Radioactive iodine released from nuclear power plants has been recognized to pose significant risks and environmental hazards. In response to these challenges, extensive investigations into iodine sorbents have been conducted with a particular focus on the utilization of layered double hydroxides (LDH) as a promising candidate. Herein, we have focused on the investigation of LDH materials featuring diverse transition metals for their synthesis, with specific emphasis on CoAl LDH for its proficiency in removing iodine species, particularly IO3 –. Nevertheless, a comprehensive understanding of the removal mechanisms employed by these LDH materials remained elusive. Hence, the primary aim of this study is to elucidate the intricacies of the removal mechanisms through sorption tests, spectroscopic techniques, and theoretical chemistry analyses, subsequently contrasting the experimental outcomes with computational results. For the experimental facet, the synthesis of CoAl LDH was conducted utilizing 0.15 mol L−1 of Co(NO3)2⋅6H2O and 0.06 mol L−1 of Al(NO3)3⋅9H2O to attain a molar ratio (M2+:M3+) of 2.5:1. Subsequently, pH-dependent IO3 – sorption tests were carried out, coupled with X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopy, facilitating the elucidation and discourse of the removal mechanism. The theoretical chemistry in this research harnessed ab initio molecular dynamics (AIMD) simulations for structural modeling, atomic density profiles, radial distribution function, analysis of oxide species, and MD-EXAFS spectrum analysis. In summary, this study aims to elucidate iodine removal mechanisms using diverse experimental results, culminating in the revelation that ion-exchange with NO3 – present in the interlayer predominates as the principal mechanism for IO3 – removal. Notably, a distinct spectral feature at approximately 33,190 eV emerged, defying identification through XANES and EXAFS analyses conducted under experimental conditions. In the AIMD simulations, meticulous scrutiny of individual iodine atoms uncovered the prevalence of I−O and I−O−H molecular species, marked by interactions between O and H atoms, with a coordination number of I−O = ~3. This transformation was primarily instigated by proton hopping. As a result, the comparative investigation reveals the dominance of IO3 – intercalation in the CoAl LDH material with the potential to undergo a transformation to the I−O−H molecule upon interaction with protons.

The immobilization of low- and intermediate-level radioactive waste (LILW) is crucial for its final disposal in repositories. While cementitious waste forms have conventionally been used for immobilizing various LILWs, they suffer from several issues, including poor durability, low resistance to leaching, and limited waste loading capacity. As an alternative, alkali or acid-activated geopolymer waste forms have garnered global attention. Unlike cementitious waste forms, geopolymer waste forms exhibit excellent physicochemical characteristics due to their three-dimensional amorphous structure and low calcium content. In this work, we provide an overview of geopolymer waste form research being conducted in countries such as Japan, the United Kingdom, the European Union, and South Korea. We specifically focus on the immobilization of soil waste, spent ion exchange resins, organic liquid waste, and evaporator concentrate (borate waste). We also identify the factors influencing the physicochemical characteristics of geopolymer waste forms and their immobilization performance. We propose a guide for optimizing the molar mixing formulations of geopolymer waste forms, including the selection of appropriate precursor materials. Additionally, we discuss the future prospects and significant challenges in the field of geopolymer waste forms that need to be addressed for their application in radioactive waste management.

A disposal system for spent nuclear fuel mainly divides into two parts; Engineered barriers include spent nuclear fuel, canister, buffer and backfill and natural barriers mean a host rock surrounding engineered barriers. If radionuclides released from a repository, they can migrate to the ecosystem. Sorption plays an important role in retarding the migration of released radionuclides. Hence, the safety assessment for the disposal of a spent nuclear fuel should consider the migration and retardation of radionuclides in geosphere. Distribution coefficient is one of input parameters for the safety assessment. In this work, distribution coefficients for crystalline rock as a natural barrier were collected and evaluated for the purpose of safety assessment for the deep geological disposal of a spent nuclear fuel. The radionuclides considered in this work are as follows; alkali and alkaline earth metals (Cs, Sr, Ba), lanthanides (Sm), actinides (Ac, Am, Cm, Np, Pa, Pu, Th U), transition elements (Nb, Ni, Pd, Tc, Zr), and others (C, Cl, I, Rn, Se, Sn). The sorption of radionuclides is influenced by various geochemical conditions such as pH/carbonates, redox potential, ionic strength, radionuclide concentration, kinds and amounts of minerals, and microbes. For the evaluation of distribution coefficients, the data from Sweden (SKB), Finland (Posiva), Switzerland (Nagra), and Japan (JAEA) were collected, analyzed, and the recommended distribution coefficients have been suggested.

Bacterial metabolisms influence the behavior of uranium (U) in deep geological repository (DGR) system because bacteria are ubiquitous in the natural environment. Nevertheless, most studies for the U(VI) bioreduction have focused on a few model bacterium, such as Shewanella putrefaciens, Desulfovibrio desulfuricans, and Geobacter sulfurreducens. In this study, the potential of aqueous U(VI) ((U(VI)aq) reduction by indigenous bacteria was examined under anaerobic conditions with addition of 20 mM sodium acetate for 24 weeks. Three different indigenous bacterial communities obtained from granitic groundwater at depths of 44–60 m (S1), 92–116 m (S2), and 234–244 m (S3) were applied for U(VI)aq reduction experiments. The S2 groundwater contained the highest U concentration of 885.4 μg/L among three groundwater samples, where U mainly existed in the form of Ca2UO2(CO3)3(aq). The S2 groundwater amended 20 mM of sodium acetate was used for the U(VI)aq bioreduction experiment. Variations in the U(VI)aq concentration and redox potential were monitored for 24 weeks to compare U(VI)aq removal efficiency in response to indigenous bacteria. The U(VI)aq removal efficiencies varied among three indigenous bacteria: 57.8% (S3), 43.1% (S2), and 37.7% (S1). The presence of the thermodynamically stable uranyl carbonate complex resulted in the incomplete U(VI)aq removal. Significant shifts in indigenous bacterial communities were observed through highthroughput 16S rRNA gene sequencing analysis. Two SRB species, Thermodesulfovibrio yellowstonii and Desulfatirhabdium butyrativorans, were dominant in the S3 sample after the anaerobic reaction, which enhanced the bioreduction of U(VI)aq. The precipitates produced by bacterial activity were determined to be U(IV)-silicate nanoparticles by a transmission electron microscope (TEM)-energy dispersive spectroscope (EDS) analysis. These results demonstrated that considerable U immobilization is possible by stimulating the activity of indigenous bacteria in the DGR environment.

The soils contaminated with radionuclides such as Cs-137 and Sr-90 should be solidified using a binder matrix, because radioactively contaminated soils pose environmental concerns and human health problems. Ordinary Portland cement has been widely used to solidify various radioactive wastes due to its low cost and simple process. In this study, simulant soil waste was solidified using cement waste form. The soils were collected around ‘Kori Nuclear Power Plant Unit 1’ and they were contaminated with the prepared simulant liquid waste containing Fe, Cr, Cs, Ni, Co, and Mn. The water-to-dry ingredients (W/D) ratio of cement waste form was 0.40. The cement paste was poured into a cubic mold (5×5×5 cm) and then cured for 28 days at room temperature. The 28-day compressive strength, water immersion, and EPA1311-toxicity characteristic leaching procedure (TCLP) tests were performed to evaluate the structural stability of cement waste form. The compressive strength was not proportional to soil waste loading, and the lowest compressive strength (4±0.1 MPa) was achieved in cement waste form containing 50wt% soil waste. After the water immersion test for 90 days, the compressive strength of cement waste form with 50wt% soil waste increased to 7.5±0.6 MPa, meeting the waste form acceptance criteria in the repository. It is believed that long-term water immersion test contributed to the additional curing and hydration reaction, resulting in the enhanced compressive strength. As a result of the TCLP test, the released amount of As, Ba, Cd, Cr, Pb, Se, Co, Cs, and Sr was less than the domestic and international standards. These results imply that cement waste form can be a promising candidate for the solidification of radioactive soil wastes.

In underground repository environments, various types of engineered barriers are installed to hinder the mobility of radionuclides. Cement admixtures, especially used to improve workability for concrete, are composed of fairly high organic molecules and have a dispersing effect through bonding with the C-S-H of the concrete. Previous studies have shown that complex-forming organics like EDTA, NTA, and ISA have a significant effect on the mobility of radionuclides, but the studies on the behavior and stability of combined complexes in hydrated cement are lacking. So, we selected a commonly used polycarboxylic-ester (PCE) type cement admixture and stable Co as a surrogate of Co-60 to perform desorption experiments from hydrated cement containing the admixture. Radioactive Co is known to be a common contaminant in nuclear fission and medical facilities and considered to exist as a relatively stable phase in repositories. In addition, the evaluation of cobalt can be a standard of safety issue for other radionuclides with the presence of cement admixture in repository. In this study, cement samples were prepared at water/cement ratio of 0.55 and cured for 28 days at 23-25°C and at least 80% of humidity with varying cement admixtures of 0.0, 0.1, and 2.0wt%. To evaluate the stability of cobalt in the weathered cement, a 0.001 M HCl solution was used to simulate cement weathering conditions on a hot plate at 60°C for 1 day using a solid/liquid ratio of 1:100. Degree of weathering was confirmed using XRD analysis. The adsorption experiments were performed by adding 0.0042 mmol of cobalt (CoCl2, Sigma-Aldrich, anhydrous ≥ 98.0%) to the weathered cement for 3 days using a platform shaker at 200 rpm, and the supernatant was separated using a syringe filter (<0.20 um) before ICP-MS analysis to determine the amount of Co adsorption. Cobalt desorption was tested for the Co-adsorbed cement using 0.019 mmol of calcium (Ca(NO3)2·4H2O, Sigma-Aldrich, 99%) for 3 hours to 14 days. The results showed that adsorbed cobalt with and without cement admixture was stably bound to cement, and did not increase any noticeable Co release by 2.0wt% PCE admixture. However, additional experiments using varying contents of PCE and other admixtures should be conducted to provide a standard for assessing the safety of cement admixtures in repositories.

The homogeneity of radioactive spent ion exchange resins (IERs) distribution inside waste form is one of the important characteristics for acceptance of waste forms in long-term storage because heterogenous immobilization can lead to the poor structural stability of waste form. In this study, the homogeneity of metakaolin-based geopolymer waste form containing simulant IERs was evaluated using a laser-induced breakdown spectroscopy (LIBS) and statistical approach. The cation-anion mixed IERs (IRN150) were used to prepare the simulant spent IERs contaminated by non-radioactive Cs, Fe, Cr, Mn, Ni, Co, and Sr (0.44, 8.03, 6.22, 4.21, 4.66, 0.48, and 0.90 mg/g-dried IER, respectively). The K2SiO3 solution to metakaolin ratio was kept constant at 1.2 and spent IERs loading was 5wt%. For the synthesis of homogeneous geopolymer waste form, spent IERs were mixed with K2SiO3 solution and metakaolin first, and then the fresh mixture slurry was poured into plastic molds (diameter: 2.9 cm and height: 6.0 cm). The heterogeneous geopolymer waste form was also fabricated by stacking two kinds of mixtures (8wt% IERs loading in bottom and 2wt% in top) in one mold. Geopolymers were cured for 7d (1d at room temperature and 6d at 60°C). The hardened geopolymers were cut into top, middle, and bottom parts. The LIBS spectra and intensities for Cs were obtained from the top and bottom of each part. Cs was selected for target nuclide because of its good sensitivity for measurement. Shapiro-Wilk test was performed to determine the normality of LIBS data, and it revealed that data from the homogeneous sample is normal distribution (p-value = 0.9246, if p-value is higher than 0.05, it is considered as normal distribution). However, data from the heterogeneous sample showed abnormal distribution (p-value = 7.765×10-8). The coefficient of variation (CoV) was also calculated to examine the dispersion of data. It was 31.3% and 51.8% from homogeneous and heterogeneous samples, respectively. These results suggest that LIBS analysis and statistical approaches can be used to evaluate the homogeneity of waste forms for the acceptance criterion in repositories.

A disposal system for spent nuclear fuel divides into two parts; (1) engineered barriers including spent nuclear fuel, canister, buffer and backfill, (2) natural barriers surrounding engineered barriers. Sorption and diffusion are main retardation mechanisms for the migration of released radionuclides. We analyzed the sorption properties of radionuclides for bentonite as a buffer material and collected/ evaluated the distribution coefficients for the purpose of safety assessment for the deep geological disposal of a spent nuclear fuel. Through this, we presented recommended distribution coefficients for radionuclides required for the safety assessment. This work included the radionuclides as follows; alkali and alkaline earth metals (Cs, Sr, Ba), lanthanides (Sm), actinides (Ac, Am, Cm, Np, Pa, Pu, Th U), transition elements (Nb, Ni, Pd, Tc, Zr), and others (C, Cl, I, Rn, Se, Sn). The sorption of radionuclides affected various geochemical conditions such as pH/carbonates, redox potential, ionic strength, radionuclide concentration, kinds and amounts of minerals, and microbes. Among the evaluated radionuclides, Cs, Ni, Pd, and Ra is sensitive to the ionic strength, while Np, Pu, U, Se, and, Tc is sensitive to the redox condition. For the evaluation of distribution coefficients, the data from Sweden (SKB), Finland (Posiva), Switzerland (Nagra), and Japan (JAEA) were collected, analyzed, and the recommended distribution coefficients were suggested.

Concrete is used as the main engineering barrier in low and intermediate level radioactive waste disposal facilities. As the time passed, the radionuclides stored in repository may contact with groundwater and leak into the ecosystem through the rock media. In this process, the radionuclides can react with calcite via sorption or coprecipitation, because calcite is the major mineral of concrete. Under the various background conditions in repository, frequent dissolution-precipitation reactions can happen. Dissolution of Sr-coprecipitated calcite may be different from that of SrCO3(s) which can mislead the safety performance of radioactive Sr and the estimate of Sr mobility based on the solubility of SrCO3(s). Strontium is not only one of the fission products but also emits beta rays with a long half-life almost 29 years. The strontium may be released or retarded by the dissolution-precipitation reactions in repository. In this study, the dissolution of Sr-coprecipitated with respect to calcite was tested in various environment conditions. The Sr-coprecipitated calcite, (Sr,Ca)CO3(s) was synthesized by coprecipitation method in alkaline condition. The 250 mL of 0.1 M of CaCl2 solution was mixed with 250 mL of 1.14 mM SrCl2·6H2O solution. Then, independently prepared 500 mL of 0.1 M Na2CO3 solution was mixed with the mixed solution of CaCl2 and SrCl2. The precipitates could be made and they were aged for 3 days at room temperature. Then, the supernatant was separated by the centrifugation and the solid at the bottom was dried in an oven at temperature 80°C. After that, the Srcoprecipitated calcite powder was washed using the DI water several times and dried again before use. Characterization of solid powder was conducted by XRD and SEM, and the ICP-MS and ICP-AES were used to analyze the concentrations of Ca and Sr. The batch dissolution experiment was conducted with a solid-to-solution ratio of 10 g/L groundwater in polyethylene tubes. The oxidative groundwater was synthesized by simulating the chemical composition of KAERI Underground Research Tunnel (KURT) DB-3 groundwater. Different temperatures and pHs were prepared and tested for the release of Sr and Ca from the coprecipitated (Sr,Ca)CO3(s) to compare the results with the release of Sr and Ca from SrCO3(s) and CaCO3(s), respectively. Such as, these results will be used to provide better understanding of Sr release and mobility in various repository environments.

Polycarboxylic ether-based high-range water reducer (PCE) has been proposed to use due to the operational advantages of reduced water content and increased fluidity of cementitious mixtures. But the concern about using PCE can increase the mobility of radionuclides as well. Nuclear Decommissioning Authority (NDA) showed that the PCE formulations increased radionuclide solubility in free solution. Solubility of U(VI), 239Pu, 241Am with the cementitious materials tested with 3:1 pulverized fuel Ash/Ordinary Portland Cement (PFA:OPC) and 9:1 Ground Granulated Blast Furnace Slag/OPC (GGBS:OPC) with PCE that increased at least one and, in some cases, more than three orders of magnitude (between 10-9 and 10-4 mol dm-3) for these radionuclides in the cement-equilibrated solution. It is possible that the relatively low molecular weight substances present in the PCE cement mixture increase the solubility of radionuclides. In addition, the organic substances that are easily miscible with water can contribute to increase the solubility. In this study, several radionuclides (Nb, Ni, Pd, Zr, and Sn) that may be present in intermediate and low-level waste (LIW) repositories were selected based on the half-life and the estimated dose accordingly, and the solubility tests were conducted with and without PCE in solution. To simulate the field condition of the underground repository, synthetic groundwater was prepared based on the recipe by the KAERI Underground Research Tunnel (KURT) DB-3 GW and used as a solvent. The solubility limiting solid phase (SLSP) of each radionuclide was determined using Geochemist’s WorkBench (GWB) model. The selected solid phases are Ni(OH)2, ZrSiO4, Nb2O5, Pd(metal), and SnO2, respectively, and the solubility experiments were conducted with 1.0wt% of PCE per total weight and 0.5 g / 250 ml of selected radionuclide’s SLSP for 90 days at room temperature (25°C). Compared with and without PCE presence in solution, the selected radionuclides also showed an increased solubility with the presence of water reducing agent like PCE. This results can be used to correctly estimate the mobility of target radionuclides with the presence of PCE in repository environments.

Radioactive nickel (Ni59 and Ni63) is a major radionuclide that needs to be determined for quantifying the total radioactivity in radioactive waste disposal repository. Also, radioactive waste containing organic wastes, such as cotton and tissue can be decomposed to produce the Isosaccharinic acid (ISA) in a disposal facility. The presence of ISA in the disposal facility could increase the mobility of radionuclides. Therefore, it is necessary to confirm the mobility of Ni with the presence of ISA in the repository. This study investigated the effect of ISA on the sorption and the solubility of Ni in synthesized groundwater. The sorption test was conducted in different time intervals with Ni and ISA. Nickel nitrate hexahydrate and Ca(ISA)2 were used after purchase. Granite was used as the solid medium to simulate the major rock type of the repository. Ni and ISA solution with the medium were mixed using a platform shaker for 6 days. After 6 days, the solid parts were separated by centrifugation and additional syringe filters, and the supernatant was analyzed for Ni and ISA concentration using ICP-MS and IC, respectively. The solubility experiments were conducted at different temperatures (20, 40, and 80°C). Nickel hydroxide was used as the solubility limiting solid phase. To balance the ionic strength and confirm the effect of ISA on Ni solubility, 0.01 M of CaCl2 solution was prepared in a sample without ISA, and 0.01 M of Ca(ISA)2 solution was prepared in a sample with ISA. In solubility tests, the solution was also analyzed by ICP-MS and IC for Ni and ISA, respectively. The concentration of Ni was found to increase with ISA compared to Ni concentration without ISA. The concentration of ISA was not changed during the solubility test periods. For solubility tests, the concentration of Ni also increased according to the increase in temperature. The solid phase was characterized by XRD, FT-IR, and SEM-EDS. Based on the results of this study, the presence and effect of ISA on radioactive Ni mobility should be carefully investigated to secure the long-term safety assessment for the low and intermediate-level waste repository.

Technetium (Tc) is a long-lived radioactive isotope, which exists as TcO4 - with high solubility under oxidative condition. The solubility of Tc is fundamental to assess the safety of radioactive waste repository in the case of a leakage of radioactive wastes. Cellulosic materials (paper, wood, cotton, etc.) contaminated by radionuclides are disposed of in low-level and intermediate-level radioactive waste repositories. Cellulose can be decomposed under anaerobic and alkaline conditions when cement pore water is saturated, and then isosaccharinic acid (ISA) is generated as a degradation product of cellulose. ISA forms complexations with radionuclides in solution and affects the solubilities of radionuclides. Therefore, the effect of ISA should be accurately evaluated to predict and assess the mobility of radionuclides in repository environments. In this study, batch tests were conducted to confirm the effect of ISA on the solubility of Rhenium(IV) Oxide. Herein, rhenium was used as a non-radioactive analog of Tc due to their similar chemical properties. Deionized water (DIW) and 0.1 M NaOH solution in pH 12.5 were used as background solutions, and ISA concentration was varied to 1~20 mM using Ca(ISA)2 and NaISA, respectively. The batch tests were conducted under both aerobic and anaerobic conditions. The whole batch tests under anaerobic conditions were performed in the glove box using oxygen purged DIW with a high purity nitrogen gas (99.9%) and low oxygen concentration (< 0.5 ppm). As a result, the rhenium concentration decreases as more ISA is dissolved in the solution, which shows the contrary effect of ISA on the solubility of other metals and radionuclides (e.g., Co, Th, Fe, Ni, etc.). It is assumed that the reducing capacity of ISA decreases the rhenium dissolution in the solution. Additional characterization of the oxidation state of rhenium oxide and the mechanism will be tested and presented.

Spent nuclear fuel (SNF) is the main source of high-level radioactive wastes (HLWs), which contains approximately 96% of uranium (U). For the safe disposal of the HLWs, the SNF is packed in canisters of cast iron and copper, and then is emplaced within 500 m of host rock surrounded by compacted bentonite clay buffer for at least 100,000 years. However, in case of the failure of the multi-barrier disposal system, U might be migrated through the rock fractures and groundwater, eventually, it could reach to the biosphere. Since the dissolved U interacts with indigenous bacteria under natural and engineered environments over the long storage periods of geologic disposal, it is important to understand the characteristics of U-microbe interactions under the geochemical conditions. In particular, a few of bacteria, i.e., sulfate-reducing bacteria (SRB), are able to reduce soluble U(VI) into insoluble U(IV) under anaerobic conditions by using their metabolisms, resulting in the immobilization of U. In this study, the aqueous U(VI) removal performance and change in bacterial community in response to the indigenous bacteria were investigated to understand the interactions of U-microbe under anaerobic conditions. Three different indigenous bacteria obtained from different depths of granitic groundwater (S1: 44–60 m, S2: 92–116 m, and S3: 234–244 m) were used for the reduction of U(VI)aq. After the anaerobic reaction of 24 weeks, the changes in bacterial community structure in response to the seeding indigenous bacteria were observed by high-throughput 16S rDNA gene sequencing analysis. The highest uranium removal efficiency of 57.8% was obtained in S3 sample, and followed by S2 (43.1%) and S1 (37.7%). Interestingly, SRB capable of reducing U(VI) greatly increased from 4.8% to 44.1% in S3 sample. Among the SRB identified, Thermodesulfovibrio yellowstonii played a key role on the removal of U(VI)aq. Transmission electron microscopy (TEM) analysis showed that the dspacing of precipitates observed in this study was identical with that of uraninite (UO2). This study presents the potential of U(VI)aq removal by indigenous bacteria under deep geological environment.

Magnesium potassium phosphate cements (MKPCs) are prepared by the acid-base reaction of dead burned magnesia (MgO) and monopotassium phosphate (KH2PO4). Low-pH cementitious materials such as MKPCs are currently of interest for the geological disposal of nuclear waste. MKPCs have advantages such as high early strength, high bonding strength, small drying shrinkage, low permeability, and high sulfate resistance. According to the results of previous studies, it is known that cesium, strontium, and cobalt are immobilized in the form of MgCsxK1−xPO4·6H2O, MgxSr1−xKPO4·6H2O, and Co3(PO4)2, respectively, in MKPCs. However, these results were predicted based on thermodynamic data, not directly observed precipitates to clearly show the evidence. Therefore, in this study, we directly analyzed the immobilized forms of Cs, Sr, and Co, respectively. CsNO3, Sr(NO3)2, and Co(NO3)2·6H2O powders (0.3 mol each) were mixed individually in each of the MKPC suspensions. The suspensions in which KH2PO4 was dissolved were pH 4.3 and the dissolution of MgO decreased the H+ concentration, raising the pH close to 11. The hydration products according to pH evolution in the MKPC suspensions were analyzed, and the change in the concentration of ions in the aqueous solution was also measured. An aqueous solution was obtained using a syringe filter (0.45 μm) to analyze the ion concentrations in the solution of the suspension. The collected solutions were diluted with nitric acid and analyzed using inductively coupled plasma mass spectrometry. To characterize the solid phases, the suspensions were obtained with a pipette at specific times and filtered under a vacuum in a Buchner funnel. Because the amounts of hydration products including Cs, Sr, and Co were small, it was not observed by XRD and TGA analysis, but their components could be analyzed by SEM-EDS. The final precipitate forms of Cs, Sr, and Co in the MKPC matrix are MgCsPO4·6H2O, SrHPO4, and Co3(PO4)2·8H2O, respectively.

Liquid scintillation cocktail is liquid waste, which consists of an organic solvent, scintillator, surfactant, and radionuclide. Large volumes of liquid scintillation waste are generated each year, and both the organic compound and radionuclide content can negatively affect on the health and the environment. Therefore, the liquid scintillation waste should be treated in an appropriate way. In this study, to facilitate the treatment of liquid scintillation waste, the sulfate-radical advanced oxidation process (SR-AOP) was performed for the mineralization of liquid scintillator waste. In SR-AOP, highly reactive sulfate radicals, which react more selectively and efficiently with organic compounds, are produced in situ by cleaving the peroxide bond in the persulfate molecule. For the experiment, 100 times diluted ULTIMA GOLD-LLT (initial TOC=699,800 ppm) was used as a liquid scintillation waste. The TOC removal efficiency of liquid scintillation waste by the OXONE (potassium peroxymonosulfate, PMS, 2KHSO5+KHSO4+K2SO4) and sodium persulfate (PS) with varying dosages (4–12 mM) was tested, and the effects of Co2+ and Cu2+ catalysts were compared at a range of pHs (3, 7, and 9). The experimental results demonstrated that 91% TOC removal of ULTIMA GOLD-LLT could be achieved for SR-AOP at initial pH=9, Co2+=1.2 mM (catalyst), PMS=4.8 mM (oxidant) for 60 min reaction. Compared to traditional Fenton AOP which is effective only at low pH, PMS based SR-AOP with Co2+ catalyst is effective at wide range of pHs and less dependent on the treatment efficiency of the operational pH. Therefore, it can be useful for the mineralization of liquid scintillation waste which is difficult to treat with a general treatment method due to the mixture of various organic compounds.