 470/471: 855-864

[14] Fan L J, Zhao F H, Cheng C. Research Advances in Stable Nitrogen Isotope in Water Bodies. Ying Yong Sheng Tai Xue Bao, 2016, 27(8): 2699-2707

[15] Foster S, Chilton J, Nijsten G J, et al. . Groundwater—A Global Focus on the ‘Local Resource’. Current Opinion in Environmental Sustainability, 2013, 5(6): 685-695

[16] Fukada T, Hiscock K M, Dennis P F, et al. . A Dual Isotope Approach to Identify Denitrification in Groundwater at a River-Bank Infiltration Site. Water Research, 2003, 37(13): 3070-3078

[17] Gibrilla A, Fianko J R, Ganyaglo S, et al. . Nitrate Contamination and Source Apportionment in Surface and Groundwater in Ghana Using Dual Isotopes (¹⁵N and ¹⁸O-NO₃) and a Bayesian Isotope Mixing Model. Journal of Contaminant Hydrology, 2020, 233: 103658

[18] Greer F R, Shannon M, Nutrition T C O. Infant Methemoglobinemia: The Role of Dietary Nitrate in Food and Water. Pediatrics, 2005, 116(3): 784-786

[19] Gu Y S, Guan S, Ma T, et al. . Quaternary Sedimentary Environment Documented by Borehole Stratigraphical Records in Eastern Jianghan Basin. Earth Science, 2018, 43(11): 3989-4000(in Chinese with English Abstract)

[20] Hinkle S R, Tesoriero A J. Nitrogen Speciation and Trends, and Prediction of Denitrification Extent, in Shallow US Groundwater. Journal of Hydrology, 2014, 509: 343-353

[21] Hossain M. Sustainable Arsenic Mitigation A Strategy for Scaling-Up Safe Water Access: A Strategy for Scaling-Up Safe Water Access, 2015,

[22] Kaown D, Koh D C, Mayer B, et al. . Identification of Nitrate and Sulfate Sources in Groundwater Using Dual Stable Isotope Approaches for an Agricultural Area with Different Land Use (Chuncheon, Mid-Eastern Korea). Agriculture, Ecosystems & Environment, 2009, 132(3/4): 223-231

[23] Kendall C. Tracing Nitrogen Sources and Cycling in Catchments. Isotope Tracers in Catchment Hydrology, 1998, Amsterdam. Elsevier

[24] Kendall C, Elliott E M, Wankel S D. Tracing Anthropogenic Inputs of Nitrogen to Ecosystems. Stable Isotopes in Ecology and Environmental Science, 2008, Oxford. Blackwell Publishing Ltd.

[25] Kim S H, Kim H R, Yu S, et al. . Shift of Nitrate Sources in Groundwater due to Intensive Livestock Farming on Jeju Island, South Korea: With Emphasis on Legacy Effects on Water Management. Water Research, 2021, 191: 116814

[26] Korom S F. Natural Denitrification in the Saturated Zone: A Review. Water Resources Research, 1992, 28(6): 1657-1668

[27] Landon M K, Green C T, Belitz K, et al. . Relations of Hydrogeologic Factors, Groundwater Reduction-Oxidation Conditions, and Temporal and Spatial Distributions of Nitrate, Central-Eastside San Joaquin Valley, California, USA. Hydrogeology Journal, 2011, 19(6): 1203-1224

[28] Li J, Shi Z M, Liu M Z, et al. . Identifying Anthropogenic Sources of Groundwater Contamination by Natural Background Levels and Stable Isotope Application in Pinggu Basin, China. Journal of Hydrology, 2021, 596: 126092

[29] Liang X, Zhang J W, Lan K, et al. . Hydrochemical Characteristics of Groundwater and Analysis of Groundwater Flow Systems in Jianghan Plain. Geological Science and Technology Bulletin, 2020, 39(1): 21-33(in Chinese with English Abstract)

[30] Liu C Q, Li S L, Lang Y C, et al. . Using Δ¹⁵N- and Δ¹⁸O-Values to Identify Nitrate Sources in Karst Ground Water, Guiyang, Southwest China. Environmental Science & Technology, 2006, 40(22): 6928-6933

[31] Minet E P, Goodhue R, Meier-Augenstein W, et al. . Combining Stable Isotopes with Contamination Indicators: A Method for Improved Investigation of Nitrate Sources and Dynamics in Aquifers with Mixed Nitrogen Inputs. Water Research, 2017, 124: 85-96

[32] Morrissy J G, Currell M J, Reichman S M, et al. . Nitrogen Contamination and Bioremediation in Groundwater and the Environment: A Review. Earth-Science Reviews, 2021, 222: 103816

[33] Niu B B, Wang H H, Loáiciga H A, et al. . Temporal Variations of Groundwater Quality in the Western Jianghan Plain, China. Science of the Total Environment, 2017, 578: 542-550

[34] Petelet-Giraud E, Baran N, Vergnaud-Ayraud V, et al. . Elucidating Heterogeneous Nitrate Contamination in a Small Basement Aquifer. A Multidisciplinary Approach: NO₃ Isotopes, CFCS-SF₆, Microbiological Activity, Geophysics and Hydrogeology. Journal of Contaminant Hydrology, 2021, 241: 103813

[35] Qin S P, Hu C S, Clough T J, et al. . Irrigation of DOC-Rich Liquid Promotes Potential Denitrification Rate and Decreases N₂O/(N₂O + N₂) Product Ratio in a 0–2 m Soil Profile. Soil Biology and Biochemistry, 2017, 106: 1-8

[36] Rivett M O, Buss S R, Morgan P, et al. . Nitrate Attenuation in Groundwater: A Review of Biogeochemical Controlling Processes. Water Research, 2008, 42(16): 4215-4232

[37] Robertson G P, Vitousek P M. Nitrogen in Agriculture: Balancing the Cost of an Essential Resource. Annual Review of Environment and Resources, 2009, 34: 97-125

[38] Sebilo M, Mayer B, Nicolardot B, et al. . Long-Term Fate of Nitrate Fertilizer in Agricultural Soils. Proceedings of the National Academy of Sciences of the United States of America, 2013, 110(45): 18185-18189

[39] Senbayram M, Chen R, Budai A, et al. . N₂O Emission and the N₂O/(N₂O + N₂) Product Ratio of Denitrification as Controlled by Available Carbon Substrates and Nitrate Concentrations. Agriculture, Ecosystems & Environment, 2012, 147: 4-12

[40] Shen S, Ma T, Du Y, et al. . The Spatial Distribution Characteristic and Genesis of Nitrogen of Shallow Groundwater in the East of Jianghan Plain. Environmental Science & Technology, 2018, 41(2): 47-56(in Chinese with English Abstract)

[41] Showers W J, Genna B, McDade T, et al. . Nitrate Contamination in Groundwater on an Urbanized Dairy Farm. Environmental Science & Technology, 2008, 42(13): 4683-4688

[42] Singleton M J, Esser B K, Moran J E, et al. . Saturated Zone Denitrification: Potential for Natural Attenuation of Nitrate Contamination in Shallow Groundwater under Dairy Operations. Environmental Science & Technology, 2007, 41(3): 759-765

[43] Stoliker D L, Repert D A, Smith R L, et al. . Hydrologic Controls on Nitrogen Cycling Processes and Functional Gene Abundance in Sediments of a Groundwater Flow-through Lake. Environmental Science & Technology, 2016, 50(7): 3649-3657

[44] Wang H L, Lu K Y, Shen C Y, et al. . Human Health Risk Assessment of Groundwater Nitrate at a Two Geomorphic Units Transition Zone in Northern China. Journal of Environmental Sciences, 2021, 110: 38-47

[45] Ward M H, Mark S D, Cantor K P, et al. . Drinking Water Nitrate and the Risk of Non-Hodgkin’s Lymphoma. Epidemiology, 1996, 7(5): 465-471

[46] Xia Y Q, Li Y F, Zhang X Y, et al. . Nitrate Source Apportionment Using a Combined Dual Isotope, Chemical and Bacterial Property, and Bayesian Model Approach in River Systems. Journal of Geophysical Research: Biogeosciences, 2017, 122(1): 2-14

[47] Xiong Y J, Du Y, Deng Y M, et al. . Contrasting Sources and Fate of Nitrogen Compounds in Different Groundwater Systems in the Central Yangtze River Basin. Environmental Pollution, 2021, 290: 118119

[48] Xue D M, Botte J, de Baets B, et al. . Present Limitations and Future Prospects of Stable Isotope Methods for Nitrate Source Identification in Surface- and Groundwater. Water Research, 2009, 43(5): 1159-1170

[49] Yue F J, Li S L, Liu C Q, et al. . Using Dual Isotopes to Evaluate Sources and Transformation of Nitrogen in the Liao River, Northeast China. Applied Geochemistry, 2013, 36: 1-9

[50] Zhang J W, Liang X, Jin M G, et al. . Identifying the Groundwater Flow Systems in a Condensed River-Network Interfluve between the Han River and Yangtze River (China) Using Hydrogeochemical Indicators. Hydrogeology Journal, 2019, 27(7): 2415-2430

[51] Zhou J H, Gao Z, Ma H, et al. . Prevention and Study on Agricultural Non-Point Source Pollution in China. Advances in Electrical Engineering and Electrical Machines, 2011, Berlin, Heidelberg. Springer

[52] Zhou X, Jiang Y H. Application of Nitrogen and Oxygen Isotopes in the Study of Nitrate Pollution in Groundwater. Journal of the Earth, 2007, 28(4): 389-395(in Chinese with English Abstract)

[53] Zhou Y, Wang Y X, Li Y L, et al. . Hydrogeochemical Characteristics of Central Jianghan Plain, China. Environmental Earth Sciences, 2013, 68(3): 765-778

RIGHTS & PERMISSIONS

China University of Geosciences (Wuhan) and Springer-Verlag GmbH Germany, Part of Springer Nature