ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Zhuang Wang,Dongping Su,Ting Luo,Qiao Yu,Yiting Wang,Xingyue Liu,Xuanhao Huang,Songdong Ding
The separation of thorium from uranium and rare earths is of great significance for a thorium molten salt reactor nuclear energy system. Herein, a novel Aliquat 336@SiO2–P extraction resin, prepared by the in situ encapsulation of an amine-based ionic liquid (Aliquat 336) into a porous silica–polymer matrix at the same time as the polymerization, was developed for the highly selective separation of Th(IV) over U(VI) and rare earth ions. Batch adsorption studies showed that the prepared Aliquat 336@SiO2–P extraction resin has excellent selectivity, strong adsorption affinity, and high adsorption capacity for Th(IV). The adsorption process of Th(IV) follows pseudo-second-order kinetics and the Langmuir model, and the adsorption of Th(IV) is a monolayer-type, chemical, exothermic, and spontaneous process with increased entropy, achieving a maximum Th(IV) adsorption capacity (qmax) of 52.4 mg/g. Thorium is adsorbed as a complex anion in an HNO3 solution, and its adsorption conforms to the anion exchange mechanism. Furthermore, column experiments indicated that Th(IV) can be selectively separated from simulated monazite HNO3 leach liquor with a recovery rate as high as 97.7%, and the prepared extraction resin has good reusability. Compared to the conventional impregnation method, the Aliquat 336 extractant encapsulated in a porous silica–polymer matrix has significantly lower loss during the adsorption process. Overall, this new extraction resin demonstrates great application potential for the highly efficient separation and recovery of Th(IV) from monazite HNO3 leach liquor.
研究领域:
核能科学
·
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS & DESIGN
·
2019
·
IF 5.77
Hao Zhang,Fan Yang,Ruixi Bai,Zhigang Zhao,Chunqing Cai,Jianguo Li,Ying Ma
Thorium (Th) is an associated ore of rare earth metals that is radioactive and harmful to the environment, but it is also a potential nuclear fuel replacement for uranium. The separation of Th from rare earth elements (REEs) is of great importance in environmental governance and clean-energy development. In this work, a monolithic cerium (Ce) doped silica aerogel-like with flexibility was synthesized using a low consumption and rapid technique, and it was used in a continuous solid-phase extraction as an adsorbent for the selective separation of Th/REEs. The batch adsorption experiments showed that the adsorption efficiency of Th(IV) can be up to 96% when abnormally high levels of metal ions (20 ppm) exist. Under the same conditions, the adsorption efficiency of REEs is at a near-zero level, which demonstrates the great selective separation of Th/REEs for the aerogel-like. The results also indicated that Th(IV) could desorb from the adsorbent in weak acidic media, which is friendly to the environment. Therefore, the material has application prospects for the separation of Th/REEs and removal of radioactive contamination from the environment.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Fan Zhang,Kai-Qiang Ma,Yi Li,Qi Ran,Cheng-Yu Yao,Chu-Ting Yang,Hai-Zhu Yu,Sheng Hu,Shu-Ming Peng
The potential nuclear industry applications of Th make its separation from rare earth elements and U a task of great importance. Herein, materials based on phosphorodiamidate-functionalized silica were synthesized for efficient capture of Th(IV) from acidic solutions and subjected to in-depth characterization. SBA-15-O-DMAP, prepared by oxidation grafting, possessed the largest specific surface area, pore volume and grafted group density as well as abundant oxygenated groups, featuring a high Th(IV) sorption capacity, rapid sorption kinetics, and excellent selectivity. The sorption of Th(IV) by SBA-15-O-DMAP was found to be monolayer-type, chemical, endothermic, and spontaneous. In 0.01–1 M HNO 3 , SBA-15-O-DMAP achieved an excellent Th separation performance with separation factors of SF Th/Ln > 1,000 and SF Th/U > 50, and is thus one of the best materials reported so far for Th separation under highly acidic conditions. Theoretical calculations revealed that the high electron deficiency of the Th(IV) center compared to that of other metals contributed to the Th selectivity. In addition, SiO 2 spheres functionalized with phosphorodiamidate groups allowed one to successfully separate Th(IV) from U(VI) and Ln(III) and achieve good element recoveries (>95%), a high Th decontamination factor (>4.7 × 10 4 ), and excellent reusability. Most importantly, the separation of trace Th from excess U and the extraction of Th from monazite were realized. Thus, the prepared adsorbents were concluded to be promising materials for the practical and selective isolation of Th from highly acidic solutions.
研究领域:
核化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Yao He,Liangang Zhuo,Sha Deng,Zeng Huang,Zhen Qin,Xiang Xie,Ruijie Deng,Yuchuan Yang
Replacing conventional solvents by ionic liquids is a promising route to greener nuclear fuel cycles. Here, we report a unique multi-functional task-specific ionic liquid (TSIL) for the extraction and separation of trace thorium (Th). The phosphoramidate substituted butyl groups to imidazolium ionic liquid (PN-TSIL) shows superior extraction ability and selectivity (distribution rations of Th ~ 8302 and separation factor of Th to uranium (U) ~ 793 at 2 mol/L HNO 3 ). For industial application purpose, an extraction chromatographic resin perpared by PN-TSIL (called PN-TSIL Resin) was made to develop a rapid, highly specific separation technique for simulative 229 Th/ 233 U separation process. Moreover, combination of spectroscopic investigations, quantum-mechanical calculations and thermodynamic parameters mearsurment, an unprecedented resolution picture of extraction process was delineated. The extraction ability and selectivity of thorium could be explained by the multiple binding sites though hybrid interactions (coordination and hydrogen bond) between thorium and PN-TSIL, leading to an entropy-driven extraction process. The understanding of solvent extraction mechanism in molecular scale will inspire new ways for TSIL design for nuclear fuel cycles.
研究领域:
化学
·
核燃料循环
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 3
·607-616
·
IF 1.6
Zhou Zhulin,Fu Yongmei,Wang Xiaoqin,Si Xuting,Lu Youcai
Rare earth (RE) elements is usually associated with radioactive thorium (Th) in nature. Here, we develop a new solid-phase extraction system for the separation of Th, and the effects of acidity, equilibrium time and cycle times on the adsorption performance of the resin were investigated. Kinetic studies show the extraction system has excellent chemical stability and cyclic stability. Further study the application of the resin in industry demonstrated that the separation efficiency is still up to 88%. Therefore, this work not only provides a new strategy for solid-phase extraction system, but also opens up a new way for Th separation.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jing Tang,Linyuan Liao,Xuexiang He,Lidan Lv,Xiangbiao Yin,Wenlong Li,Yuezhou Wei,Shunyan Ning,Lifeng Chen
212 Pb serves as one of the most important nuclides for targeted alpha therapy (TAT), with good potential in the treatment of malignant tumors. However, medical and clinical applications are seriously limited by its extremely short supply, which strongly depends on the acquisition of its parent nuclides such as 228 Ra or 224 Ra. To address this issue, we conducted a systematic investigation on the separation of trace radium from natural thorium using the ion exchange chromatography method, and a novel porous silica-based composite resin functionalized with sulfonic acid groups was prepared, characterized, and employed. Experimental results showed that the silica-supported resin was successfully prepared with the sulfonic acid groups, and possessed small particle size, mesoporous pore structure and large specific surface area. The resin exhibited high selectivity toward thorium compared with barium, and the separation factor reached 123 at low acidity and at low temperature. The resin demonstrated a fast adsorption speed and an excellent separation performance, and the adsorption mechanism was confirmed based on the ion exchange between the sodium carried and the target cations. On the basis, column experiments were further conducted and finally the separation of trace radium from thorium was realized using a small column filled with about 1.0 g resin. The chemical recovery of radium reached 97 %, and the decontamination factor for thorium exceeded 40,000. This work verifies the feasibility of directly extracting 228 Ra and 224 Ra from natural thorium using the sulfonic acid group functionalized materials in the dilute nitric acid solution, and presents an excellent material and systematic experimental data on the separation activities, rendering this study particularly significant.
研究领域:
核化学
·
放射化学
·
医学物理
·
癌症治疗
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）