Abstract

Fluoride-enriched geothermal resources have the potential risks for human health, which may cause dental fluorosis and bone fluorosis. Previous research has predominantly focused on the hydrochemical characteristics of high-fluoride groundwater in the North China Plain (NCP), with limited attention given to the evolution of fluoride-enriched geothermal groundwater. This study, utilizing a dataset of major ion concentrations, ?D, and ?18O from 45 samples, aims to investigate the hydrochemistry, evolution, and genetic mechanisms of fluoride-enriched geothermal groundwater in southern NCP. Our findings indicate that the geothermal groundwater originates from precipitation in the Taihangshan area, with a recharge elevation of 1415~1838 m. After deep circulation at depths of 3556~4135 m and heating by a geothermal reservoir at 150~170 °C, the groundwater mixes with shallow cold groundwater during upwelling, incorporating a proportion of 58~93%. The hydrological evolution process of fluoride-enriched geothermal groundwater is primarily driven by water–rock interactions and the dissolution of fluoride-enriched minerals, while also being influenced by the alkaline groundwater environment and cation exchange interactions. Based on these analyses, a conceptual model of the evolution of fluoride-enriched geothermal groundwater in the NCP is proposed. Health risk assessment results reveal that children are at a higher health risk from fluoride—enriched geothermal groundwater compared to adult females and males.

Acknowledgements

The authors are very thankful to Chinese Academy of Geological Science, the Department of Natural Resources of Hebei Province, Natural Science Basic Research Program of Shaanxi and National Natural Science Foundation of China for providing the necessary fund and facilities during the entire period of study.

Funding

This study is supported by Deep Earth Probe and Mineral Resources Exploration -National Science and Technology Major Project (2024ZD1004103), Chinese Academy of Geological Sciences Basal Research Fund (No. JKY202406, No. JKYQN202307 and No. JKYZD202401), the geological exploration project of Department of Natural Resources of Hebei Province (454–0503-YBN-5DAN), Natural Science Basic Research Program of Shaanxi (2022JQ-238), and National Natural Science Foundation of China (42302301).

Author information

Authors and Affiliations

Contributions

Jiemin Jin: Conceptualization, Data curation, Formal Analysis, Funding acquisition, Project administration, Writing–original draft. Haimin Wang: Data curation, Funding acquisition, Methodology, Project administration. Shouchuan Zhang: Conceptualization, Data curation, Formal Analysis, Funding acquisition, Methodology, Software, Writing–review and editing. Renxia Wang: Conceptualization, Data curation, Funding acquisition, Methodology, Software, Writing–review and editing. Jiahui He: Investigation and Visualization. Kun Yu: Investigation and Funding acquisition.

Corresponding authors

Correspondence to Shouchuan Zhang or Renxia Wang.

References

  • Aitken, A. R. A., Li, L., Kulessa, B., et al. (2023). Antarctic sedimentary basins and their influence on ice-sheet dynamics. Reviews of Geophysics, 61(3), e2021RG000767.

    Google Scholar

  • Bagheri-Gavkosh, M., Hosseini, S. M., Ataie-Ashtiani, B., et al. (2021). Land subsidence: A global challenge. Science of the Total Environment, 778, 146193.

    CAS  Google Scholar

  • Banner, J. L., Wasserburg, G. J., Dobson, P. F., et al. (1989). Isotopic and trace element constraints on the origin and evolution of saline groundwaters from central Missouri. Geochimica Et Cosmochimica Acta, 53(2), 383–398.

    CAS  Google Scholar

  • Barbieri, M., Franchini, S., Barberio, M. D., et al. (2021). Changes in groundwater trace element concentrations before seismic and volcanic activities in Iceland during 2010–2018. Science of the Total Environment, 793, 148635.

    CAS  Google Scholar

  • Cao, W., Zhang, Z., Guo, H., et al. (2023). Spatial distribution and controlling mechanisms of high fluoride groundwater in the coastal plain of Bohai Rim, North China. Journal of Hydrology, 617, 128952.

    CAS  Google Scholar

  • Chen, S., Zhang, Q., Andrews-Speed, P., et al. (2020). Quantitative assessment of the environmental risks of geothermal energy: A review. Journal of Environmental Management, 276, 111287.

    Google Scholar

  • Craig, H. (1961). Isotopic variations in meteoric waters. Science, 133, 1702–1703.

    CAS  Google Scholar

  • Diamond, L. W., Wanner, C., & Waber, H. N. (2018). Penetration depth of meteoric water in orogenic geothermal systems. Geology, 46(12), 1063–1066.

    CAS  Google Scholar

  • Deng, W. P., Yu, X. X., & Jia, G. D. (2012). Sources and Stable Isotope Characteristies of Precipitation in North China (In Chinese). Bulletin of Mineralogy, Petrology and Geochemistry., 31(5), 489–494.

    Google Scholar

  • Gibbs, R. J. (1970). Mechanisms controlling world water chemistry. Science, 170(3962), 1088–1090.

    CAS  Google Scholar

  • Guo, Q., Pang, Z. H., Wang, Y. C., et al. (2017). Fluid geochemistry and geothermometry applications of the Kangding high-temperature geothermal system in eastern Himalayas. Applied Geochemistry, 81, 63–75.

    CAS  Google Scholar

  • Hatton, J. W. (1970). Ground subsidence of a geothermal field during exploitation. Geothermics, 2, 1294–1296.

    Google Scholar

  • He, S., Li, P., Su, F., et al. (2022). Identification and apportionment of shallow groundwater nitrate pollution in Weining Plain, northwest China, using hydrochemical indices, nitrate stable isotopes, and the new Bayesian stable isotope mixing model (MixSIAR). Environmental Pollution, 298, 118852.

    CAS  Google Scholar

  • Hu, Y., Cheng, H., & Tao, S. (2023). Environmental and human health impacts of geothermal exploitation in China and mitigation strategies. Critical Reviews in Environmental Science and Technology, 53(11), 1173–1196.

    CAS  Google Scholar

  • Jia, W., Liu, K., Liu, L., et al. (2023). Characteristics of geothermal waters in eastern Wugongshan based on hydrogen, oxygen, and strontium isotopes. Applied Geochemistry, 2024, 161.

    Google Scholar

  • Jing, H., He, X., Tian, Y., Lancia, M., Cao, G., Crivellari, A., Guo, Z., & Zheng, C. (2023). Comparison and interpretation of data-driven models for simulating site-specific human-impacted groundwater dynamics in the North China Plain. Journal of Hydrology, 616, 128751.

    Google Scholar

  • Kumari, W. G. P., & Ranjith, P. G. (2019). Sustainable development of enhanced geothermal systems based on geotechnical research—A review. Earth-Science Reviews, 199, 102955.

    Google Scholar

  • Li, J., Wang, X., Ruan, C., Sagoe, G., & Li, J. (2022a). Enrichment mechanisms of lithium for the geothermal springs in the southern Tibet China. Journal of Hydrology, 612, 128022.

    CAS  Google Scholar

  • Li, J., Wang, Y., Zhu, C., Xue, X., Qian, K., Xie, X., & Wang, Y. (2020). Hydrogeochemical processes controlling the mobilization and enrichment of fluoride in groundwater of the North China Plain–ScienceDirect. Science of The Total Environment, 730, 138877.

    CAS  Google Scholar

  • Li, J., Wu, Z., Tian, G., Ruan, C., Sagoe, G., & Wang, X. (2022b). Processes controlling the hydrochemical composition of geothermal fluids in the sandstone and dolostone reservoirs beneath the sedimentary basin in north China. Applied Geochemistry, 138, 105211.

    CAS  Google Scholar

  • Liu, J., Zhou, X., Li, Y., et al. (2023). Relationship between hydrogeochemical characteristics of hot springs and seismic activity in the Jinshajiang fault zone, Southeast Tibetan Plateau. Frontiers in Earth Science, 10, 1015134.

    Google Scholar

  • Lu, R., Xie, W., Liu, B., Zhang, S., Zhu, J., & Lin, W. (2024). Geothermal fluid chemistry and isotope for interpreting the formation of complex geothermal system in the Gonghe Basin, northeastern Tibetan Plateau. Journal of Hydrology, 633, 130813.

    CAS  Google Scholar

  • Mao, H., Wang, G., Shi, Z., Liao, F., & Xue, Y. (2021). Spatiotemporal variation of groundwater recharge in the lower reaches of the Poyang Lake Basin, China: insights from stable hydrogen and oxygen isotopes. Journal of Geophysical Research: Atmospheres, 126(6), e0200JD33760.

    Google Scholar

  • Nan, T., Cao, W., Wang, Z., Gao, Y., Zhao, L., Sun, X., & Na, J. (2023). Evaluation of shallow groundwater dynamics after water supplement in North China Plain based on attention-GRU model. Journal of Hydrology, 625, 130085.

    Google Scholar

  • Qu, S., Zhao, Y., Zhang, K., Wang, J., Li, M., Yang, X., Ren, X., Hao, Y., & Yu, R. (2024a). Multi-isotopes (?D, ?18Owater, 87Sr/86Sr, ?34S and ?18Osulfate) as indicators for groundwater salinization genesis and evolution of a large agricultural drainage lake basin in Inner Mongolia, Northwest China. Science of the Total Environment, 946, 174181.

    CAS  Google Scholar

  • Qu, S., Zhao, Y., Li, M., Zhang, K., Wang, J., Duan, L., Ma, H., Miao, P., & Yu, R. (2024). Spatio-seasonal characteristics and controlling factors of surface water stable isotope values (?18O and ?D) across the inner Mongolia reaches of the yellow River Basin China implication for hydrological cycle. Journal of Hydrology: Regional Studies., 53, 101843.

    Google Scholar

  • Qu, S., Duan, L., Mao, H., et al. (2023a). Hydrochemical and isotopic fingerprints of groundwater origin and evolution in the Urangulan River basin, China’s Loess Plateau. Science of the Total Environment., 866, 161377.

    CAS  Google Scholar

  • Qu, S., Duan, L., Shi, Z., Mao, H., Wang, G., Liu, T., Yu, R., & Peng, X. (2022). Identifying the spatial pattern, driving factors and potential human health risks of nitrate and fluoride enriched groundwater of Ordos Basin, Northwest China. Journal of Cleaner Production, 376, 134289.

    CAS  Google Scholar

  • Qu, S., Liang, X., Liao, F., Mao, H., Xiao, B., Duan, L., Shi, Z., Wang, G., & Yu, R. (2023b). Geochemical fingerprint and spatial pattern of mine water quality in the Shaanxi-Inner Mongolia Coal Mine Base, Northwest China. Science of the Total Environment, 854, 158812.

    CAS  Google Scholar

  • Sayed, E. T., Wilberforce, T., Elsaid, K., Rabaia, M. K. H., Abdelkareem, M. A., Chae, K.-J., & Olabi, A. G. (2021). A critical review on environmental impacts of renewable energy systems and mitigation strategies: Wind, hydro, biomass and geothermal. Science of the Total Environment, 766, 144505.

    CAS  Google Scholar

  • Soltani, M., Moradi Kashkooli, F., Souri, M., Rafiei, B., Jabarifar, M., Gharali, K., & Nathwani, J. S. (2021). Environmental, economic, and social impacts of geothermal energy systems. Renewable and Sustainable Energy Reviews, 140, 110750.

    Google Scholar

  • Sun, D., Li, J., Li, H., Liu, Q., Zhao, S., Huang, Y., Wu, Q., & Xie, X. (2022). Evolution of groundwater salinity and fluoride in the deep confined aquifers of Cangzhou in the North China plain after the South-to-North Water Diversion Project. Applied Geochemistry, 147, 105485.

    CAS  Google Scholar

  • Wang, J., Liu, C., Chen, Z., Zhang, Z., Zhang, F., & Zhang, S. (2024a). Geochemical characterization and implications of soil gas and geothermal fluids in the fault zone of Xiongan new area. Applied Geochemistry, 161, 105886.

    CAS  Google Scholar

  • Wang, L., Liu, K., Ma, Y., Zhang, Y., Tong, J., Jia, W., Zhang, S., & Sun, J. (2024b). Geochemical and isotopic techniques constraints on the origin, evolution, and residence time of low-enthalpy geothermal Water in Western Wugongshan, SE China. Acta Geologica Sinica–English Edition, 98, 801–818.

    CAS  Google Scholar

  • Wang, M., Su, C., Wang, X., Jiang, J., Ren, F., & Liu, H. (2024c). Spatial pattern, hydrogeochemical controlling processes and non-carcinogenic risks of fluoride-enriched groundwater in the North Henan Plain. Northern China. Applied Geochemistry, 163, 105934.

    CAS  Google Scholar

  • Wang, Y. Y., Cao, W. G., Pan, D., Wang, S., Ren, Y., & Li, Z. Y. (2022). Distribution and origin of high arsenic and fluoride in groundwater of the North Henan Plain (In Chinese). Rock and Mineral Analysis., 41(6), 1095–1109.

    CAS  Google Scholar

  • Wei, W., Aeschbach-Hertig, W., & Chen, Z. (2015). Identification of He sources and estimation of He ages in groundwater of the North China Plain. Applied Geochemistry, 63, 182–189.

    CAS  Google Scholar

  • Wu, G. W., Li, H. L., Wang, Q. B., Gu, S., Guo, Z. F., & Liu, Z. Y. (2023). Mobilization mechanisms of high fluorine and iodine groundwater in the Northwest Shandong plain (In Chinese). Rock and Mineral Analysis., 42(4), 793–808.

    CAS  Google Scholar

  • Xiao, Y., Hao, Q., Zhang, Y., Zhu, Y., Yin, S., Qin, L., & Li, X. (2022). Investigating sources, driving forces and potential health risks of nitrate and fluoride in groundwater of a typical alluvial fan plain. Science of the Total Environment, 802, 149909.

    CAS  Google Scholar

  • Yang, N., Wang, G., Hou, E., Guo, L., Xiong, L., & Song, X. (2024). Triple isotopes (?D, ?18O, ?17O) characteristic of river water and groundwater in an arid watershed from Qaidam Basin, Northwestern China: Implications for hydrological cycle. Science of The Total Environment., 927, 172229.

    CAS  Google Scholar

  • Zhang, H., Jiang, X.-W., Li, G., Ji, T.-T., Wang, X.-S., Wan, L., & Guo, H. (2023a). Geological carbon cycle in a sandstone aquifer: Evidence from hydrochemistry and Sr isotopes. Journal of Hydrology, 617, 128913.

    CAS  Google Scholar

  • Zhang, L., Chen, S., & Zhang, C. (2019). Geothermal power generation in China: Status and prospects. Energy Science & Engineering, 7(5), 1428–1450.

    Google Scholar

  • Zhang, L., Dong, D., Lv, S., Ding, J., Yan, M., & Han, G. (2023b). Spatial evolution analysis of groundwater chemistry, quality, and fluoride health risk in southern Hebei Plain China. Environmental Science and Pollution Research, 30(21), 61032–61051.

    CAS  Google Scholar

  • Zhang, L., Guo, L., Zhou, X., Yang, Y., Shi, D., & Liu, Y. (2021). Temporal variations in stable isotopes and synchronous earthquake-related changes in hot springs. Journal of Hydrology, 599, 126316.

    CAS  Google Scholar

  • Zhang, S., Shi, Z., Wang, G., Zhang, Z., & Guo, H. (2023c). The origin of hydrological responses following earthquakes in a confined aquifer: Insight from water level, flow rate, and temperature observations. Hydrology and Earth System Sciences, 27(2), 401–415.

    Google Scholar

  • Zhang, S., Liu, K., Ma, Y., Wang, L., & Sun, J. (2024a). Identifying the hydrochemical characteristics, genetic mechanisms and potential human health risks of fluoride and nitrate enriched groundwater in the Tongzhou District, Beijing, North China. Acta Geologica Sinica–English Edition, 98, 468–476.

    CAS  Google Scholar

  • Zhang, S., Liu, K., Yu, C., Deng, Y., Zhang, Y., & Jia, W. (2024b). Identifying the genetic mechanism of medium–low temperature fluoride-enriched geothermal groundwater by the self-organizing map and evaluating health risk in the Wugongshan area, southeast China. Environmental Geochemistry and Health, 46, 274.

    CAS  Google Scholar

  • Zhang, S., Liu, K., Wang, L. Y., Zhu, W., Deng, Y. F., & Yu, C. H. (2024c). Identifying the hydrochemical characteristics and genetic mechanism of medium-low temperature fluoride-enriched geothermal groundwater in the Hongjiang-Qianshan fault of Jiangxi Province (In Chinese). Rock and Mineral Analysis., 43(4), 568–581.

    CAS  Google Scholar

  • Zhang, X., Chen, J., Chen, J., Ma, F., & Wang, T. (2022). Lake expansion under the groundwater contribution in Qaidam Basin. China., 14(7), 1756.

    Google Scholar

ABSTRACT ONLINE AT https://link.springer.com/article/10.1007/s10653-025-02623-5