This study aimed to develop an efficient recycling process for wastewater generated from soil-washing used to remediate uranium (U(VI))-contaminated soil. Under acidic conditions, U(VI) ions leached from the soil were precipitated and separated through neutralization using hydrazine (N2H4). N2H4, employed as a pH adjuster, was decomposed into nitrogen gas (N2), water (H2O), and hydrogen ions (H+) by hydrogen peroxide (H2O2). The residual N2H4 was precipitated when the pH was adjusted using sulfuric acid (H2SO4) to recycle the wastewater in the soil-washing process. This purified wastewater was reused in the soil-washing process for a total of ten cycles. The results confirmed that the soil-washing performance for U(VI)-contaminated soil was maintained when using recycled wastewater. All in all, this study proposes an efficient recycling process for wastewater generated during the remediation of U(VI)-contaminated soil.
The rise of nuclear power plants to meet escalating global energy needs has made environmental pollution including the contamination of uranium due to improper disposal of radioactive wastewater during uranium milling and mining processes. Adsorption, a water purification method known for its fast kinetics, high selectivity, and ease of use, has emerged as a popular choice for the treatment of radioactive wastewater. In response to the critical need for the purification of radioactive wastewater contaminated with U(VI), this review provides a comprehensive summary of the various types of materials, synthetic methods, and adsorption mechanisms used for the purification process. The materials are categorized into four main groups: organic, inorganic, composite/nanomaterials, and framework materials. To enhance the adsorption capacity for U(VI), researchers have explored physical and chemical modifications as well as the development of organic-inorganic hybrids. The improved adsorption performance resulting from these modifications is mostly attributed to electrostatic interaction, surface complexation, and ion exchange mechanisms. However, despite the present understanding of the processes involved, further research is still needed to fully determine the optimal approach for purifying contaminated radioactive wastewater.
Korea faces decommissioning the nation’s first commercial nuclear power plant, the Kori-1 and Wolseong-1 reactors. In addition, other nuclear power plants that will continue to operate will also face decommissioning over time, so it is essential to develop independent nuclear facility decommissioning and site remediation technologies. Among these various technologies, soil decontamination is an essential not only in the site remediation after the decommissioning of the highly radioactive nuclear facility, but also in the case of site contamination caused by an accident during operation of the nuclear facility. But the soil, which is a porous material, is difficult to decontaminate because radionuclides are adsorbed into the pores. Therefore, with the current decontamination technology, it is difficult to achieve the two goals of high decontamination efficiency and secondary waste reduction at the same time. In this study, a soil decontamination process with supercritical carbon dioxide as the main solvent was presented, which has better permeability than other solvents and is easy to maintain critical conditions and change physical properties. Through prior research, a polar chelating ligand was introduced as an additive for smooth extraction reaction between radionuclides present as ions in soil and nonpolar supercritical carbon dioxide. In addition, for the purpose of continuity of the process, a candidate group of auxiliary solvents capable of liquefying the ligand was selected. In this research evaluated the decontamination efficiency by adding the selected auxiliary solvent candidates to the supercritical carbon dioxide decontamination process, and ethanol with the best characteristics was selected as the final auxiliary solvent. In addition, based on the decontamination effect under a single condition of the auxiliary solvent found in the Blank Test process, the possibility of a pre-treatment leaching process using alcohol was tested in addition to the decontamination process using supercritical carbon dioxide. Finally, in addition to the existing Cs and Sr, the possibility of decontamination process was tested by adding U nuclides as a source of contamination. As a result of this research, it is expected that by minimizing secondary waste after the process, waste treatment cost could be reduced and the environmental aspect could be contributed, and a virtuous cycle structure could be established through reuse of the separated carbon dioxide solvent. In addition, adding its own extraction capacity of ethanol used for liquefaction of solid-phase ligands is expected to maximize decontamination efficiency in the process of increasing the size of the process in the future.
Radioactively contaminated metal components from a nuclear power plant must be decontaminated to reduce the risk of radiation exposure to workers, which can be cleaned using a foam decontamination used to reduce the amount of wastewater significantly. Metal components with a fixed radioactive contamination can be effectively decontaminated using a foam consist of 0.5wt% nonionic surfactant, 0.5 M H2SO4, and 0.2 M Ce(SO4)2. However, strongly acidic wastewater is generated from the decontamination method, which contains a high concentration of the nonionic surfactant and ionic materials with radioactive nuclides. This wastewater must be treated as a stable form. In this study, an integrated process of precipitation and low pressure distillation was evaluated for the treatment of wastewater. It was confirmed that the surfactant and ionic materials were effectively removed from the wastewater through the integrated process.
Today, the domestic and international nuclear power industry is experiencing an acceleration in the scale of the nuclear facility decommissioning market. This phenomenon is also due to policy changes in some countries, but the main reason is the rapid increase in the proportion of old nuclear power plants in the world, mainly in countries that introduced nuclear power plants in the early stages. Decontamination is essential in the process of decommissioning nuclear facilities. Among various decontamination targets, radionuclides are adsorbed between pores in the soil, making physical decontamination quite difficult. Therefore, various chemical decontamination technologies are used for contaminated soil decontamination, and the current decontamination technologies have a problem of generating a large amount of secondary wastes. In this study, soil decontamination technology using supercritical carbon dioxide is proposed and aimed to make it into a process. This technology applies cleaning technology using supercritical fluids to decontamination of radioactive waste, it has important technical characteristics that do not fundamentally generate secondary wastes during radioactive waste treatment. Supercritical carbon dioxide is harmless and is a very useful fluid with advantages such as high dissolution, high diffusion coefficient, and low surface tension. However, since carbon dioxide, a non-polar material, shows limitations in removing polar and ionic metal wastes, a chelating ligand was introduced as an additive. In this study, a ligand material that can be dissolved in supercritical carbon dioxide and has high binding ability with polar metal ions was selected. In addition, in order to increase the decontamination efficiency, an experiment was conducted by adding an auxiliary ligand material and ultrasonic waves as additives. In this study, the possibility of liquefaction of chelating ligands and auxiliary ligands was tested for process continuity and efficiency, and the decontamination efficiency was compared by applying it to the actual soil classified according to the particle size. The decontamination efficiency was derived by measuring the concentration of target nuclides in the soil before and after decontamination through ICP-MS. As a result of the experiment, it was confirmed that the liquefaction of the additive had a positive effect on the decontamination efficiency, and a difference in the decontamination efficiency was confirmed according to the actual particle size of the soil. Through this study, it is expected that economic value can be created in addition to the social value of the technology by ensuring the continuity of the decontamination process using supercritical carbon dioxide.
The purpose of this study was to effectively purify U-contaminated soil-washing effluent using a precipitation/distillation process, reuse the purified water, and self-dispose of the generated solid. The U ions in the effluent were easily removed as sediments by neutralization, and the metal sediments and suspended soils were flocculated–precipitated by polyacrylamide (PAM). The precipitate generated through the flocculation–precipitation process was completely separated into solid–liquid phases by membrane filtration (pore size < 45 μm), and Ca2+ and Mg2+ ions remaining in the effluent were removed by distillation. Even if neutralized or distilled effluent was reused for soil washing, soil decontamination performance was maintained. PAM, an organic component of the filter cake, was successfully removed by thermal decomposition without loss of metal deposits including U. The uranium concentration of the residual solids after distillation is confirmed to be less than 1 Bq·g−1, so it is expected that the self-disposal of the residual solids is possible. Therefore, the treatment method of U-contaminated soil-washing effluent using the precipitation/distillation process presented in this study can be used to effectively treat the washing waste of U-contaminated soil and self-dispose of the generated solids.
본 연구에서는 역삼투막공정을 이용하여 수용액 중 저준위 방사성이온인 세슘과 요오드 이온을 제거하는 실험을 수행하였다. 국내에서 생산되는 역삼투막모듈 두 가지와 그리고 폐모듈 세정한 후 세슘과 요오드 이온에 대한 제거성능을 비 교하였다. 공급수의 농도와 압력을 달리하여 실험을 진행한 결과, 세 가지 모듈 모두 세슘에 비해 요오드의 제염계수가 높은 것을 알 수 있었으며, 특히, 세정한 모듈은 요오드에 대한 제염계수가 1140으로 확인되었다. 대체적으로 실험조건이 고압일 때보다 저압일 때 제염성능이 좋은 것으로 나타났으며 이는 저압조건에 가까운 압력을 갖는 수도수에 직접 모듈을 설치할 경우에도 사용이 가능하리라 판단되었다. 또한 EDTA와 SBS, NaOH, 마이크로버블 등을 사용하여 세정한 막의 제염성능이 세정 전의 제염성능보다 높아졌으며 저압, 저농도 조건에서 요오드에 대한 회수율이 세정 후에 6.3% 증가한 결과를 얻었다.
A continuous process of persulfate oxidation and citric acid washing was investigated for ex-situ remediation of complex contaminated soil containing total recoverable petroleum hydrocarbons (TRPHs) and heavy metals (Cu, Pb, and Zn). The batch experiment results showed that TRPHs could be degraded by Fe2+ activated persulfate oxidation and that heavy metals could be removed by washing with citric acid. For efficient remediation of the complex contaminated soil, two-stage and three-stage processes were evaluated. Removal efficiency of the two-stage process (persulfate oxidation - citric acid washing) was 83% for TRPHs and 49%, 53%, 24% for Cu, Zn, and Pb, respectively. To improve the removal efficiency, a three-stage process was also tested; case A) water washing - persulfate oxidation - citirc acid washing and case B) persulfate oxidation - citric acid washing (1) - citric acid washing (2). In case A, 63% of TRPHs, 73% of Cu, 60% of Zn, and 55% of Pb were removed, while the removal efficiencies of TRPHs, Cu, Pb, and Zn were 24%, 68%, 62%, and 59% in case B, respectively. The results indicated that case A was better than case B. The three-stage process was more effective than the two-stage process for the remediation of complex-contaminated soil in therms of overall removal efficiency.
Ultrasound and Surfactant aided soil washing process has been shown to be an effective method to remove diesel from soils. The use of surfactants can improve the mobility of diesel in soil-water systems by increasing solubility of adsorbed diesel into surfactant micelles. However, a large amount of surfactant is required for treatment. In addition, synthetic surfactants, specially anionic, are more toxic and the surfactant wastewater is hard to treat by conventional wastewater treatments even by AOPs. Ultrasound improves desorption of the diesel adsorbed on to soil. The mechanisms are based on physical breakage of bonds by hot spot, directly impact onto soil particle surface, the fragmentation of long-chain hydrocarbons by micro-jet and microstreaming in the soil pores. The use of ultrasound as an enhancement method in both anionic and nonionic surfactant aided soil-washing processes were studied. And all experiments were examined proceeded under CMC surfactant concentration, frequency 35 khz, power 400 W, Soil-water ratio 1:3(wt%), particle size 0.24 ~ 2mm and initial diesel concentration. 20,000 mg/kg. Combination with ultrasound showed significant enhancements on all the processes. Especially, nonionic surfactant Triton-X100 with ultrasound showed remarkable enhancements and diesel removal rate enhanced by ultrasound helps desorpting of surfactant adsorbed onto soils which prevented decreasing surfactant activity.
This study has been carried out to examine the feasibility of soil washing process for reducing arsenic contamination level of soil around Dalchên Mine. The results of physicochemical tests of the target soil showed that pH was weak alkalic (pH ~- 7.8), soil texture was coarse sand, and organic contents (5.7%) and CEC (Cation exchange capacity; 21.5 meq/100 g) were similar with those of soils generally found in Korea. Contamination levels of arsenic were found to over 201 mg/kg which exceed the Korea standard levels of countermeasure and concern. To investigate chemical partitioning of heavy metals, sequential extraction procedures were adopted and it was found that arsenic was predominantly associated with the residual fraction among five fractional forms as much as over 85%, which is demonstrating that only less than 15% of all might be vulnerable to a selected washing agents. Among 6 kinds of washing agents applied on the screening for arsenic-contaminated soil, HCl and H3PO4 solution were selected as promising washing agents. In comparison with HCl and H3PO4 solutions for arsenic washing by kinetic experiment in the change of pH, soil-solution ratio, temperature, and washing solution concentration, H3PO4 solution was determined to best one of agents tested, which showed faster washing rate than HCl to accomplish regulatory goal.
Three kinds of toxic heavy metals, such as lead, copper, and cadmium, existing abundantly in contaminated soils were selected to investigate pH change, electroosmotic flow, and the removal rate in the application of electrokinetic process. In the change of pHs, they reached to about 12 and 2 at each cathodic and anodic region, respectively, and maintained for reaction being proceeded. Electroosmotic flow rates were not influenced by the kind of metal species but by electropotential gradient. On the soils contaminated by each metal, the removal rate of Cd was the fastest among three as in the order of Cd>Pb>Cu. While on the soils contaminated by mixed metal species, Cu was the fastest. Metal species transported by electrokinetic processes were distributed in between 0.9 and 1.0 of normalized region. In the case of soils contaminated by one kind of metal. the relative concentrations of Pb and Cd estimated in between normalized region 0.9 and 1.0 were 5.2 and 5.7, respectively.