Nature of radioactivity of quarry drainage waters in the Novosibirsk region

This study is relevant for obtaining the first geochemical data (including information on radionuclides) on the drainage waters of developed and flooded quarries in the eastern areas of the Novosibirsk Region. The objective of the study was to identify the features of the chemical composition of drainage waters (a wide range of chemical elements from Li to U). The study was carried out by titrimetry, ion chromatography and mass spectrometry with inductively coupled plasma in a laboratory setting at the Hydrogeochemical Problem Research Laboratory (PNIL GGH) of the Engineering School of Natural Resources of Tomsk Polytechnic University (IShPR TPU). Measurements of ²²²Rn in waters were carried out at the Alfarad Plus facility of the Laboratory of Siberian Sedimentary Basins Hydrogeology of the A. A. Trofimuk Institute of Petroleum Geology and Geophysics, Siberian Branch of the Russian Academy of Sciences (INGG SB RAS). The data were divided into homogeneous geochemical populations using the coefficients Ca / Na, Ca/ Mg, Ca / Si, Mg/ Si, Na / Si. The chemical composition of the studied objects was found to be highly diverse. The dominant waters have the chemical formula SO₄-HCO₃ / Na-Mg-Ca with a TDS (total dissolved solids) of 400 to 700 mg/dm³. Three geochemical groups of waters were identified. The first is represented by drainage waters of the developed rubble stone quarries, the second includes facilities of the Gorlovka coal basin, and the third refers to abandoned flooded quarries. The first group is characterized by oxidizing conditions with Eh varying over a wide range from +84.6 to +261.0 mV, pH from 6.9 to 8.6, and O_2dissoi_ved from 3.43 to 14.39 mg/dm³. The radionuclide concentrations are (mg/dm³): ²³⁸U 9.30 • 10^-3 - 1,40; ²³²Th 1,00 • 10^-6 - 2,16 • 10^-3; ²²²Rn activity varies from 1 to 572.5 Bq/dm³. The ²³²Th / ²³⁸U ratio ranges from 4.20 • 10^-5 to 2.69 • 10^-3 with an average of 8.40 • 10^-4. The second group has a smaller Eh variation range of +133.2 to +199.6 mV, pH from 7.5 to 8.5, and O_2dissolved from 6.81 to 10.43 mg/dm³. The radionuclide concentrations vary in the following ranges (mg/dm³): ²³⁸U 2.26 • 10^-3 - 2.90 • 10^-2; ²³²Th 7.5 • 10^-6 - 5.57 • 10^-4. The ²³²Th / ²³⁸U ratio ranges from 8.37 • 10^-4 to 4.80 • 10^-2 at an average of 9.54 • 10^-3. The third group is also characterized by an oxidizingizing geochemical environment with Eh +131.3 - +250.0 mV, pH from 6.9 to 8.8 and O_2dissolved from 4.00 to 16.59 mg/dm³. The radionuclide concentrations are (mg/dm³): ²³⁸U 3.00 • 10^-4 - 2.74 • 10^-2; ²³²Th 1.65 • 10^-6 - 1.15 • 10^-5; ²²²Rn activity varies from 2 to 31 Bq/dm³. The ²³²Th/ ²³⁸U ratio ranges from 2.36 • 10^-4 to 1.02 • 10^-3 at an average of 6.25 • 10^-4. Overall, the ²³²Th / ²³⁸U ratio of the studied waters indicates their uranium nature of radioactivity. The data obtained indicate a slight impact of the drainage water discharge from the abandoned quarries on the environment.

1. Posokhov E.V., Tolstikhin N.I. Mineral waters (medicinal, industrial, energy). Leningrad: Nedra Publ.; 1977. 240 p. (In Russ.)

2. Verigo E.K., Bykova V.V., Gusev V.K. Zaeltsovskoye radon water deposit (Novosibirskoye Priobye). In: New data on geology and minerals of Western Siberia. 1979;(14):47–51. (In Russ.)

3. Gusev V.K., Verigo E.K. Radon waters of the Kolyvan-Tomsk folded zone, their use and protection. In: Changes in natural conditions due to human activity. Novosibirsk; 1984. Pp. 99–107. (In Russ.)

4. Chupakov A.V., Pokrovsky O.S., Moreva O.Y. et al. High resolution multi-annual riverine fluxes of organic carbon, nutrient and trace element from the largest European Arctic river, Severnaya Dvina. Chemical Geology. 2020;538:119491. https://doi.org/10.1016/j.chemgeo.2020.119491

5. El-Mezayen A.M., Ibrahim E.M., El-Feky M.G. et al. Physico-chemical conditions controlling the radionuclides mobilisation in various granitic environments. International Journal of Environmental Analytical Chemistry. 2022;102(4):970–986. https://doi.org/10.1080/03067319.2020.1729758

6. Zhao C., Zhang P., Li X. et al. Distribution characteristics and influencing factors of uranium isotopes in saline lake waters in the northeast of Qaidam basin. Minerals. 2020;10(1):74. https://doi.org/10.3390/min10010074

7. Yu C., Berger T., Drake H. et al. Geochemical controls on dispersion of U and Th in Quaternary deposits, stream water, and aquatic plants in an area with a granite pluton. Science of the Total Environment. 2019;663:16–28. https://doi.org/10.1016/j.scitotenv.2019.01.293

8. Faraj T., Ragab A., Alfy M.E. Geochemical and hydrogeological factors influencing high levels of radium contamination in groundwater in arid regions. Environmental Research. 2020;184:109303. https:// doi.org/10.1016/j.envres.2020.109303

9. Krall L., Auqué-Sanz L., Garcia-Orellana J. et al. Radium isotopes to trace uranium redox anomalies in anoxic Groundwater. Chemical Geology. 2019;531:119296. https://doi.org/10.1016/j.chemgeo.2019.119296

10. Ogawa Y., Ishiyama D., Shikazono N. et al. Fractionation of rare earth elements (REEs) and actinides (U and Th) originating from acid thermal water during artificial and natural neutralization processes of surface waters. Geochimica et Cosmochimica Acta. 2019;249:247–262. https://doi.org/10.1016/j.gca.2019.01.030

11. Ram R., Vaughan J., Etschmann B., Brugger J. The aqueous chemistry of polonium (Po) in environmental and anthropogenic processes. Journal of Hazardous Materials. 2019;380:120725. https://doi. org/10.1016/j.jhazmat.2019.06.002

12. Vosel Y.S., Melgunov M.S., Vosel S.V. et al. Isotopic-geochemical evidence of authigenic U(IV)-phases existence in carbonate lake sediments. In: Radioactivity and Radioactive Elements in the Human Environment. Materials of the V International Conference. September 13–16, 2016, Tomsk, Russia. Pp. 167–172. (In Russ.)

13. Ivanov A.Y., Arbuzov S.I.Geochemistry of uranium and thorium in bottom sediments of small artificial water reservoirs and lakes in the south of the Tomsk region. Bulletin of the Tomsk Polytechnic University. Geo Аssets Engineering. 2019;330(4):136–146. (In Russ.) https://doi.org/10.18799/24131830/2019/4/233

14. Zelenin V.I., Saduakasova A.T., Samoilov V.I. et al. Method for uranium extraction from diluted solutions and natural waters. Mining Information and Analytical Bulletin. 2016;(9):252–258. (In Russ.)

15. Samoylov V.I., Saduakasova A.T., Zelenin V.I., Kulenova N.A. The study of uranium sorption extraction from lake water by using natural sorptive mediums and products of their modification. Mining Information and Analytical Bulletin. 2016;(4):283–291. (In Russ.)

16. Isupov V.P., Kolpakova M.N., Borzenko S.V. et al. Uranium in brine lakes of the Altai Territory. Proceedings of the Academy of Sciences. 2016;470(5):566–569. (In Russ.) https://doi.org/10.7868/ S086956521629020X (In Russ.)

17. Tashekova A.Zh., Lukashenko S.N., Koygeldinova M.T., Mukhamediyarov N.Zh. Characteristic of element structure of water r. Shagan. Bulletin of KrasGAU. 2016;12:141–146. (In Russ.)

18. Mazukhina S.I., Pozhilenko V.I., Masloboev V.A. et al. The formation of the chemical composition of groundwater in south prohibiny using the example of “Predgorny” water intake. Bulletin of MSTU. 2018;21(1):88–98. (In Russ.) https://doi.org/10.21443/1560-9278-2018-21-1-88-98

19. Yakovlev E.Yu., Kiselev G.P., Druzhinin S.V., Zykov S.B. Uranium isotopic fractionation (234U, 238U) in the formation of ice crystals. Vestnik Severnogo (Arkticheskogo) Federal’nogo Universiteta. Ser.: Estestvennye nauki. 2016;(3):15–23. (In Russ.) https://doi.org/10.17238/issn2227-6572.2016.3.15

20. Zykova E.N. Establishment of the basis for conducting monitoring studies of uranium isotopes at the lake Kudmozero. In: Lukina L.I., Bezhina N.A., Lyamina N.V. (eds.) International Scientific and Practical Conference “Environmental, Industrial and Energy Security”. September 24–27, 2018, Arkhangelsk, Russia. P. 474–476. (In Russ.)

21. Zykova Е.N., Zykov S.B., Yakovlev Е.Yu., Larionov N.S. Evolutionary isotopes of uranium in surface waters of the group of small lakes of the northwest of the Arkhangelsk region. Advances in Current Natural Sciences. 2018;(4):114–120. (In Russ.) URL: https://s.natural-sciences.ru/pdf/2018/4/36734.pdf

22. Chernyshev I.V., Golubev V.N., Chugaev A.V. et al. Behavior of the 238U, 235U, and 234U isotopes at weathering of volcanic rocks with u mineralization: a case study at the Tulukuevskoe deposit, Eastern Transbaikalia. Petrology. 2019;27(4):446–467. (In Russ.) https://doi.org/10.31857/S0869-5903274446-467

23. Doynikova O.A., Tarasov N.N., Kartashov P. M. Uranium mineralization of Vitim paleovalleys deposits. Prospect and Protection of Mineral Resources. 2018;(12):24–30. (In Russ.)

24. Shkil I.E., Porshnev A.I., Malov A.I. Hydro-geo-ecological conditions changing under pits drainage of the southern group of tubes in the M.V. Lomonosov deposit. Problems of Subsoil Use. 2016;(3):105–114. (In Russ.) https://doi.org/10.18454/2313-1586.2016.03.105

25. Novikov D.A., Dultsev F.F., Kamenova-Totzeva R.M., Korneeva T.V. Hydrogeological conditions and hydrogeochemistry of radon waters in the Zaeltsovsky-Mochishche zone of Novosibirsk, Russia. Environmental Earth Sciences. 2021;80:216. https://doi.org/10.1007/s12665-021-09486-w

26. Novikov D.A., Kopylova Yu.G., Vakulenko L.G. et al. Isotope geochemical features of occurrence of low-radon waters “Inskie Springs” (South-Western Siberia). Bulletin of the Tomsk Polytechnic University. Geo Аssets Engineering. (In Russ.) 2021;332(3):135–145. https://doi.org/10.18799/24131830/2021/03/3108

27. Novikov D.A., Dultsev F.F., Maksimova A.A. et al. Initial results of the integrated isotopehydrogeochemical studies of the Novobibeevo occurrence of radon-rich waters. Bulletin of the Tomsk Polytechnic University.Geo Аssets Engineering. 2022;333(1):57–72. (In Russ.) https://doi.org/10.18799/24131830/2022/1/3447

28. Novikov D.A., Dultsev F.F., Sukhorukova A.F. et al. Monitoring of radionuclides in the natural waters of Novosibirsk, Russia. Groundwater for Sustainable Development. 2021;15:100674. https://doi.org/10.1016/j. gsd.2021.100674

29. Babin G.A., Chernykh A.I., Golovina A.G. et al. State geological map of the Russian Federation. Scale 1:1000000 (third generation). Altai-Sayan series. Sheet N-44 – Novosibirsk. Explanatory letter. St. Petersburg: Cartographic factory VSEGEI; 2015. 392 p. URL: https://www.geokniga.org/sites/geokniga/files/mapcomments/ n-44-novosibirsk-gosudarstvennaya-geologicheskaya-karta-rossiyskoy-federacii-t.pdf

30. Nebera T.S. Typomorphism of rock-forming minerals as an indicator of the evolution of the melt and the physicochemical conditions of the Kolyvan-Tomsk folded zone granitoid formation. [Abstract Dis. Cand. Geol.-Min. Sciences]. Tomsk: Tomsk Polytechnic University; 2010. 23 p. (In Russ.)