A study of radionuclides, metals and stable lead isotope ratios in sediments and soils in the vicinity of natural U-mineralisation areas in the Northern Territory

Australian guidelines recommend that tailings materials from uranium (U) mining and milling be contained without any detrimental impact on the environment for at least 1000 years. Natural analogue sites are being investigated to determine if they can provide data on the rates of natural erosion processes which occur over these timescales, for input into predictive geomorphic computer models. This paper presents radionuclide, metal and stable lead (Pb) isotope data from sediment cores and surface soils in the vicinity of two mineralised areas in the Alligator Rivers Region.Surface scrapes from the natural Anomaly #2, south of the Ranger mineral lease, exhibit radiogenic ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios, and elevated U and metal concentrations typical for a near surface U anomaly. In contrast, samples taken from the Koongarra mineral lease (KML) show radionuclide activity and metal concentrations similar to natural areas elsewhere in the Alligator Rivers Region and Pb isotope ratios are closer to present day average crustal ratios (PDAC), as the orebodies at KML are covered by surficial sand. A sediment core collected from Anbangbang Billabong, downstream of KML, exhibits small variations in Pb isotope ratios that indicate that approximately 1% of the upper sediments in the sediment core may be derived from material originating from the U anomaly at Koongarra.     

Comprehensive Analysis of Radioactive and Chemical Contamination of Water Bodies in the Area of Radium-Industry Waste Storage

Genotoxicity and cytotoxicity of water samples from the creeks flowing through the area of radium mining waste storage into the Ukhta River and from this river were assessed using biological tests with Allium schoenoprasum L. Chemical analysis of the samples indicated that concentrations of parent heavy natural radionuclides, ²¹⁰Pb, and ²¹⁰Po do not exceed the allowable level. Of ten heavy metals, only Zn and Mn concentrations exceeded MACs. The results of biological tests provided evidence for the significantly increased genotoxicity of water samples. The mitotic index increased with an increase in the concentration of Zn ions and manifested an inverse dependence on the activity of ²³⁸U. The genotoxic effect linearly depended on Zn concentration. Possible mechanisms responsible for the induction of these biological effects are discussed.     

Polonium (210Po) and lead (210Pb) in marine organisms and their transfer in marine food chains

The determination of ²¹⁰Po and ²¹⁰Pb was performed in marine organisms from the seashore to abyssal depths, encompassing a plethora of species from the microscopic plankton to the sperm whale. Concentrations of those radionuclides ranged from low values of about 5 × 10⁻¹ Bq kg⁻¹ (wet wt.) in jellyfish, to very high values of about of 3 × 10⁴ Bq kg⁻¹ (wet wt.) in the gut walls of sardines, with a common pattern of ²¹⁰Po > ²¹⁰Pb.These radionuclides are primarily absorbed from water and concentrated by phyto- and microzooplankton, and then are transferred to the next trophic level along marine food chains. Investigation in epipelagic, mesopelagic, bathypelagic and abyssobenthic organisms revealed that ²¹⁰Po is transferred in the marine food webs with transfer factors ranging from 0.1 to 0.7, and numerically similar to those of the energy transfer in the marine food chains. As ²¹⁰Po preferentially binds to amino acids and proteins, its transfer in food chains likely traces protein transfer and, thus, ²¹⁰Po transfer factors are similar to ecotrophic coefficients. ²¹⁰Pb is transferred less efficiently in marine food chains and this contributes to increased ²¹⁰Po:²¹⁰Pb activity ratios in some trophic levels.     

Radium and radium-daughter nuclides in carbonates: a brief overview of strategies for determining chronologies

Radium isotopes have been used extensively to trace the movement of groundwater as well as oceanic water masses, but these radionuclides (and their daughters) are also useful chronometers for the determination of the time scales of other Earth and environmental processes. The purpose of this overview is to present the application of Ra and Ra daughters in the dating of carbonates. We show that the choice of dating method (decay of excess radionuclide or ingrowth of daughter) depends strongly on the parent/daughter activity ratios in the water in which the carbonate was precipitated. Thus freshly precipitated carbonates uniformly show excesses of ²²⁶Ra relative to its parent ²³⁰Th, and ²²⁶Ra decay can provide ages of carbonates over Holocene time scales. In contrast, carbonates are precipitated in waters of greatly varying ²¹⁰Pb/²²⁶Ra. Corals, deep-sea hydrothermal vent clams and the shelled cephalopod Nautilus live in waters with significant dissolved ²¹⁰Pb and all show excesses of ²¹⁰Pb in their carbonate. Bivalve molluscs from nearshore and coastal waters, and carbonates deposited from groundwater environments (e.g. travertines) in which ²¹⁰Pb is efficiently scavenged from solution, show deficiencies of ²¹⁰Pb relative to ²²⁶Ra. In contrast, fish otoliths strongly discriminate against ²¹⁰Pb regardless of the environment in which the fish lives. Deficiencies of ²²⁸Th relative to ²²⁸Ra are common in all carbonates. Useful time ranges for the ²¹⁰Pb/²²⁶Ra and ²²⁸Th/²²⁸Ra chronometers are ∼100 y and ∼10 y, respectively.     

Solid state speciation and potential bioavailability of depleted uranium particles from Kosovo and Kuwait

A combination of synchrotron radiation based X-ray microscopic techniques (μ-XRF, μ-XANES, μ-XRD) applied on single depleted uranium (DU) particles and semi-bulk leaching experiments has been employed to link the potential bioavailability of DU particles to site-specific particle characteristics. The oxidation states and crystallographic forms of U in DU particles have been determined for individual particles isolated from selected samples collected at different sites in Kosovo and Kuwait that were contaminated by DU ammunition during the 1999 Balkan conflict and the 1991 Gulf war. Furthermore, small soil or sand samples heavily contaminated with DU particles were subjected to simulated gastrointestinal fluid (0.16 M HCl) extractions. Characteristics of DU particles in Kosovo soils collected in 2000 and in Kuwait soils collected in 2002 varied significantly depending on the release scenario and to some extent on weathering conditions. Oxidized U (+6) was determined in large, fragile and bright yellow DU particles released during fire at a DU ammunition storage facility and crystalline phases such as schoepite (UO₃·2.25H₂O), dehydrated schoepite (UO₃·0.75H₂O) and metaschoepite (UO₃·2.0H₂O) were identified. As expected, these DU particles were rapidly dissolved in 0.16 M HCl (84 ± 3% extracted after 2 h) indicating a high degree of potential mobility and bioavailability. In contrast, the 2 h extraction of samples contaminated with DU particles originating either from corrosion of unspent DU penetrators or from impacted DU ammunition appeared to be much slower (20–30%) as uranium was less oxidized (+4 to +6). Crystalline phases such as UO₂, UC and metallic U or U–Ti alloy were determined in impacted DU particles from Kosovo and Kuwait, while the UO_2,34 phase, only determined in particles from Kosovo, could reflect a more corrosive environment. Although the results are based on a limited number of DU particles, they indicate that the structure and extractability of DU particles released from similar sources (metallic U penetrators) will depend on the release scenarios (fire, impact) and to some extent environmental conditions. However, most of the DU particles (73–96%) in all investigated samples were dissolved in 0.16 M HCl after one week indicating that a majority of the DU material is bioaccessible.     

Influence of macroalgal diversity on accumulation of radionuclides and heavy metals in Bulgarian Black Sea ecosystems

Radionuclides and heavy metals were studied in green, brown and red Black Sea macroalgae by low-level gamma spectrometry and atomic absorption spectrometry. The samples were collected along the whole Bulgarian coast from 1996 to 2004. The levels have been depending on algae species, locations and year of sampling. The highest ¹³⁷Cs levels were found in red Ceramium rubrum species from all studied locations, while ²²⁶Ra and ²¹⁰Pb were up to three orders of magnitude higher in Bryopsis plumosa. The data showed that the red algae species (Rhodophyta) accumulate more heavy metals than the other phyla (except for Fe whose values were higher in green algae). The data confirmed that algae are valuable indicators of the environmental contamination. The observed elevated levels were mainly due to Danube, Dnieper and Dnester inputs in the NW corner of the Black Sea.     

210Po in the marine environment with emphasis on its behaviour within the biosphere

The distribution and behaviour of the natural-series alpha-emitter polonium-210 in the marine environment has been under study for many years primarily due to its enhanced bioaccumulation, its strong affinity for binding with certain internal tissues, and its importance as a contributor to the natural radiation dose received by marine biota as well as humans consuming seafoods. Results from studies spanning nearly 5 decades show that ²¹⁰Po concentrations in organisms vary widely among the different phylogenic groups as well as between the different tissues of a given species. Such variation results in ²¹⁰Po concentration factors ranging from approximately 10³ to over 10⁶ depending upon the organism or tissue considered. ²¹⁰Po/²¹⁰Pb ratios in marine species are generally greater than unity and tend to increase up the food chain indicating that ²¹⁰Po is preferentially taken up by organisms compared to its progenitor ²¹⁰Pb. The effective transfer of ²¹⁰Po up the food chain is primarily due to the high degree of assimilation of the radionuclide from ingested food and its subsequent strong retention in the organisms. In some cases this mechanism may lead to an apparent biomagnification of ²¹⁰Po at the higher trophic level. Various pelagic species release ²¹⁰Po and ²¹⁰Pb packaged in organic biodetrital particles that sink and remove these radionuclides from the upper water column, a biogeochemical process which, coupled with scavenging rates of this radionuclide pair, is being examined as a possible proxy for estimating downward organic carbon fluxes in the sea. Data related to preferential bioaccumulation in various organisms, their tissues, resultant radiation doses to these species, and the processes by which ²¹⁰Po is transferred and recycled through the food web are discussed. In addition, the main gaps in our present knowledge and proposed areas for future studies on the biogeochemical behaviour of ²¹⁰Po and its use as a tracer of oceanographic processes are highlighted in this review.     

Bioaccumulation and biological effects in the earthworm Eisenia fetida exposed to natural and depleted uranium

The accumulations of both natural (U) and depleted (DU) uranium in the earthworms (Eisenia fetida) were studied to evaluate corresponding biological effects. Concentrations of metals in the experimental soil ranged from 1.86 to 600 mg kg⁻¹. Five biological endpoints: mortality, animals’ weight increasing, lysosomal membrane stability by measuring the neutral red retention time (the NRRT), histological changes and genetic effects (Comet assay) were used to evaluate biological effects in the earthworms after 7 and 28 days of exposure. No effects have been observed in terms of mortality or weight reduction. Cytotoxic and genetic effects were identified at quite low U concentrations. For some of these endpoints, in particular for genetic effects, the dose (U concentration)-effect relationships have been found to be non-linear. The results have also shown a statistically significant higher level of impact on the earthworms exposed to natural U compared to depleted U.     

Observations and modelling of thoron and its progeny in the soil-atmosphere-plant system

Samples of pasture vegetation, mainly Trifolium pratensis, were collected at the Botanic Garden of the University of Bologna during the period 1998-2000 and measured by gamma-spectrometry for determining thoron progeny. Concentrations of ²¹²Pb were between 1.5 and 20 Bq m⁻², with individual peaks up to 70 Bq m⁻². Soil samples were collected at the same location and physically characterised. Their chemical composition (particularly Th and U) was determined by X-ray fluorescence spectroscopy. Lead-212 on plants mainly originates from dry and wet deposition of this isotope generated in the lower atmosphere by the decay of its short-lived precursor ²²⁰Rn, which is produced in the upper soil layers as a member of the natural thorium decay chain and exhales into the atmosphere. Concentrations of ²²⁰Rn in the atmosphere depend on (1) the amount of Th present in soil, (2) the radon fraction which escapes from the soil minerals into the soil pore space, (3) its transport into the atmosphere, and (4) its redistribution within the atmosphere. The mobility of radon in soil pore space can vary by orders of magnitude depending on the soil water content, thus being the main factor for varying concentrations of ²²⁰Rn and ²¹²Pb in the atmosphere. We present a simple model to predict concentrations of thoron in air and its progeny deposited from the atmosphere, which takes into account varying soil moisture contents calculated by the OPUS code. Results of this model show close agreement with our observations.     

The importance of physico-chemical parameters on the speciation of natural radionuclides in riverine ecosystems

External gamma radiation levels were measured in the catchment areas of the Sharavathi River and the dose rates in air were found to be in the range 26.0-61.0 nGy h⁻¹. Soil and sediment samples of the riverine environment were analysed for natural radionuclides such as ²²⁶Ra, ²³²Th and ⁴⁰K using a NaI(Tl) gamma spectrometer. The activity concentration of ²¹⁰Pb and ²¹⁰Po in soil and sediment samples was determined by radiochemical separation techniques. Evaluation of the activity concentration of radionuclides with grain size revealed an increase in the activity of ²²⁶Ra, ²³²Th and ⁴⁰K towards fine grain size. The activity concentrations for all isotopes in all samples were not significantly correlated with pH. However, the activity of ²¹⁰Po and ²¹⁰Pb in sediment showed a moderate positive correlation with organic matter content and a good correlation with clay content of sediment.     

Bioaccumulation and lack of oxidative stress response in the ragworm H. diversicolor following exposure to Ra in sediment

The main effluent from oil and gas production, produced water, from some platforms in the North Sea contains elevated concentrations of ²²⁶Ra. The aim of this study was to investigate whether ²²⁶Ra in sediment would accumulate in and affect sediment-dwelling organisms. In addition, we wanted to determine if the bioavailability would be modulated by the presence of a scale inhibitor which is used during oil and gas production. Hediste diversicolor was therefore exposed to different levels of ²²⁶Ra (30–6600 Bq kg⁻¹) in combination with scale inhibitor in the sediments in a flow through system. The levels of radioactivity in the exposures were close to levels that can be measured in proximity to oil/gas production facilities. ²²⁶Ra spiked to natural sediment partitioned into pore water and accumulated in the sediment-dwelling polychaete following a four-week exposure period. The results suggest that ²²⁶Ra did not bind strongly to sediment (low sediment:water partitioning coefficient), but it was not shown to bioaccumulate in any great extent (bioaccumulation factors of 0.019–0.022). Exposure of H. diversicolor in sediments with up to 6600 Bq kg⁻¹²²⁶Ra had no measurable effect on the total oxyradical scavenging capacity of the organisms compared to control. So although they accumulated the alpha-emitter, the treatments did not appear to cause oxidative stress in polychaete tissues.     

Polonium-210 in mussels and its implications for environmental alpha-autoradiography

Alpha-autoradiographic and radiochemical studies of the distributions of transuranic nuclides in the tissues and organs of mussels collected from the vicinity of the British Nuclear Fuels plc reprocessing plant at Sellafield, Cumbria, England, appeared to require assessment also of baseline alpha-activities of natural ²¹⁰ Po levels. Results for the latter were found to be in excess of the anthropogenic activities of Pu and Am isotopes. To ensure that the levels of ²¹⁰ Po in Cumbrian mussels were not artificially enhanced by local discharges and in the absence of published data, mussels from remote British and French coastal sites were also analyzed. General similarities in ²¹⁰Po concentrations (111 to 459 Bq kg⁻¹ dry) found in mussels soft parts suggest that the ²¹⁰Po levels in the Ravenglass mussels (279 Bq kg⁻¹) are natural and largely unsupported by ²¹⁰Pb; however these levels are as much as four times greater than the present day ^239+240Pu concentrations in the same samples. As the transuranic nuclide content of Cumbrian mussels produces a major component of the local critical group radiation exposure from the Sellafield discharges, this finding places in some perspective the significance of the baseline natural radionuclide concentrations in generating total exposure of the public. More specifically, these findings severely limit the usefulness of alpha-autoradiographic studies for transuranic nuclides performed on such samples. Because of the recently lower concentrations of alpha-emitting transuranic nuclides (mainly ²³⁸Pu, ^239+240Pu and ²⁴¹Am) in the Ravenglass environment, natural ²¹⁰Po is now a major contributor to alpha-track distributions in autoradiographic studies.     

Common buzzards (Buteo buteo) bio-indicators of heavy metals pollution in Sicily (Italy)

The aim of this study was to evaluate the accumulation of toxic (As, Cd and Pb) and essential (Cu, Mn and Zn) metals in samples (feathers, liver, kidney, lung, intestine and muscle) of common buzzards (Buteo buteo) from Sicily, used as bio-indicators for monitoring environmental metals pollution. All samples of buzzards were collected at the “Recovery Center of Wild Fauna” of Palermo, through the Zooprophilactic Institute. The quantitative determinations of metals were carried out using an atomic absorbtion spectrophotometer (AAS). The results obtained showed the presence of metals in all samples analyzed. For toxic metals the highest levels of Pb and As were found in liver and those of Cd in kidney; for essential metals Zn levels were higher than Cu and Mn in all tissues analyzed. Significant differences are observed in metal levels between female and male and juvenile and adult bird samples.Highest metal levels found in liver, kidney and muscle can be considered indicative of chronic exposure to metals while the presence of metals in feathers can be consequential to storing and elimination processes. The results obtained suggest that common buzzards (Buteo buteo) may be very useful as bio-indicators for monitoring environmental pollution.     

Distributional U, Ra, Pb and Po in soil

A soil profile from 0 to 90 cm was collected in an undisturbeded area of Cape Cod, Massachusetts. Five centimeter increments of the profile were analyzed for ^234,238U, ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po. The factors affecting the activity distribution of these naturally-occurring radionuclides are discussed for this particular soil type.     

Distributional 234,238U, 226Ra, 210Pb and 210Po in soil

A soil profile from 0 to 90 cm was collected in an undisturbeded area of Cape Cod, Massachusetts. Five centimeter increments of the profile were analyzed for ^234,238U, ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po. The factors affecting the activity distribution of these naturally-occurring radionuclides are discussed for this particular soil type.     

Biomonitoring of ²¹⁰Po and ²¹⁰Pb using lichens and mosses around coal-fired power plants in Western Turkey

Mosses and lichens are useful biological indicators of environmental contamination for a variety of metals and radionuclides of both natural and artificial origin. These plants lack a well-developed root system and rely largely on atmospheric deposition for nourishment. Therefore in the study, different lichens (Cladonia convoluta, Cladonia foliacea) and mosses (Homalothecium sericeum, Hypnum lacunosum, Hypnum cupressiforme, Tortella tortuosa, Didymodon acutus, Syntrichia ruralis, Syntrichia intermedia, Pterogonium graciale, Isothecium alopecuroides, Pleurochatae squarrosa) were collected around the Yata?an (Mu?la), Soma (Manisa), Seyitömer - Tunçbilek (Kütahya) coal-fired power plants and investigated for potential use as biomonitors for ²¹⁰Po and ²¹⁰Pb deposition. While the activity concentrations of ²¹⁰Po and ²¹⁰Pb in lichens are in the ranges of 151 ± 7-593 ± 21 and 97 ± 5-364 ± 13 Bq kg⁻¹, for mosses the ranges for ²¹⁰Po and ²¹⁰Pb are 124 ± 5-1125 ± 38 and 113 ± 4-490 ± 17 Bq kg⁻¹, respectively. In the study, the moss samples were observed to accumulate more ²¹⁰Po and ²¹⁰Pb compared to lichens. While the most suitable biomonitor was a moss species (H. lacunosum) for Yata?an (Mu?la), it was another moss species (S. intermedia) for Soma (Manisa) and Seyitömer - Tunçbilek (Kütahya) sites. ²¹⁰Po concentrations were found higher than ²¹⁰Pb concentrations at the all sampling stations.     

Remobilization of trace elements by forest fire in Patagonia,Chile

Temporal changes in the amounts of trace elements (As, Co, Cu, Mn, Ni, Pb, and Zn) and their correlations with temporal changes in charcoal abundance in age-dated sediments collected from Lake Thompson in Patagonia, Chile, attest to the substantial pyrogenic remobilization of contaminants that occurred in Patagonia during the mid-1900s. This remobilization was concurrent with the extensive slash and burn period in the region during that period. The changes in concentrations of Co, Cu, and Ni in relation to charcoal abundance in the lacustrine sediments over time were small compared to those of As, Mn, Pb, and Zn. However, the relatively low enrichment factors of all those trace elements, normalized to Fe, indicate that they were predominantly derived from local, natural sources impacted by fires rather than industrial sources. The primarily local source of Pb in the sediments was corroborated by the temporal consistency of its isotopic ratios (²⁰⁶Pb/²⁰⁷Pb:²⁰⁸Pb/²⁰⁶Pb), which were similar to previously reported values for natural lead in Central and Southern Chile. However, the pyrogenic remobilization of both natural and industrial trace elements by forest fires in Chile and elsewhere is expected to rise as a consequence of climate change, which is projected to increase both the frequency and intensity of forest fires on a global scale.     

Migration of radium from the thorium ore deposit of Morro do Ferro,Poços de Caldas,Brazil

A large thorium ore deposit is located in Morro do Ferro, a hill in the Poços de Caldas Plateau, Minas Gerais, Brazil, which contains an estimated 30 000 t of Th and 100 t of U in a highly weathered matrix exposed to erosion and leaching. ²²⁸Ra and ²²⁶Ra were analyzed in surface waters collected at various points in the drainage basin and in groundwaters from wells drilled through and around the ore body. The concentrations in groundwater demonstrated that radium is markedly leached by rainwater percolating through the ore body. In its transit underground, radium is removed from groundwater by sorption on soil particles and this natural process greatly reduces the radium discharged to the environment. In dry weather, the concentration of dissolved ²²⁸Ra in the main stream draining the Morro do Ferro is 7·0 ± 1·1 mBq litre⁻¹ and in a control stream 1·6 ± 0·3 mBq litre⁻¹. The estimated ²²⁸Ra mobilization rate by solubilizations is of the order of 10⁻⁷ y⁻¹.     

Aspects on the analysis of 210Po

There has been little development regarding analysis of polonium (Po) in environmental samples since the 1960ies. This is due to the straightforward spontaneous deposition of this element on silver (Ag), nickel (Ni) or copper (Cu) without any radiochemical separation. For many years, no radiochemical yield determinant was used and it was generally supposed that the yield was 100% after two depositions. Counting was often done using ZnS scintillation counter coupled to a photomultiplier tube. However, the use of the yield determinants ²⁰⁸Po and ²⁰⁹Po and the development of alpha spectrometry showed that the yield was lower. Furthermore, the tendency of Po to volatilize at low temperatures constrains the sample preparation techniques; dry-ashing cannot be used. But during the wet-ashing procedure, there are still some losses.The aim of this study was to evaluate the Po losses during wet-ashing by the use of a double-tracer technique. We have found that the losses were about 30% when open glass beakers were used and about 17% when the samples were digested in microwave oven. When long-necked bottles (Kjeldahl flasks) were used, a loss of about 20% was registered.It has also been observed that ²¹⁰Pb to some extent is plating out together with its daughter nuclide Po during the electrochemical deposition. This will result in a systematic error since an unknown amount of supported ²¹⁰Po will be produced from the ²¹⁰Pb decay depending on the fraction of ²¹⁰Pb being deposited on the disc and the waiting time between deposition and measurement of the sample. A further consequence of this is that in the assessment of the ²¹⁰Pb content in the sample, very often the remaining liquid is stored after deposition for build-up of ²¹⁰Po. Since some ²¹⁰Pb is lost on the disc, the result for ²¹⁰Pb will be too low. Both these systematic errors give rise to a too high ²¹⁰Po/²¹⁰Pb ratio. The fraction of ²¹⁰Pb which is plating out has been assessed in this study for different matrices and is about 50-90%. During the measurement by solid state Si-detectors, some Po is evaporated in the vacuum conditions contaminating the detectors. Experiments have here been done by heating the discs after deposition which indicate that less Po is evaporated from Ag than from Ni. The losses from Ag are less than that from the other metals probably due to a deeper penetration into the surface of Po. We conclude that in most aspects, Ag is better to use than the other plating metals.     

Radium geochemistry in Na-Cl type groundwater in Niigata Prefecture, Japan

Radium isotopes in 23 Na-Cl type groundwater sampled mainly from deep wells in Niigata Prefecture, which is the site of the largest oil- and gas-fields in Japan, were measured along with U isotopes, chemical components and hydrogen and oxygen isotope ratios to elucidate the distribution and behavior of Ra in a brackish environment underground. Also analyzed were U and Th isotopes in 38 rock samples collected from outcrops at 17 locations. Ra-226 concentrations (8.86-1637 mBq kg⁻¹) of groundwater samples roughly correlated with total dissolved solid (TDS) concentrations and other alkaline earth contents. Their ²²⁸Ra/²²⁶Ra activity ratios (0.32-5.2) were similar to or higher than the ²³²Th/²³⁸U activity ratios (0.6-1.7) in the rocks. The most likely transport mechanism of Ra isotopes into groundwater was due to their α-recoil from the solid phase, probably from the water-rock interface where Th isotopes had accumulated, and adsorption/desorption reaction based on the increase in ²²⁶Ra contents with TDS.