Natural waters usually demonstrate the disturbance of radioactive equilibrium between parent 238U and and daughter 234U (usually, 234U/238U ≈ 0.8–3 in activities). The ratio of 234U/238U > 10 found in groundwaters can be explained by climatic variations, and it is result of 234U accumulation in permafrost rocks during cold periods and its more rapid loss compared to 238U during thawing. We tested this hypothesis for data on uranium isotope composition in water, and also chemo- and biogenic formations of the World Ocean. Most significant enrichment in 234U is discovered in the northern and internal seas during climatic warmings, which is consistent with an inferred influence of the permafrost formation and degradation on the anomalous increase of 234U/238U in groundwaters. Sampling of the Barents Sea shows that the uranium-234 enrichment in oceanic water increases with increase (a) of isolation from oceanic circulation system, (b) of the relative length of the coastal line, (c) and the contribution of continental waters to the chemical balance of the basin.
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R. F. Anderson, H. Cheng, R. L. Edwards, M. Q. Fleisher, C. T. Hayes, K.-F. Huang, D. Kadko, P. J. Lam, W. M. Landing, Y. Lao, Y. Lu, C. I. Measures, S. B. Moran, P. L. Morton, D. C. Ohnemus, L. F. Robinson, and R. U. Shelley, “How well can we quantify dust deposition to the ocean?” Phil. Trans. R. Soc. A. 374, 20150285 (2016).
M. F Arndt, and L. West, “A Study of the factors affecting the gross alpha measurement, and a radiochemical analysis of some groundwater samples from the state of Wisconsin exhibiting an elevated gross alpha activity, Wisconsin Groundwater Management Practice Monitoring Pproject, DNR–176. (2004).
E. Bard, B. Hamelin, and R. G. Fairbanks “U-Th ages obtained by mass spectrometry in corals from Barbados: sea level during the past 130.000 years,” Nature 346, 456–458 (1990).
E. Bard, R. G. Fairbanks, B. Hamelin, A. Zindler, and C. T. Hoang, “Uranium-234 anomalies in corals older than 150,000 years,” Geochim. Cosmochim. Acta 55, 2385–2390 (1991).
E. Bard, B. Hamelin, M. Arnold, L. Montaggioni, G. Cabioch, G. Faure, and F. Rougerie, “Deglacial sea-level record from Tahiti corals and the timing of global meltwater discharge,” Nature 382, 241–244 (1996).
M. Bar-Matthews, G. J. Wasserburg, and J. H. Chen, “Diagenesis of fossil coral skeletons: correlation between trace elements, textures, and 234U/238U,” Geochim. Cosmochim. Acta 57, 257–276 (1993).
W. S. Broecker, A. Kaufman, and R. M. Trier, “The residence time of thorium in surface sea water and its implications regarding the rate of reactive pollutants,” Earth Planet. Sci. Lett. 20 (1), 35–44 (1973).
G. Cabioch and L. K. Ayliffe, “Raised coral terraces at Malakula, Vanuatu, Southwest Pacific, indicate high sea level during Marine Isotope Stage 3,” Quat. Res. 56, 357–365 (2001).
P. Calsteren van and L. Thomas, “Uranium-series dating applications in natural environmental science,” Earth-Sci. Rev. 75, 155–175 (2006).
F. Chabaux, J. Riotte, and O. Dequincey, “U–Th–Ra fractionations during weathering and river transport,” Rev. Mineral. Geochem. 52 (1), 533–576 (2003).
P. I. Chalov, “U234/U238 isotope ratio in some secondary minerals,” Geokhimiya, No. 2, 165–170 (1959).
P. I. Chalov, Extended Abstracts of Candidate’s Dissertation in Geology and Mineralogy (Alma-Ata, 1954) [in Russian].
P. I. Chalov, Isotope Fractionation of Natural Uranium (Ilim, Frunze, 1975) [in Russian].
P. I. Chalov, Methodical Guide on Uranium–Isotope Modeling of Groundwaters under Active Water-Exchange Conditions (Ilim, Bishkek, 1991) [in Russian].
J. Chappell, A. Omura, T. Esat, M. McCulloch, J. Pandolfi, Y. Ota, and B. Pillans “Reconcilitation of late Quaternary sea levels derived from coral terraces at Huon Peninsula with deep sea oxygene isotope records,” Earth Planet. Sci. Lett. 141, 227–236 (1996).
J. H. Chen, R. L. Edwards, and G. J. Wasserburg, “238U, 234U and 232Th in seawater,” Earth Planet. Sci. Lett. 80, 241–251 (1986).
H. Cheng, J. F. Adkins, R. L. Edwards, and E. A. Boyle, “230Th dating of deep-sea corals,” Geochem. Cosmochim. Acta 64 (14), 2401–2416 (2000).
V. V. Cherdyntsev, “Isotope composition of radioelements in natural objects and their significance in geochronology,” Proc. 3 rd Session of Commission on Determination of Absolute Age of Geological Formations (Moscow, 1955), pp. 175–233 [in Russian].
V. V. Cherdyntsev, Uranium-234 (Atomizdat, 1967) [in Russian]
J. K. Cochran and S. Krishnaswami, “Radium, thorium, uranium and 210Pb in deep–sea sediments and sediment pore waters from the north equatorial Pacific,” Am. J. Sci. 280, 849–889 (1980).
K. Copard, C. Colin, G. M. Henderson, J. Scholten, E. Douville, M.-A. Sicre, and N. Frank Late “Holocene intermediate water variability in the northeastern Atlantic as recorded by deep–sea corals,” Earth and Planet. Sci. Lett. 313–314, 34–44 (2012).
K. B. Cutler, L. R. Edwards, F. W. Taylor, H. Cheng, J. Adkins, C. D. Gallup, P. M. Cutler, G. S. Burr, and A. L. Bloom, “Rapid sea-level fall and deep-ocean temperature change since the last interglacial period,” Earth Planet. Sci. Lett. 206, 253–271 (2003).
K. B. Cutler, S. C. Gray, G. S. Burr, R. L. Edwards, F. W. Taylor, G. Cabioch, J. W. Beck, H. Cheng, and J. Moore, “Radiocarbon calibration and comparison to 50 Kyr BP with paired 14C and 230Th dating of corals from Vanuatu and Papua New Guinea,” Radiocarbon 46, 1127–1160 (2004).
A. N. Dia, A. S. Cohen, R. K. O’Nions, and N. J. Shackleton, “Seawater Sr isotope variation over the past 300 kyr and influence of global climate cycles,” Nature 356, 786–788 (1992).
M. Douarin, M. Elliot, S. R. Noble, D. Sinclair, L.‑A. Henry, D. Long, S. G. Moreton, and J. M. Roberts, “Growth of north–east Atlantic cold–water coral reefs and mounds during the Holocene: a high resolution U–series and 14C chronology,” Earth Planet. Sci. Lett. 375, 176–187 (2013).
E. O. Dubinina, S. A. Kossova and A. Yu. Miroshnikov, “Sources and mechanisms of seawater freshening in Tsivolky and Sedov bays (Novaya Zemlya Archipelago) based on isotope data (δD and δ18O),” Oceanology 59 (6), 836–847 (2019).
R. M. Dunk, R. A. Mills, and W. J. Jenkins, “A reevaluation of the oceanic uranium budget for the Holocene,” Chem. Geol. 190, 45–67 (2002).
A. Dutton, K. Rubin, N. McLean, J. Bowring, E. Bard, R. L. Edwards, G. M. Henderson, M. R. D. Reid, A. Richards, K. W. W. Sims, J. D. Walker, and Y. Yokoyama, “Data reporting standards for publication of U–series data for geochronology and timescale assessment in the earth sciences,” Quat. Geochronol. 39, 142–149 (2017).
M. H. Eisele, The Long–Term Development of Cold–Water Coral Mounds in the NE–Atlantic. Diss. zur Erlangung des Akadem. Grades eines Doktors der Naturwiss (Bremen, 2010).
A. Eisenhauer, G. J. Wasserburg, J. H. Chen, G. Bonani, L. B. Collins, Z. R. Zhu, and K. H. Wyrwoll, “Holocene sea-level determination relative to the Australian continent: U/Th(TIMS) and 14C(AMS) dating of coral cores from the Abrolhos Islands,” Earth Planet. Sci. Lett. 114, 529–547 (1993).
T. M. Esat and Y. Yokoyama, “Correlated uranium and sea-level fluctuations in Late Quaternary oceans,” Goldschmidt–2000, J. Conf. Abstr. 5 (2), 387–388 (2000).
T. M. Esat and Y. Yokoyama, “Variability in the uranium isotopic composition of the oceans over glacial–interglacial timescales,” Geochim. Cosmochim. Acta 70, 4140–4150 (2006).
T. M. Esat, M. T. McCulloch, J. Chappell, B. Pillans, and A. Omura, “Rapid fluctuations in sea level recorded at Huon Peninsula during the Penultimate deglaciation,” Science 283, 197–201 (1999).
C. D. Gallup, R. L. Edwards, and R. G. Johnson, “The timing of high sea levels over the past 200.000 years,” Science 263, 796–800 (1994).
M. Gutjahr, D. Vance, D. L. Hoffmann, C.–D. Hillenbrand, G. L. Foster, J. W. B. Rae, and G. Kuhn, “Structural limitations in deriving accurate U-series ages from calcitic cold–water corals contrasts with robust coral radiocarbon and Mg/Ca systematics,” Chem. Geol. 355, 69–87 (2013).
B. Hamelin, E. Bard, A. Zindler, and R. G. Fairbanks, “234U/238U mass spectrometry of corals: How accurate is the U–Th age of the last interglacial period?” Earth Planet. Sci. Lett. 106, 169–180 (1991).
G. M. Henderson and R. F. Anderson, “The U-series toolbox for paleoceanography,” Rev. Mineral. Geochem. 52 (1), 493–531 (2003).
G. M. Henderson and K. W. Burton, “Using (234U/238U) to assess diffusion rates of isotope tracers in ferromanganese crusts,” Earth Planet. Sci. Lett. 170, 169–179 (1999).
G. M. Henderson, N. C. Slowey, and G. A. Haddad, “Fluid flow through carbonate platforms: constraints from 234U/238U and Cl– in Bahamas pore-waters,” Earth Planet. Sci. Lett. 169 (1–2), 99–111 (1999).
G. M. Henderson, “Seawater (234U/238U) during the last 800 thousand years,” Earth Planet. Sci. Lett. 199 (1–2), 97–110 (2002).
https://data.giss.nasa.gov/. Accessed date, February 10, 2020.
G. P. Kiselev, Even-Numbered Isotopes in Geosphere (UrO RAN, Yekaterinburg, 1999) [in Russian].
J. Kronfeld, “Uranium deposition and Th-234 alpha-recoil: an explanation for extreme U–234/U–238 fractionation within the Trinity aquifer,” Earth Planet. Sci. Lett. 21, 327–330 (1974).
J. Kronfeld and J. C. Vogel, “Uranium isotopes in surface waters from southern Africa,” Earth Planet. Sci. Lett. 105, 191–195 (1991).
J. Kronfeld, E. Gradsztajn, H. W. Müller, J. Radin, A. Yaniv, and R. Zach, “Excess 234U: an aging effect in confined waters,” Earth Planet. Sci. Lett. 27, 342–345 (1975).
T. L. Ku, “An evaluation of the 234U/238U method as a tool for dating pelagic sediments,” J. Geophys. Res. 70 (14), 3457–3474 (1965).
T. L. Ku, K. G. Knauss, and G. G. Mathieu, “Uranium in open ocean: concentration and isotopic composition,” Deep Sea Res. Part II Topical Stud. Oceanogr. 24 (11), 1005–1017 (1977).
M. I. L’vovich, Water and Life (Mysl’, Moscow, 1986) [in Russian].
M. López Correa, P. Montagna, N. Joseph, A. Rüggeberg, J. Fietzke, S. Flögel, B. Dorschel, S. L. Goldstein, A. Wheeler, and A. Freiwald, “Preboreal onset of cold-water coral growth beyond the Arctic Circle revealed by coupled radiocarbon and U-series dating and neodymium isotopes,” Quat. Sci. Rev. 34, 24–43 (2012).
K. R. Ludwig, B. J. Szabo, J. G. Moore, and K. R. Simmons, “Crustal subsidence rate off Hawaii determined from 234U/238U ages of drowned coral reefs,” Geology 19, 171–174 (1991).
K. R. Ludwig, D. R. Muhs, K. R. Simmons, R. B. Halley, and E. A. Shinn, “Sea-level records at ~80 ka from tectonically stable platforms: Florida and Bermuda,” Geology 24 (3), 211–214 (1996).
Method of Measurement of Volume Activity of Uranium Isotopes (238U, 234U, 235U) in samples of natural (fresh and mineralized), Technological, and Sewage Waters by Alpha-Spectrometric Method with Radiochemical Preparation. FR.1.40.2013.15389 (VIMS, Moscow, 2013) [in Russian].
W. S. Moore, “The thorium isotope content of ocean water,” Earth Planet. Sci. Lett. 53 (3), 419–426 (1981).
D. R. Muhs, “The geologic records of dust in the Quaternary,” Aeolian Res. 9, 3–48 (2013).
V. A. Polyakov, “Study of hydrochemical variations and resources of groundwaters of coastal water inlet: isotope data,” Proceedings of All-Union Conference on Hydrogeology (Zvenigorod, 1991), pp. 60–62 [in Russian].
E.-K. Potter, C. H. Stirling, U. H. Wiechert, A. N. Halliday, and C. Spötl, “Uranium–series dating of corals in situ using laser–ablation MC–ICPMS,” Int. J. Mass Spectrometry 240, 27–35 (2005).
D. K. Rea, “The paleoclimatic record provided by eolian deposition in the deep sea: The geologic history of wind,” Rev. Geophys. 32 (2), 159–195 (1994).
G. P. Roberts, S. L. Houghton, C. Underwood, I. Papanikolaou, P. van Calsteren, T. Wigley, F. J. Cooper, and J. M. McArthur, “Localization of Quaternary slip rates in an active rift in 105 years: An example from central Greece constrained by U–234–Th–230 coral dates from uplifted paleoshorelines,” J. Geophys. Res. 114, B1046 (2009).
L. F. Robinson, N. S. Belshaw, and G. M. Henderson, “U and Th isotopes in seawater and modern carbonates from the Bahamas,” Geochim. Cosmochim. Acta 68 (8), 1777–1789 (2004).
A. D. Russell, S. R. Emerson, B. K. Nelson, J. Erez, and D. Lea, “Uranium in foraminiferal calcite as a recorder of seawater uranium concentrations,” Geochim. Cosmochim. Acta 58 (2) 671–681 (1994a).
A. D. Russell, R. L. Edwards, J. A. Hoff, D. McCorkle, and Sayles, “Sediment source of 234U suggested by d234U in North Pacific pore waters. Fall Meeting Supplement,” EOS 75 (44), 332 (1994b).
J. C. Scholten, R. Botz, H. Paetsch, P. Stoffers, and M. Weinelt, “High-resolution uranium-series dating of Norwegian–Greenland Sea sediments: 230Th vs. δ18O stratigraphy,” Marine Geol. 121 (1–2), 77–85 (1994).
Y. Shaked, A. Agnon, B. Lazar, S. Marco, U. Avner, and M. Stein, “Large earthquakes kill coral reefs at the north-west Gulf of Aqaba,” Terra Nova 16, 133–138 (2004).
C.-C. Shen, K.-S. Li, K. Sieh, D. Natawidjaja, H. Cheng, X. Wang, R. L. Edwards, D. D. Lam, Y.-T. Hsieh, T.‑Y. Fan, A. J. Meltzner, F. W. Taylor, T. M. Quinn, H.-W. Chiang, and K. H. Kilbourne, “Variation of initial 230Th/232Th and limits of high precision U-Th dating of shallow-water corals,” Geochim. Cosmochim. Acta 72, 4201–4223 (2008).
R. M. Spratt and L. E. Lisiecki, “A Late Pleistocene sea level stack,” Clim. Past. 12, 1079–1092 (2016).
M. Stein, G. J. Wasserburg, P. Aharon, J. H. Chen, Z. R. Zhu, A. Bloom, and J. Chappell, “TIMS U-series dating and stable isotopes of the last interglacial event in Papua New Guinea,” Geochim. Cosmochim. Acta 57, 2541–2554 (1993).
C. H. Stirling, T. M. Esat, K. Lambeck, and M. T. McCulloch, “Timing and duration of the Last Interglacial: evidence for a restricted interval of widespread coral growth,” Earth Planet. Sci. Lett. 160, 745–762 (1998).
I. D. Streletskaya, A. A. Vasil’ev, G. E. Onblogov, and I. V. Tokarev, “Reconstruction of paleoclimate of the Russian Arctic in the Late Neopleistocene–Holocene based on isotope data on polygonal–vein ices,” Kriosfera Zempli 19 (2), 98–106 (2015).
A. L. Thomas, K. Fujita, Y. Iryu, E. Bard, G. Cabioch, G. Camoin, J. E. Cole, P. Deschamps, N. Durand, B. Hamelin, K. Heindel, G. M. Henderson, A. J. Mason, H. Matsuda, L. Ménabréaz, A. Omori, T. Quinn, S. Sakai, T. Sato, K. Sugihara, Y. Takahashi, N. Thouveny, A. W. Tudhope, J. Webster, H. Westphal, and Y. Yokoyama, “Assessing subsidence rates and paleo water–depths for Tahiti reefs using U–Th chronology of altered corals,” Marine Geol. 295–298, 86–94 (2012).
W. G. Thompson, M. W. Spiegelman, S. L. Goldstein, and R. C. Speed, “An open-system model for U-series age determinations of fossil corals,” Earth Planet. Sci. Lett. 210 (1–2), 365–381 (2003).
W. G. Thompson, H. A. Curran, M. A. Wilson, and B. White, “Sea-level oscillations during the last interglacial highstand recorded by Bahamas corals,” Nature Geosci. Lett. 4, 684–687 (2011).
I. V. Tokarev, “Application of isotope data (δ2H, δ18O, 234U/238U) in studying the permafrost degradation owing to long-term climatic variations,” Zap. Gornoho Inst. 176, 191–195 (2008).
I. V. Tokarev, A. A. Zubkov, V. G. Rumynin, S. P. Pozdnyakov, V. A. Polyakov, and V. Yu. Kuznetsov, “Assessment of the long-term safety of radioactive waste disposal: 1. Paleoreconstruction of groundwater formation conditions,” Water Res. 36 (2), 206–213 (2009a).
I. V. Tokarev, A. A. Zubkov, V. G. Rumynin, and S. P. Pozdnyakov, “Assessment of the long-term safety of radioactive waste disposal: 2. Isotopic study of water exchange in a multilayer system,” Water Res. 36 (3), 345–356 (2009b).
I. V. Tokarev, A. A. Zubkov, V. G. Rumynin, V. A. Polyakov, V. Yu. Kuznetsov, and F. E. Maksimov, “Origin of high 234U/238U ratio in post–permafrost aquifers,” In Uranium in the Environment (Mining Impact and Consequences), Ed. by B. J. Merkel and A. Hasche-Berger (Taylor & Francis, 2006), pp. 847–856.
Uranium–Series Disequilibrium, Ed. By M. Ivanovich and R. S. Harmon, 2nd ed. (Clarendon Press, Oxford, 1992).
Y. Yokoyama and T. M. Esat, “Long term variations of uranium isotopes and radiocarbon in the surface seawater recorded in corals,” In Global Environmental Change in the Ocean and on Land, Ed. by M. Shiyomi H. Kawahata, H. Koizumi, A. Tsuda and Y. Awaya (TERRAPUB, Tokyo, 2004), pp. 279–309.
Y. Yokoyama and T. M. Esat, “Global climate and sea level: Enduring variability and rapid fluctuations over the past 150.000 years,” Oceanography 24 (2), 54–69 (2011).
Y. Yokoyama, T. M. Esat, and K. Lambeck, “Coupled climate and sea-level changes deduced from Huon Peninsula coral terraces of the Last Ice Age,” Earth Planet. Sci. Lett. 193, 579–587 (2001).
S. B. Zykov, G. P. Kiselev, and E. N. Zykova, “New data on uranium-isotope composition of the Barents sea water,” in Radioactivity and Radioactive Elements in the Human Environment, (Tomsk, 2013), pp. 214–217 [in Russian].
E. N. Zykova and S. B. Zykov, “Variations of isotope composition of surface waters of the Severnaya Dvina River,” Privolzhsk. Nauchn. Ts. 5 (69), 25–29 (2017).
We are grateful to O.L. Balakina, the head of the Hydrometeorological Department of the Northern UGMS and chief of the R/V Mikhail Somov expedition, for providing favorable conditions for the performance of research works and uninterrupted attention to our studies. We also thank the captain and crew of the R/V Mikhail Somov for the assistance in solving the problems arising during the expedition.
Expedition works were carried out in the framework of the Transarctica-2019 project.
Analytical works were financially supported by the Russian President Foundation for Support of Young Scientists, project no. МК-1919.2020.5. Data interpretation was supported by the Russian Science Foundation, project no. 20-77-10057.
Translated by M. Bogina
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Tokarev, I.V., Yakovlev, E.Y., Zykov, S.B. et al. Disequilibrium Uranium (234U/238U) in Natural Aqueous Objects and Climatic Variations: World Ocean. Geochem. Int. 59, 895–902 (2021). https://doi.org/10.1134/S001670292109007X
- disequilibrium uranium
- climatic variations
- World Ocean