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CHEMICAL PHYSICS · 2020 · IF 1.771

Comparison analysis of wet digestion and stripping methods on recovery of lithium isotopes in the loaded phase

Bing Liu,Yongzhong Jia,Yan Jing,Ying Yao

6 Li and 7 Li play important roles in the nuclear industry. In this study, the recovery of lithium isotopes in the loaded phase after extraction was compared for the first time between the stripping and wet digestion method. The results showed non-significant differences in the data obtained after processing in the two methods. The recovery of lithium isotopes by wet digestion is simple and complete. But it destroys the organic phase and requires heating at high temperatures, making it suitable for handling small amounts of samples. The stripping method is recommended for sample processing because it involves lesser chemical reagents and related hazards without damaging the sample.

CAS / MDL: 100-66-3 7447-41-8
研究领域: 化学 · 核科学与技术
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Mechanism demystification and factor optimization of uranium decontamination on fabrics via supercritical CO2: Role of off-line prepared additives

Huitao Lv,Bin Hu,Jiaqi Chen,Tianyu Li,Chao Peng,Yiming Wang,Yun Xue,Fuqiu Ma,Yongde Yan,Emmanuel Osei Tutu

Supercritical CO 2 (SC-CO 2 ) technology promises to overcome the trade-off between secondary waste volume and decontamination efficiency in traditional radioactivity decontamination methods. However, attempts to use this technology for decontaminating uranium-contaminated fabrics have remained unexplored. Hence, we investigated the role of additives in decontaminating uranium-contaminated fabrics using SC-CO 2 technology, with particular emphasis on off-line versus in-situ preparation methods. Additives prepared via the off-line method, comprising H(NO 3 ) · TBP complexes, demonstrated superior efficiency owing to immediate solubility and reactivity in SC-CO 2 . Molecular dynamics (MD) simulations also supported these experimental observations by visualizing the microstructural evolution of the additive molecules. The factors, including pressure (20 MPa) and temperature (343 K), were optimized, achieving up to 97.4 % decontamination efficiency in 40 min. The radioactivity of the fabric surface was reduced to the level that allowed for reuse in the nuclear field. Notably, the mechanism analysis revealed the transformation of uranium contaminants from UO 2 (OH) 2 to UO 2 (NO 3 ) 2 · 2TBP complexes, which were efficiently dissolved in SC-CO 2 . Furthermore, the technology demonstrated high versatility, successfully decontaminating various fabric types and real radioactive samples, achieving results suitable for reuse in the nuclear field. These findings suggest that SC-CO 2 , when combined with optimized additives, offers an environmentally sustainable and highly effective method for uranium decontamination in the nuclear industry.

研究领域: 环境科学 · 放射化学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Innovative deep decontamination of radioactive solid surfaces using microemulsions of deep eutectic solvents in supercritical carbon dioxide

Huitao Lv,Jianzhang Gao,Jiaqi Chen,Tianyu Li,Yi Liang,Bin Hu,Fuqiu Ma,Yun Xue,Yongde Yan,Emmanuel Osei Tutu

Radioactive solid wastes resulting from the application of nuclear energy pose a risk to the environment, yet traditional decontamination methods generate many secondary wastes. Thus, sustainability-driven innovations are receiving increasing attention to achieve eco-friendly decontamination methods characterized by minimizing secondary waste generation. Here, we proposed a sustainable and pioneering approach to decontaminate radioactive solid wastes using microemulsions of deep eutectic solvents (DESs) in supercritical carbon dioxide (SC-CO 2 ). We also determined the optimal ratios of the additives as follows: prepared DESs with a molar ratio of choline chloride (ChCl) to p-toluenesulfonic acid monohydrate (ptsa) of 1:2, and nonyl phenol polyoxyethylene ether (NP-10) to ChCl:ptsa DESs in a molar ratio of 0.8. Remarkably, after optimization of the decontamination process in terms of pressure, temperature and cleaning time, the radioactivity on the sample surface can be reduced to a level that is reusable in the nuclear field. Detailed analyses provided insights into the intermolecular interactions within the DESs. And the decontamination mechanisms involved the spontaneous evolution of microemulsions with ChCl:ptsa as the core to facilitate the solvation and removal of radioactive contaminants. Additionally, repeated cleaning was proved to be effective for ultra-deep decontamination, with the radioactivity on the sample surface reaching a clearance level and a decontamination efficiency of 99.8%. The DESs-in-CO 2 systems successfully decontaminated various materials and simulated radionuclides, even real radioactive metal wastes from the nuclear industry. It was notable that the DESs-in-CO 2 systems achieved decontamination efficiencies of more than 95.0% for radioactive contaminants on these solid surfaces. Overall, this innovative approach provided a green alternative to conventional radioactive solids decontamination, meeting the need for sustainable development of nuclear energy.

CAS / MDL: 67-48-1 6192-52-5
研究领域: 核工程 · 环境科学 · 化学工程 · 材料科学
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APPLIED RADIATION AND ISOTOPES · 2022 · IF 1.787

Synergistic removal of U(VI) from aqueous solution by TAC material: Adsorption behavior and mechanism

Yunyun Bao,Yan Liu,Changfu Wang,Yun Wang,Dingzhong Yuan,Jianda Xu,Zuqing Zhu,Yan He,Jinbiao Liu

The adsorption and recovery of uranium from wastewater is of positive significance to the development of nuclear industry and environmental remediation. The ternary polymer (PZS-co-TA) was prepared from hexachlorocyclotriphosphazene (HCCP), 4,4-sulfonyldiphenol (BPS) and tannic acid (TA) under ultrasonic . TAC was then obtained after carbonization under high temperature from PZS-co-TA. The structure and performance of TAC were analyzed using SEM , EDS, FT-IR, XRD, Raman, BET and TG. The adsorption capacity of TAC for uranium under different static adsorption conditions was investigated. The adsorption process was more consistent with pseudo-second-order model. The maximum adsorption capacity calculated by non-linear Langmuir model was 492.5 mg/g at pH 5.5. The thermodynamic values suggested that the adsorption process was spontaneous and endothermic. Moreover, after five cycles of adsorption-desorption tests, TAC remained effective at adsorbing uranium, implying the introducing of TA to the precursor (PZS-co-TA) could enhance the adsorption capacity for uranium.

研究领域: 环境科学 · 材料科学 · 核工程
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Urushiol-resourced dopamine analogue as a trigger to construct clay-hexacyanoferrate hydrogel for cesium removal

Hang SHEN,Lingdan ZHU,Qi LIN,Shujun GUO,Huagui ZHANG

To guarantee the sustainable development of the nuclear industry, it is vital to have a low-cost, green, and scalable route developed to synthesize efficient adsorbents for rapid and effective remediation of nuclide-contaminated water. In this study, a natural catechol derivative with unsaturated alkyl chain, urushiol, was aminated by mildly thiol-ene click with cysteamine to form a dopamine analogue, which can self-polymerize and trigger the formation of silicate plates into hydrogel framework and in-situ immobilize the potassium copper hexacyanoferrate, an efficient adsorbent, when hexacyanoferrate and excess Cu 2+ were present in the silicate suspension. The chelation between Cu 2+ , poly-urushiol and hexacyanoferrate that assemble the hybrid hydrogel was confirmed by SEM and XPS and the performance of this hydrogel was evaluated in terms of adsorption capacity (214 mg g −1 ), selectivity (K d >10 6 mg L −1 ), kinetics and reversible self-healing behavior with pleasing results obtained. The economic and nature-sourced property of the urushiol offers a green and novel concept to develop a satisfying adsorbing system for Cs + removal.

研究领域: 环境科学 · 材料科学 · 核工业
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Metals · 2025 ·Vol. 15 ·期 5 ·468 · IF 2.5

Selective Extraction of Zirconium from Sulfuric Acid Solutions at High Concentration with Trioctylamine (TOA)

Shuo Tian,Jing Song,Hongqian Sun,Congcong Zhao,Zhiyu Zhang,Mingming Han,Tao Qi

Zirconium (Zr) and hafnium (Hf) are very important in nuclear and high-temperature applications, but their similar physical and chemical properties bring great challenges to separation. The current extraction methods have defects, such as low efficiency at high metal concentration. In this article, a zirconium (Zr)/hafnium (Hf) solvent extractive separation from sulfuric acid solutions using trioctylamine (TOA) as the extractant was researched at room temperature. The aqueous solution is prepared using zirconium sulfate (containing Hf), and the concentration of metal ions (Zr4+and Hf4+) was about 1.096 mol·L−1. The effects of the aqueous acidity, the concentration of TOA, the contacting time, and the organic to aqueous O/A ratio on the separation of Zr and Hf were investigated. It is observed that the Zr can be extracted in the organic phase selectively, and the optimal conditions were: TOA concentration of 40 vol%, organic to aqueous O/A ratio of 3, contacting time of 5 min. Under these conditions, the single-stage extraction rate of Zr is 61.23%, while the Hf is almost not extracted. The mechanism of Zr extraction by TOA was studied through the saturation capacity and slope methods. Based on the results, it is believed that the structure of the extracted complex may be [R3NH]2[Zr(SO4)3]. This study provides a new approach for the development of industrialized Zr-Hf separation.

研究领域: 化学工程 · 核工业
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2024 ·Vol. 333 ·期 6 ·2691-2696 · IF 1.5

Efficient separation of europium by solvent extraction using bis(2-ethylhexyl) phosphate

Wang Yi,Yang Jiajia,Sui Jixue,Wang Lan,Tang Jia,Yang Yu,Lu Yunyun,Dai Shuang,Cao Qi

Efficient separation of europium (Eu) from aqueous solution is pivotal for the sustainable development of nuclear industry and rare earth industry. In this work, bis(2-ethylhexyl) phosphate (P204) was employed to separate Eu(III) by solvent extraction method using kerosene as diluent. The extraction equilibrium could reach within 30-min contact time. The extraction ratio enhanced as the increased O:A phase ratio, extractant concentration, and temperature. However, the HCl introduction caused its clear descent. Combined with the slope method and FT-IR analysis, extraction mechanism could be unveiled, which is the coordination between P=O double bond and Eu(III) ions in a proportion of 3:1.

CAS / MDL: 298-07-7 10025-75-9
研究领域: 化学工程 · 核工业 · 稀土工业
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

Photochemical synthesis of hierarchical adsorbents for gaseous iodine capture and storage

Mei Wu,Xin Zhao,Bowen Li,Wenhao Zhang,Hao Zeng,Xuao Zhang,Weichuan Xu,Lingling Bi,Zhiqiang Chen,Jinlong Jiang

Developing rapid, cleaner synthesis strategies for adsorbent preparation through preparative chemistry , and elucidating pore and metal adsorption mechanisms, represent essential goals in achieving highly efficient capture and storage of radioactive iodine in the nuclear industry. This work utilizes solvent-free photopolymerization and one-step photoreduction methods to synthesize hierarchical zeolite Silicaite-1 (denoted as MS-1) and copper-modified zeolite Cu@MS-1, respectively. Focusing on the effects of metal species and pore structure on adsorption performance and mechanisms, their application to radioactive iodine sequestration from spent fuel is evaluated. The findings show adsorption of gaseous iodine by hierarchical zeolite MS-1 is predominantly physical. At 75 °C, it rapidly reaches high equilibrium adsorption capacity (524 mg/g) within 40 min, with faster iodine uptake kinetics than fully microporous zeolites and higher capacity than fully mesoporous silica . Introduction of metallic copper contributes additional chemical adsorption , efficaciously enhancing the MS-1 affinity for gaseous iodine. Cu@MS-1 achieves considerable equilibrium adsorption capacity (520 mg/g) in only 30 min, and improved radioactive iodine retention. The photochemical synthesis approach generates no liquid waste and forms the zeolite framework in 10 min. The obtained hierarchical zeolites MS-1 and Cu@MS-1 have high gaseous iodine capture and storage abilities, opening a new route for rapid and cleaner synthesis of highly efficient radioactive iodine adsorbents.

研究领域: 核工业 · 材料科学 · 环境工程
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EUROPEAN POLYMER JOURNAL · 2024 · IF 5.8

Modified polyethyleneimine with abundant N/O/S-heteroatoms and aromatic segments: Convenient synthesis via sulfur-isocyanide-amine multicomponent reaction and application in high-performance iodine capture

Junyang Zhang,Wei Shi,Maoting Yang,Kaiping Huang,Yuanqiang Zhu,Zhengfeng Xie

With the continuous development of nuclear industry, the discharge of radioactive iodine ( 129 I and 131 I) become a potential danger to ecological environment. The development of high-performance iodine capture materials has important practical significance to reduce the harm of radioactive iodine. With the aim to construct new iodine-adsorbing polymer under the “bottom-up” structural designing guidance, using sulfur (S), branched polyethyleneimine (PEI) and 4,4’-oxybis(isocyanobenzene) (OBI) as starting substrates, a thiourea-modified PEI derivative (PEI-SIA) with abundant N/S/O-heteroatoms and aromatic molecular fragments was successfully prepared here via efficient sulfur-isocyanide-amine multicomponent polymerization (SIA-MCP). Characterization of PEI-SIA’s fundamental properties indicated that it is a new type of covalent organic polymer (COP). The iodine adsorption performance of PEI-SIA was systematically investigated. Experimental results showed that PEI-SIA can effectively adsorb iodine in steam (75 °C), cyclohexane, and aqueous phases, with the equilibrium adsorption capacities up to 6.48, 2.63, and 3.01 g g −1 , respectively. The iodine adsorption mechanism of PEI-SIA was characterized by experimental investigation and Density Functional Theory (DFT) calculation. The results revealed that PEI-SIA’s high iodine adsorption performance can be attributed to the synergistic effect brought by N/S/O-containing segments and the electron rich aromatic skeletons in PEI-SIA.

CAS / MDL: 101-80-4
研究领域: 材料科学 · 环境科学 · 核工业
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

MIL-88A(Al)/chitosan/graphene oxide composite aerogel with hierarchical porosity for enhanced radioactive iodine adsorption

Xinxin Wang,Ruixue Meng,Shiyong Zhao,Zhenyu Jing,Yonghui Jin,Jie Zhang,Qiujiu Du,Xinxin Pi,Long Chen,Yanhui Li

To ensure the sustainable development of the nuclear industry, the effective capture of radioiodine from nuclear wastewater has attracted much attention. Herein, a novel MIL-88A(Al)/chitosan/graphene oxide (MCG) composite aerogel was prepared by using crosslinked chitosan and graphene oxide as the 3D network skeleton, and MIL-88A(Al) nanocrystalline particles were introduced into the skeleton by freeze-drying method. MIL-88A(Al) adsorption capacities for volatile and soluble iodine were 2.02 g g −1 and 850.00 mg g −1 , respectively. Owing to the synergistic effect of MIL-88A(Al), GO, CS, and the hierarchically porous structures of the MCG aerogel, the adsorption capacities for volatile and soluble iodine by the MCG aerogel were increased to 2.62 g g −1 and 1072.60 mg g −1 , respectively. Furthermore, the adsorption performance of the MCG aerogel for volatile and soluble iodine could be maintained at 83 % and 82 % after 5 cycles, suggesting excellent recoverability. Meanwhile, the adsorption mechanism studies showed the interactions between iodine and N H, Al O, and C O in MCG aerogel. Furthermore, the adsorption process is consistent with the Elovich kinetic and Sips isotherm models. MCG aerogels are potential candidates for enhanced radioiodine adsorption due to their high radioiodine capture performance and excellent recyclability.

CAS / MDL: 7553-56-2 7681-11-0
研究领域: 材料科学 · 环境科学 · 核工业
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2020 ·Vol. 325 ·期 2 ·673-682 · IF 1.137

Lithium isotope effect in extraction of lithium chloride by 4-Aminobenzo-15-crown-5 in water-anisole ionic liquid double solvent system

Liu Bing,Jia Yongzhong,Jing Yan,Zhang Quanyou,Shao Fei,Yao Ying

Abstract The lithium isotope separation (LIS) plays a vital role in development of nuclear industry. The liquid–liquid extraction technologies open up new possibilities for LIS. This work presents preliminary results of the study on the extractions and separation of 6 Li/ 7 Li by mixed system, comprising amino-derivatives of benzo-15-crown-5 (4AB), ionic liquid and anisole. 4AB was used as an extractant. The eparation factor ( α ) is 1.031 ± 0.001, and abundance of 6 Li in loaded organic phase is 7.76%. Meanwhile, the reason why 4AB has better separation efficiency than B15C5 was explored brief by Fourier transform infrared (FT-IR) spectrum and quantum chemical calculations. Graphic abstract

研究领域: 核工业 · 化学工程
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2020 ·Vol. 324 ·期 1 ·339-348 · IF 1.137

A new diphosphonic acid extractant N,N-n-octylamine di(methylene phenylphosphinic acid) for extraction and separation of zirconium and hafnium in hydrochloric acid

Zhao Jialin,Sui Ying,Peng Xiujing,Sun Guoxin,Cui Yu

Abstract Nuclear grade zirconium and hafnium are the key to promoting the development of nuclear industry. We designed and synthesized a new diphosphonic acid extractant N , N - n -octylamine di(methylene phenylphosphinic acid) (OADMPPA) with excellent extraction ability and priority for extraction of zirconium. This paper focused on the changes in extraction mechanisms and composition of complexes. With increasing concentration of HCl, cation exchange mechanism gradually changed into solvation mechanism, and complexes converted in the order of ZrOA, Zr(HA) 2 Cl 2 and ZrCl 4 ·H 2 A. Compared with bis(2,4,4-trimethylpentyl)phosphinic acid (Cyanex272), OADMPPA could increase the extraction rates of zirconium and hafnium by 7.2 and 12.6 times. Graphic abstract

CAS / MDL: 1116-76-3
研究领域: 化学工程 · 核工业
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