Behavior Of Radionuclides Research Articles

Species-specific trends of plutonium, radiocesium, and potassium-40 levels in three fish species of the Yenisei river (Siberia, Russia)

The Yenisei is the largest river in the Northern Hemisphere receiving controlled radioactive discharges from nuclear facilities. The paper presents a comparative study of temporal trends of artificial radionuclides plutonium (239,240Pu) and radiocesium (137Cs), and a natural isotope of the essential macronutrient potassium (40K) in samples of three commercial fish species (Northern pike, Baikal grayling, and Siberian dace) occupying different positions in a trophic network in the Yenisei River (Siberia, Russia). Samples of fish were caught in the Yenisei in 2011–2020 during a period of significant changes in controlled radioactive releases into the river. The study has shown no increase in plutonium concentration in fish samples within two years after the upsurge in controlled Pu discharge into the river (2018–2020). Average activity concentration of 239,240Pu (mBq∙kg−1 d.w., range, mean ± sd) in muscle of grayling (0.6–31.8, 10.9 ± 8.6) was higher (p < 0.01) than in muscle of dace (1.0–4.4, 2.4 ± 1.2) and pike (1.1–11, 3.8 ± 2.9). This can be attributed to the feeding of grayling on benthic invertebrates rich in Pu. The concentration of Pu tended to increase in muscle of pike with the increasing size of the fish. Average activity concentration of 137Cs (Bq∙kg−1 d.w., range, mean ± sd) in muscle of pike, a piscivorous fish (1.8–23.4, 7.7 ± 5.1), was significantly higher (p < 0.001) than the average activity concentration of 137Cs in muscle of dace (0.7–5.7, 2.7 ± 1.6) and grayling (1.3–7.2, 2.5 ± 1.7). A similar effect was revealed for 40K. This can be attributed to biomagnification of 137Cs and 40K in food chains. The results will draw a baseline for assessment of dose-dependent ecological risks for wild fish itself and fish consumers, add field-based facts to the fundamental knowledge of behavior of artificial radionuclides in freshwater food chains, and suggests a hypothesis for consequent experimental studies.

Distribution and in situ bioaccumulation test of radioecologically relevant metals in boreal freshwater sediments

Sediments act as important sinks for metals and their radionuclides in aquatic environments and play a crucial role in their transfer and uptake to aquatic organisms. Traditional radioecological models use radionuclide concentrations in water to predict concentrations in aquatic organisms. In this study, we investigated the distribution of radioecologically important metals (Ba, Co, Ni, Sr, U) among sediment, porewater and hypolimnion over seasons. We also studied the uptake of these metals to benthic organisms and importance of sediment as an uptake source by conducting a 28-day in situ bioaccumulation experiment with oligochaete worms (Lumbriculus variegatus). The studied metals were chosen based on common occurrence of their radioactive isotopes in nuclear fuel cycle. Measurements of total elemental concentration were used as proxies to study the behavior of specific radionuclides. Sediment and water samples were collected from two small lakes connected to a former uranium mine in Eastern Finland, and from a nearby reference lake connected to a different drainage area. Environmental characteristics and concentrations measured from sediment, porewater and overlying water indicated only minor changes between seasons. Measured metals were highly associated with sediment particles, rather than porewater or hypolimnion. Both the distribution of metals and in situ experiment indicated the importance of sediment as the main source of bioaccumulation. Significant differences in Ba, Ni and U concentrations between treatments containing contaminated sediment and reference sediment were noted, regardless of water concentrations. Additionally, as U contaminated lakes lacked seasonal overturn during our monitoring period, metal distribution and environmental conditions remained unchanged in deeper parts of those lakes. Lastly, the results of this in situ bioaccumulation experiment are in line with the findings of our previous laboratory study using sediments from these same lakes.

Natural radionuclide and &lt;sup&gt;137&lt;/sup&gt;Cs activity concentration in soils of the Brazilian State of Sergipe and their correlation with environmental characteristics

Radionuclides occur naturally in the environment, exposing living organisms to ionizing radiation. In addition, human activities have introduced artificial radionuclides such as 137Cs, among others, into the environment. To better understand the occurrence and behaviour of radionuclides in soil, several countries have developed radiological studies and constructed maps. An effort has been made in Brazil to assess the radioactivity in the soils of the country. In this study, the activity concentrations of natural radionuclides 40K, 226Ra and 228Ra, and artificial 137Cs were determined in samples at a depth of 20 cm collected from the soils of the Brazilian State of Sergipe, in a regular grid of 25 km x 25 km. Samples were analysed by gamma-ray spectrometry with the use of hyperpure germanium detectors. The results were correlated with the type of soil, geology, and climate characteristics of the State. The median activity concentrations of 40K, 226Ra, and 228Ra were 210.4 Bq.kg-1, 12.33 Bq.kg-1, and 18.69 Bq.kg-1, respectively. The results are lower than those reported for soils from other Brazilian States in the same region. The activity concentration of 137Cs was lower than the minimum detectable activity. The activity concentration of 40K in young soils of the semi-arid region was higher than that found in most weathered soils of the rainy regions due to the very low pluviometry of the semi-arid area. Higher activity levels of 226Ra were found in Planosol and for 228Ra it was found in the weathered soils (Acrisol) of the coastal zone. Maps of the distribution of the studied radionuclides were designed. The median value of the outdoor absorbed dose rate in air (Dnat) calculated for the soils of the State of Sergipe is lower when compared with other Brazilian States and the UNSCEAR’s worldwide median value.

Distribution coefficient prediction using multimodal machine learning based on soil adsorption factors, XRF, and XRD spectrum data

The distribution coefficient (Kd) plays a crucial role in predicting the migration behavior of radionuclides in the soil environment. However, Kd depends on the complexities of geological and environmental factors, and existing models often do not reflect the unique soil properties. We propose a multimodal technique to predict Kd values for radionuclide adsorption in soils surrounding nuclear facilities in Republic of Korea. We integrated and trained three sub-networks reflecting different data domains: soil adsorption factors for physicochemical conditions, X-ray fluorescence (XRF) data, and X-ray diffraction (XRD) spectra for inherent soil properties. Our multimodal model achieved high performance, with a coefficient of determination (R2) of 0.84 and root mean squared error (RMSE) of 0.89 for natural log-transformed Kd. This is the first study to develop a multimodal model that simultaneously incorporates inherent soil properties and adsorption factors to predict Kd. We investigated influential peaks in XRD spectra and also revealed that pH and calcium oxide (CaO) were significant variables in soil adsorption factors and XRF data, respectively. These results promote the use of a multimodal model to predict Kd values by integrating data from different domains, providing a cost-effective and novel approach to elucidate the mechanisms of radionuclide adsorption in soil.

Sorption of Cs+ and Eu3+ onto coherent and melange-type pre-neogene sedimentary rocks

ABSTRACT Widely present in Japan’s deep subterranean formations, pre-Neogene sedimentary rocks offer an option for high-level radioactive waste (HLW) deep geological disposal due to their favorable properties. However, their barrier properties necessitate further investigation. This research examines the characteristics of pre-Neogene sedimentary rocks, focusing on two rock types: the melange type with a distinct block-in-matrix structure and the sandstone-dominant coherent type. Their ability and mechanism to sorb Cs+ and Eu3+ are assessed, and the differences between the two types are compared. The influence of inorganic carbon in groundwater and the role of clay minerals, such as illite, in the sorption of these metal ions, are highlighted. This investigation lays the groundwork for future studies on migration behaviors of radionuclides, essential for ensuring the long-term safety of HLW geological disposal.

Adsorption Behavior of Co2+, Ni2+, Sr2+, Cs+, and I- by Corrosion Products α-FeOOH from Typical Metal Tanks.

Throughout the nuclear power production process, the disposal of radioactive waste has consistently raised concerns about environmental safety. When the metal tanks used for waste disposal are corroded, radionuclides seep into the groundwater environment and eventually into the biosphere, causing significant damage to the environment. Hence, investigating the adsorption behavior of radionuclides on the corrosion products of metal tanks used for waste disposal is an essential component of safety and evaluation protocols at disposal sites. In order to understand the adsorption behavior of important radionuclides 60Co, 59Ni, 90Sr, 135Cs and 129I on α-FeOOH, the influences of different pH values, contact time, temperature and ion concentration on the adsorption rate were studied. The adsorption mechanism was also discussed. It was revealed that the adsorption of key nuclides onto α-FeOOH is significantly influenced by both pH and temperature. This change in surface charge corresponds to alterations in the morphology of nuclide ions within the system, subsequently impacting the adsorption efficiency. Sodium ions (Na+) and chlorate ions (ClO3-) compete for coordination with nuclide ions, thereby exerting an additional influence on the adsorption process. The XPS analysis results demonstrate the formation of an internal coordination bond (Ni-O bond) between Ni2+ and iron oxide, which is adsorbed onto α-FeOOH.

Reactivity and bioconcentration of stable cesium in a hyperturbid fluvial-estuarine continuum: A combination of field observations and geochemical modeling

Effective, post-accidental management needs an accurate understanding of the biogeochemical behavior of radionuclides in surface environments at a regional scale. Studies on stable isotopes (element homologs) can improve this knowledge. This work focuses on the biogeochemical behavior of stable cesium (Cs) along a major European fluvial-estuarine system, the Gironde Estuary (SW France). We present results obtained from (i) a long-term monitoring (2014–2017) of dissolved (Csd) and particulate (Csp) Cs concentrations at five sites along the freshwater continuum of the Garonne watershed, (ii) Csd and Csp concentrations during four oceanographic campaigns at contrasting hydrological conditions along longitudinal profiles of the estuarine system, (iii) a 24 h cycle of Csp at the estuary mouth, and (iv) a historical trend of Cs bioconcentration in wild oysters at the estuary mouth (RNO/ROCCH, 1984–2017). In addition, we model the partitioning of Cs within the estuarine environment for clay mineral interactions via PhreeqC. At fluvial sites, we observe a geogenic dependence of the Csp and a seasonal variability of Csd, with a downstream increase of the solid-liquid partitioning (log10 Kd values from 3.64 to 6.75 L kg−1) for suspended particulate matter (SPM) < 200 mg L−1. Along the estuarine salinity gradients, Cs shows a non-conservative behavior where fresh SPM (defined as Cs-depleted particles recently put in contact with Csd) act as a Cs sink during both flood and low discharge (drought) conditions. This sorption behavior was explained by the geochemical model, highlighting the relevance of ionic strength, water and SPM residence times. However, at high salinities, the overall log10 Kd value decreases from 6.02 to 5.20 for SPM ∼300–350 mg L−1 due to the Csd oceanic endmember. Despite wild oysters showing low bioconcentration factors (∼1220 L kg−1) at the estuary mouth, they are sensitive organisms to Cs fluxes.

Evaluation of Physico-Chemical Characteristics of Cement Superplasticizer Based on Polymelamine Sulphonate.

Cementitious materials are used to construct an engineered barrier in repositories for radioactive waste. The cement matrix may contain a variety of organic compounds, some of which are polymeric admixtures used as plasticizers. Superplasticizers (SPs) are highly effective organic cement additives for reducing water amount, increasing workability, homogeneity, plasticity and the non-segregation of mortars and grouts, improving mechanical properties and resistance to destructive environments. SPs in cement could have an impact on the long-term safety of the disposals of radioactive waste. These organic agents can leach from the cementitious matrix into groundwater and may affect the migration behaviour of radionuclides. The detailed chemical composition and other characteristics of the cement (CEM I 42.5 R, Sweden) used for the leaching experiments were evaluated. It contained mainly CaO (52.51 ± 1.37, %), and the surface area of the cement particles was 13.2 ± 1.3 m2/g. An insignificant increase in pH (from 12.6 ± 0.1 to 12.8 ± 0.1) was observed for the leachates over 10 days. A commercially available cement superplasticizer based on polymelamine sulphonate (PMS) Peramin SMF10 (Peramin AB, Sweden) was chosen for the research. The product's chemical composition was analysed using wavelength-dispersive X-ray fluorescence (WD-XRF) spectroscopy, while other physico-chemical properties of the PMS superplasticizer were assessed by Raman spectroscopy and thermo-gravimetric analysis. In aqueous solutions and powders of PMS, the same most intensive features were observed at 774 cm-1 (ring out-of-plane deformation), 977 cm-1 (C-N-C bending, SO stretching) and 1055 cm-1 (C-N=C bending) in the Raman spectra. At up to 270 °C, the polymer was thermally stable. Raman and UV/Vis spectroscopies were used to assess the rate of the alkaline degradation of PMS superplasticizer in different aqueous solutions. No changes were observed in the hydrolytic solutions with any of the above analytical methods over a period of 3 years. The results obtained revealed a good thermal and chemical stability (in highly alkaline media, pH = 9.9-12.9) of the PMS polymer.

Study on the behavior of radionuclides in geologic samples from fault zone, Gabal Um Hamd, southwestern Sinai, Egypt

The present study concerned with the activity concentrations of natural radionuclides (238U, 234U, 230Th, 226Ra, 232Th, 40K and, 235U) in ten sedimentary rock samples collected from fault zone, Gabal Um Hamd, southwestern Sinai, Egypt. These samples were investigated to study their behavior during a part of geologic time. The activity concentrations were measured using γ-ray spectrometry (HPGe detector). The investigated samples were analyzed for major oxides using the XRF technique. The results demonstrated high average activity concentrations of 238U, 234U, 230Th, 226Ra, 232Th, 40K and, 235U than the worldwide average values as reported by UNSCEAR 2008. Theil diagram showed that there are accumulation and leaching of uranium in some samples in the two sides of the fault zone. It is noticed that the ages of uranium depositions for the samples collected from the downthrown of the fault zone vary from 121.5 to 440.1 ky, while for the sample collected from the upthrown of the fault is 210.9 ky. The 230Th/232Th activity ratios range between 4.55 and 91.04 for downthrown samples and between 4.75 and 6.05 for upthrown samples which are smaller than 20 except for two samples, indicating a contamination of the samples by detrital 230Th. After subtraction of the detrital 230Th, the corrected ages for downthrown samples vary from 119.1 to 231.7 ky while for upthrown samples vary from 164.4 to 390 ky.

Effects of organic degradation products on the migration behaviour of radionuclides in cementitious materials

The impact of phthalates, which might be present in a cementitious repository as degradation products of superplasticisers or PVC additives, on the migration behaviour of An(III)/Ln(III) was investigated in batch sorption experiments on hardened cement paste. In the absence of organics, An(III)/Ln(III) sorb strongly on HCP with distribution ratios, Rd, of 105 to 106 L kg−1. Above a no-effect level of ~ 10–3 mol L−1 phthalate, a distinct decrease of the An(III)/Ln(III) sorption was observed with sorption reduction factors (i.e., the ratio between the Rd values without and with organic ligand) of 100 to 1000 at phthalate concentrations of 10–1 mol L−1. This sorption reduction is attributed to the effect of Ca complexation with phthalate on the stability of calcium silicate hydrate (C–S–H) phases as main sorbing phase. These results and ongoing diffusion experiments indicate an increase in the mobility of An(III)/Ln(III) in cementitious barriers with increasing phthalate concentrations.Graphical abstract

Efficient uptake of 85Sr and 60Co using fabricated inorganic sorbent for reducing radiation doses of simulated low-level waste

The present study investigated the sorption behavior of 85Sr and 60Co radionuclides from aqueous solutions onto tin molybdate (SnMo) sorbent. SnMo has been synthesized using the precipitation method and was characterized using four analytical techniques including FT-IR, XRD, SEM, and XRF. The sorption studies applied on 85Sr and 60Co include the effect of shaking time, pH, concentration, and saturation capacity. The experimental data revealed that the sorption process was carried out after equilibrium time (180 min). The saturation capacity for 85Sr and 60Co is measured to be 58.1 and 52.2 mg g−1, respectively. The sorption behavior of studied radionuclides is dependent on pH values. Sorption kinetic better fit with the pseudo-second-order model. Furthermore, the sorption isotherm is better represented by the model proposed by Langmuir. The results of the desorption investigations indicated that the most effective eluents for achieving full recovery of investigated radionuclides were identified. Finally, the recycling results demonstrate the suitability of SnMo for affected sorbing of 85Sr and 60Co from aqueous solutions. All the obtained data clarify that the SnMo sorbent is an effective means of removing 85Sr and 60Co from liquid waste.

Predicting the distribution coefficient of cesium in solid phase groups using machine learning

The migration and retention of radioactive contaminants such as 137Cesium (137Cs) in various environmental media pose significant long-term storage challenges for nuclear waste. The distribution coefficient (Kd) is a critical parameter for assessing the mobility of radioactive contaminants and is influenced by various environmental conditions. This study presents machine-learning models based on the Japan Atomic Energy Agency Sorption Database (JAEA-SDB) to predict the Kd values for Cs in solid phase groups. We used three different machine learning models: random forest (RF), artificial neural network (ANN), and convolutional neural network (CNN). The models were trained on 14 input variables from the JAEA-SDB, including factors such as the Cs concentration, solid-phase properties, and solution conditions, which were preprocessed by normalization and log-transformation. The performances of the models were evaluated using the coefficient of determination (R2) and root mean squared error (RMSE). The RF, ANN, and CNN models achieved R2 values greater than 0.97, 0.86, and 0.88, respectively. We also analyzed the variable importance of RF using an out-of-bag (OOB) and a CNN with an attention module. Our results showed that the environmental media, initial radionuclide concentration, solid phase properties, and solution conditions were significant variables for Kd prediction. Our models accurately predict Kd values for different environmental conditions and can assess the environmental risk by analyzing the behavior of radionuclides in solid phase groups. The results of this study can improve safety analyses and long-term risk assessments related to waste disposal and prevent potential hazards and sources of contamination in the surrounding environment.

Geochemical Modeling on Behaviors of Radionuclides (U, Pu, Pd) in Deep Groundwater Environments of South Korea

Geochemical Modeling on Behaviors of Radionuclides (U, Pu, Pd) in Deep Groundwater Environments of South Korea

Computer simulation of thermal processes involving Sr and Ca radionuclides in the process of heating radioactive graphite in an air atmosphere

The paper presents the results from a thermodynamic analysis of the behavior of Sr and Ca radionuclides in the process of heating radioactive graphite in an air atmosphere. The TERRA software package was used for the thermodynamic analysis in a temperature range of 300 to 3600 K to determine the possible composition of the ionized, gaseous and condensed phases. It has been found that strontium is in the form of condensed SrCl2(c) and gaseous SrCl2 in a temperature range of 300 to 1600 K, and in the form of gaseous SrCl2, SrO, SrCl and Sr and ionized SrCl+, Sr+ and SrO+ when the temperature is increased from 1600 to 3600 K. Calcium is in the form of condensed CaCl2(c), CaUO4(c), CaO(c) and gaseous CaCl2 in the temperature interval between 300 and 2100 K, and in the form of gaseous Ca, CaCl and CaO and ionized Ca+, CaO+ and CaCl+ when the temperature is increased from 2100 to 3600 K. The paper determines the key reactions within individual phases and among condensed, gaseous and ionized phases. The equilibrium constants of their reactions have been calculated. Based on the results obtained, dependence plots are presented for the Sr and Ca radionuclide distribution by phases.

A critical review of the quantification, analysis and detection of radionuclides in the environment using diffusive gradients in thin films (DGT): advances and perspectives

Abstract This critical review explores the quantification, analysis, and detection of radionuclides in the environment using the diffusive gradients in thin films (DGT) technique. Radionuclides, unstable isotopes emitting ionising radiation, are present in the environment due to natural and anthropogenic sources for which concerns are raised about their impact on human health and ecosystems. DGT offers a unique passive sampling approach for understanding the behaviour of radionuclides and other trace elements. This review provides insights into method development, real case scenarios, advantages, limitations, and future perspectives of DGT in radionuclide analysis. In terms of method development, various isotopes have been analysed with varying significance based on origin, concentration, risks, and persistence. Notably, U, Th, Pu, Am, Cm, 99Tc, 226Ra, 137Cs, 134Cs, 232U, 237Np, and 152Eu have been measured, revealing their diverse roles in environmental radioactivity. Real case scenarios illustrate applications in uranium mining, water quality monitoring, and metal speciation studies, shedding light on mobility, bioavailability, and ecological impacts. DGT’s advantages include in-situ monitoring, time-averaged mean concentrations, and comprehensive speciation insights. Challenges include potential influences from biofouling, temperature changes and specifically the possible degradation of the binding and diffuse layer due to ionising radiation in long term exposures. In addition, the distinction between fully labile free metal ions and partially labile metal-ligand complexes introduces a potential limitation in the DGT technique, hence being an opportunity for future studies. Looking forward, DGT is expected to contribute to radiation dose modelling, environmental risk assessment, and water quality monitoring, with ongoing developments enhancing its utility and accuracy.

Transfer factors for natural radioactivity into olive mill pomace

The transfer factor (TF) of naturally occurring radioactivity between soil and olive mill pomace (OMP) was calculated in this study. Nine samples were collected from three locations in north Jordan. The study focused on calculating the 226Ra, 232Th, 40K, and 137Cs activity concentrations in both soil and OMP samples using high-purity germanium (HPGe) gamma-ray spectrometry. The average activity levels in the soil samples were determined to be 24.0±10.1, 31.3±9.1, 323.7±68.4, and 1.0±0.4 (Bqkg−1), respectively. In the OMP samples, the average activity levels of 226Ra, 232Th, and 40K were 6.7±1.8, 3.2±1.2, and 185.5±56.6 (Bqkg−1), respectively, while no trace of 137Cs was detected. The activity concentrations of 226Ra, 232Th, and 40K in the soils and OMP samples are within the average worldwide ranges. The calculated values of the TF geometric mean (geometric standard deviation) for 226Ra, 232Th, and 40K were determined to be 0.35 (0.2), 0.11 (0.05), and 0.59 (0.19), respectively. This research offers valuable information about the behavior and movement of radionuclides in the environment.

Sorption Behavior of Radionuclides on Engineered and Natural Barriers and Prediction of Sorption Distribution Coefficients Using Support Vector Regression

A low- and intermediate-level radioactive waste repository contains various types of radionuclides and organic complexing agents. Their chemical interaction within the repository can lead to the formation of radionuclide-ligand complexes, influencing the limited retention behaviors of radionuclides. This study focuses on the sorption behavior of radionuclides on both engineered (concrete) and natural barriers (sedimentary rock and granite), as well as the prediction of sorption distribution coefficients (Kd) using support vector regression. Batch studies were conducted to determine the K d values for three radionuclides (99Tc, 137Cs, and 238U) under different conditions, including pH, temperature, and the presence of organic ligands (such as ethylenediaminetetraacetic acid, nitrilotriacetic acid, and isosaccharinic acid). The K d values for 238U exhibited a sharp decrease with increasing concentrations of organic ligands. In contrast, the K d values for 99Tc showed only a slight reduction at higher organic ligand concentrations. Meanwhile, the K d values for 137Cs remained relatively unchanged, regardless of the type and initial concentration of organic ligands. This suggests a high level of retention for 137Cs in the rock samples. The support vector regression model with a radial basis kernel function proved effective in predicting the K d values under different experimental conditions. This enhancement in predicting accuracy contributes valuable insights into understanding the sorption processes involved in radionuclide behavior. Overall, this study advances our knowledge of radionuclide behavior on both engineered and natural barriers while providing a reliable prediction tool for estimating sorption distribution coefficients.

Geochemical behavior of heavy metals and radionuclides in a pit lake affected by acid mine drainage (AMD) in the Muskau Arch (Poland)

Pit lakes in the ‘anthropogenic lake district’ in the Muskau Arch (western Poland; central Europe) are strongly affected by acid mine drainage (AMD). The studied acidic pit lake, ŁK-61 (pH <3), is also exposed to floods due to its location in the flood hazard area, which may significantly influence the geochemical behavior of elements. The elemental compositions of water and lake sediment samples were measured with ICP–OES and ICP–MS. The sediment profile was also examined for 137Cs and 210Po activity concentrations using gamma and alpha spectrometry, respectively. Grain size distribution, mineralogical composition, diatoms, and organic matter content in the collected core were also determined. The key factors responsible for the distribution of selected heavy metals (e.g., Cu, Ni, Pb, Zn) and radioisotopes (137Cs and 210Po) in the bottom sediments of Lake ŁK-61 are their coprecipitation/precipitation with Fe and Al secondary minerals and their sorption onto authigenic and allogenic phases. These processes are likely driven by the lake tributary, which is an important source of dissolved elements. The data also showed that the physiochemical parameters of Lake ŁK-61 water changed during an episodic depositional event, i.e., the flood of the Nysa Łużycka River in the summer of 2010. The flood caused an increase in the water pH, as interpreted from the subfossil diatom studies. The down-core profiles of the studied heavy metal and radionuclide (HMRs) contents were probably affected by this depositional event, which prevented a detailed age determination of the collected lake sediments with 137Cs and 210Pb dating methods. Geochemical modeling indicates that the flood-related shift in the physicochemical parameters of the lake water could have caused the scavenging of dissolved elements by the precipitation of fresh secondary minerals. Moreover, particles contaminated with HMRs have also possibly been delivered by the river, along with the nutrients (e.g., phosphorus and nitrogen).

Quantitative assessment of the dissociation behavior of Eu(III) with humic acid under varying pH, ionic strength, and pre-equilibrium period using a modified combined dissociation model

Understanding the dissociation behavior of long half-life radionuclides with humic acid (HA) is critical for their migration behavior in aqueous environments. In this study, we developed a modified combined dissociation model comprising three kinetic terms and one constant, representing the concentrations of unbound, fast-dissociating, slow-dissociating, and non-dissociating metals, respectively. For the first time, the modified dissociation model incorporated the contributions of removal kinetics of unbound metals and metal state transformations to the dissociation processes. The modified dissociation model performed well in describing the metal dissociation curves from the view of standard errors of fit calculation and coefficients of determination. Furthermore, this modified dissociation model was employed to quantitatively evaluate the effect of solution pH, ionic strength (I), and pre-equilibrium period of Eu with HA on the dissociation behavior of Eu bound to HA. Results revealed that the fraction of fast-dissociating Eu increased as pH rose, while that of slow-dissociating Eu decreased. The fraction of fast-dissociating Eu was significantly inhibited with increasing I. As the pre-equilibrium period of Eu with HA was prolonged, the fraction of fast-dissociating Eu gradually transformed into the slow-dissociating and non-dissociating Eu.

Investigating the role of Na-bentonite colloids in facilitating Sr transport in granite minerals through column experiments and modeling

Colloids play a crucial role in influencing the mobility of radionuclides in high-level radioactive waste repositories. However, the co-transport behavior of radionuclides and colloids in geological media remains insufficiently understood. This study investigated the transport of Strontium (Sr) in four types of granite minerals (quartz, biotite, K-feldspar, and plagioclase) in the presence and absence of Na-bentonite colloids (Na-BC) using column experiments. Employing a stepwise modeling strategy, this study first determined the basic flow and transport parameters through breakthrough curve analysis of the conservative tracer (Br). Then, the experimental data of Sr in the colloid-free Sr transport experiments and Na-BC in the Sr-colloid co-transport experiments were quantitatively explained using a two-site sorption model and a two kinetic sites model, respectively. Finally, the co-transport behavior of Sr and Na-BC was fitted using the colloid-facilitated solute transport model. The stepwise modeling allowed quantification of the kinetics of Sr sorption onto mobile and immobile Na-BC and highlighted the role of straining in Na-BC retention. In the absence of Na-BC, Sr transport experienced the greatest retardation in biotite, followed by plagioclase, K-feldspar, and quartz, respectively, which positively correlated with the specific surface area of the minerals. Moreover, Na-BC enhanced Sr transport with the same retardation order in all tested minerals, with recovery rate increments of 68.61%, 19.21%, 6.67%, and 4.33%, respectively. The transport of Sr in K-feldspar was found to be less affected by Na-BC compared to the other tested minerals, likely due to the strong cation exchange capacity of K+ among the cation components of minerals, making hydrated K+ more likely to exchange with Sr2+ on K-feldspar surfaces. These findings hold significant implications for assessing the risks associated with the transport of radionuclides in deep geological repositories.