JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 10
·3903-3910
·
IF 1.6
Zheng RuoChen,Mao GuoShu,Fu Zhihai,Zhang Xian,Yu ShengJie,Yue Yuanzhen,Li Jiayun
A new poly(4-vinylpyridine) resin was prepared and characterized. The adsorption of Th 4+ on resin was studied as a function of contact time, nitric acid concentration, metal ion impurity and initial Th 4+ concentration. The adsorption kinetics and isotherms were analyzed. The results revealed that the adsorption equilibrium for the adsorption of Th 4+ on resin was reached within 30 min. The efficiency of Th 4+ adsorption on resin improves when the nitric acid acidity increases. The adsorption capacity of the resin increases with an increase in the initial concentration of Th 4+ . The thorium distribution coefficient increases with metal nitrate in the system.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Xiaofeng Zhao,Weipeng Wang,Yuancheng Teng,Yuxiang Li,Xue Ma,Yang Liu,Rajeev Ahuja,Wei Luo,Zhengjun Zhang
Rhabdophane is an important permeable reactive barrier to enrich radionuclides from groundwater and has been envisaged to host radionuclides in the backend of the nuclear fuel cycle. However, understanding of how An4+ and Sr2+ precipitate into rhabdophane by wet chemistry has not been resolved. In this work, Th4+ and Sr2+ incorporation in the rhabdophane/monazite structure as La1–2xSrxThxPO4·nH2O solid solutions is successfully achieved in the acid solution at 90 °C. Some specific issues such as lattice occupation of Th4+ and Sr2+, precipitation reaction kinetics, and crystal growth affected by starting stoichiometry are discussed in detail, along with investigating the chemical stability of La1–2xSrxThxPO4·nH2O precipitations and associated La1–2xSrxThxPO4 monazite. The results reveal that the excess of Sr2+ appears to be a prevailing factor with a suggested initial Sr: Th ≥ 2 to obtain the stability domain of La1–2xSrxThxPO4·nH2O (x = 0∼ 0.1). A rapid ion removal associated with a nucleation process has been observed within 8 h, and Th4+ can be removed more than 98% after 24 h in 0.01 mol/L solutions. From structural energetics based on density functional theory, the lattice occupation of Th4+ and Sr2+ is energetically favorable in nonhydrated lattice sites of [LaO8], although two-thirds of lattice sites are associated with [LaO8·H2O] hydrated sites. Intriguingly, the crystal transformation from rhabdophane to monazite associated with the transformation from [SrO8] to [SrO9] polyhedra can greatly improve the leaching stability of Sr2+.
研究领域:
核化学与放射化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TALANTA
·
2009
·
IF 3.206
Canrong Lin,Hongqing Wang,Yuyuan Wang,Zhiqiang Cheng
A new pyrazole derivative 1-phenyl-3-methylthio-4-cyano-5-acrylicacidcarbamoyl-pyrazole (PMTCAACP) was synthesized and chosen as a complexing monomer for the preparation of surface-grafted ion-imprinted polymers for selective solid-phase extraction of thorium(IV). The silica gel, modified with maleic anhydride , was prepared as a carrier material. In the ion-imprinting process, Th(IV) was complexed with PMTCAACP, and then imprinted in the polymers grafted to the surface of modified silica gel. Subsequently, the template Th(IV) ions were removed with 6 mol/L HCl solution. The obtained ion-imprinted particles for Th(IV) showed specific recognition, and rapid adsorption and desorption kinetics process. The maximum static and total dynamic adsorption capacity of the ion-imprinted polymers (IIPs) for Th(IV) was 64.8 and 37.4 mg/g, respectively. The relative selectivity coefficient values of the imprinted adsorbent for Th(IV)/U(VI), Th(IV)/Ce(III), Th(IV)/La(III), and Th(IV)/Zr(IV) were 72.9, 89.6, 93.8, and 137.2 times greater than non-imprinted matrix, respectively. The interference effect of common cations tested did not interfere with the recovery of Th(IV). The enhancement factor of 20.2, the detection limit of 0.43 μg/L, and the precision of 2.47% ( n = 7) of the method under the optimized conditions were obtained. Additionally, the calibration curve ( r = 0.9993) was linear in the range of 1.43–103 μg/L of thorium(IV). The prepared IIPs were shown to be promising for solid-phase extraction coupled with UV–vis spectrophotometry for determination of trace Th(IV) in real samples.
研究领域:
化学
·
材料科学
·
分析化学
✓ 已验证
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 MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Congcong Chen,Ying Xie,Lingyi Jia,Yong Zhang
Efficient capture of Th(IV) from aqueous solution is of importance to both solve the radioactive pollution for environmental safety and provide clean energy for sustainable development. However, it still faces huge challenge. In this study, eucalyptus leaf extract was applied as template agent to fabricate Zn/Al-bimetallic layered double oxides (ZnAlLDO), providing more active sites for Th(IV) removal. The removal process of Th(IV) onto ZnAlLDO could reach equilibrium within 5 min and the maximum removal capacity calculated from the Langmuir model was 1153.71 mg g −1 at pH = 4.0 and 298 K. Over 97 % Th(IV) could be removed by ZnAlLDO during the dynamic adsorption process and the removal efficiency still remained at a high level (85 %) after 5 cycles. The Th(IV) removal process on ZnAlLDO was ascribed to electrostatic attraction, complexation and ion exchange. It could be believed that the ZnAlLDO with large removal capacity (1155.5 mg g −1 ), fast equilibrium time (5 min) and easy desorption (91.76 %) with high recovery (85 %) might be a promising adsorbent for the separation of Th(IV).
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaojuan Liu,Songtao Xiao,Tiantian Jin,Feng Gao,Ming Wang,Yanan Gao,Wei Zhang,Yinggen Ouyang,Guoan Ye
A novel porous material tailored for Th (IV) entrapment with not only large capacity but also high selectivity is highly desired for the thorium fuel cycle. Here, a three-dimensional COF (covalent organic framework) material, named COF-DL229 was prepared for the efficiently selective entrapment of Th (IV). Batch sorption experiments indicated that the entrapment of Th (IV) was a pH-dependent, rapid (equilibrium was reached within 1 min) process. The maximum saturated entrapment capacity could reach 513 mg g −1 , which is higher than that of the reported two-dimensional COF. The single-component batch experiments and muti-components dynamic experiments suggested that COF-DL229 has a strong affinity towards Th (IV), but little affinity with other ions, which makes COF-DL229 a promising material for selective thorium recovery from waste solution. The interaction mechanism was Th-N coordination, which was confirmed by characterizations (Fourier Transform infrared spectroscopy, FT-IR, X-ray photoelectron spectroscopy, XPS, energy dispersive spectrometer, EDS) and density functional theory (DFT) calculations. The density of states indicated that the doping of the Th (IV) can lower the band gap of the COF-DL229, indicating higher electrical conductivity and stronger adsorption energy. The differential charge exhibited an obvious charge transfer between Th (IV) and the N atom in COF-DL229.
研究领域:
材料科学
·
环境科学
·
核能技术
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 39
·e202202129
·
IF 2.307
Ting Yu,Zhenghua Qian,Lin Li,Zonghui Lu,Bin Li,Qiang Zhang,Xiaofeng Liu,Hui He,Yanbo Qiao,Guoan Ye
Graphical This is a new method of producing nuclear material. ThO 2 NPs are synthesized by pyrolysis of an undiscovered thorium-based MOF. The MOF-derived ThO 2 NPs can easily be sintered to form ThO 2 ceramics. (Twitter: @yuting0437) A new method is demonstrated for synthesizing thorium dioxide (ThO 2 ) nanoparticles (NPs) by thermal decomposition of an undiscovered thorium-based metal-organic framework (MOF). Upon heating at 520 °C, the thorium-based MOF crystals, designated Th-MTB, are converted completely to ThO 2 NPs with an average size of 150 nm. The MOF-derived ThO 2 NPs are easily sintered to form ThO 2 ceramics which have good thermal conductivity. The crystalline grains of ThO 2 grow continuously during sintering.The method for the synthesis of ThO 2 NPs could have potential applications in the production of nuclear materials.
研究领域:
材料科学
·
核材料
·
化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Dingzhong Yuan,Shiao Zhang,Jiale Tan,Yahong Dai,Yun Wang,Yan He,Yan Liu,Xiaohong Zhao,Mengmeng Zhang,Qinghua Zhang
It is challenging to extract Th (IV) and U (VI) from rare earth elements (REEs) in concentrated acidic solution. Herein, a nanoporous polymer adsorbent P (DVB-VPA) bearing phosphonic acid groups has been synthesized by solvothermal copolymerization of divinylbenzene (DVB) and vinylphosphonic acid (VPA). The maximum adsorption capacity (q max ) for Th (IV) and U (VI) onto P (DVB-VPA) was estimated to be 354.6 and 216.5 mg g −1 at 298 K in 4 mol L −1 of hydrogen nitrate media, which were much larger than most of the adsorbents reported previously. Besides, P (DVB-VPA) exhibited a good selectivity for Th (IV) and U (VI) from REEs in concentrated nitric acid solution, since the values of the selectivity for Th (IV) and U (VI) over La (III), Ce (III), Eu (III), Nd (III) and Sm (III) were 82.2% and 72.5%, respectively. XPS analysis revealed that the adsorption mechanism was achieved through the complexation of P O ligands anchored onto the polymer skeleton of P (DVB-VPA) with thorium and uranium. Due to P (DVB-VPA) showed a larger binding force toward Th (IV) than U (VI), both q max and selectivity for Th (IV) in concentrated hydrogen nitrate media was larger than those for U (VI) on P (DVB-VPA), which has been confirmed by DFT calculations.
研究领域:
核化学
·
环境化学
·
分离科学
·
材料化学
·
放射化学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2025
·
IF 1.6
Huang Xuanhao,Liu Xingyue,Wang Yiting,Wang Zhuang,Yu Qiao,Zhou Hang,Li Rui,Ding Songdong
As one of the main radiolysis products of tri-isoamyl phosphate (TiAP) in the spent fuel reprocessing process, di-isoamyl phosphate (DiAP) can lead to a significant deterioration of TiAP in extraction performance. In this context, the effect of DiAP on the extraction and stripping behaviors of U(VI), Th(IV), and Zr(IV) for 1.1 mol/L TiAP/ n -dodecane organic phase was investigated for the first time. It has been shown that DiAP can increase the ability of TiAP to extract metal ions and inhibit the stripping, as well as promote the formation of interfacial deposition. Combined with the results of DLS, FT-IR, 31 P NMR, ESI-MS and elemental analysis, the role of DiAP in the formation of interfacial deposition was also elucidated.
研究领域:
化学工程
·
核能科学与工程
·
放射化学
✓ 已验证
DOI
高影响因子
ADSORPTION SCIENCE & TECHNOLOGY
·
2024
·
IF 2.8
Yinghao Zhuang,Shuai Sun,Kai Jia,Lei Shi,Xiangshan Yang
Thorium is a promising nuclear fuel; however, even a small amount in nuclear wastewater can cause significant radioactive pollution. Therefore, it is urgent to develop effective adsorbents for the efficient removal of thorium to solve this problem. Herein, the phytic acid modification of carboxylated Zirconium-based metal-organic framework materials (UiO-66-COOH-PA) has been obtained by rapid high-temperature carbonization, which exhibits excellent performance in removing thorium (IV) in acidic aqueous solutions. The maximum adsorption capacity of UiO-66-COOH-PA-2 (with 40% mass ratio of phytic acid) in solution reaches 315.5 mg/g at a pH of 4, which is more than twice that of the unmodified Zr-based metal organic framework (MOF) material. The adsorption kinetics of UiO-66-COOH-PA on thorium has been analyzed using two different isothermal adsorption models, the Langmuir and Freundlich isotherm adsorption models. It turns out that the Freundlich model is more suitable for the data. The thorium adsorption process reaches dynamic equilibrium very quickly, while the adsorption dynamics of UiO-66-COOH-PA on thorium follows the pseudo-second-order adsorption kinetic model. The excellent adsorption performance of UiO-66-COOH-PA-2 at low pH values indicates that adsorption material containing phosphorus is suitable for the removal of thorium especially in acidic systems. It also exhibits excellent selectivity (up to 90.2%) for Th(IV) adsorption in the presence of several coexisting rare-earth ions. Overall, the integration of phosphorus-modified in Zr-MOFs represents a significant advancement in thorium adsorption technology, offering a pathway toward more effective management of radioactive acidic waste liquid.
研究领域:
环境科学
·
核化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2017
·Vol. 8
·期 1
·1-11
·
IF 12.124
Li Yuxiang,Yang Zaixing,Wang Yanlong,Bai Zhuanling,Zheng Tao,Dai Xing,Liu Shengtang,Gui Daxiang,Liu Wei,Chen Meng,Chen Lanhua,Diwu Juan,Zhu Lingyan,Zhou Ruhong,Chai Zhifang,Albrecht-Schmitt Thomas E.,Wang Shuao
Many environmental pollutants inherently exist in their anionic forms and are therefore highly mobile in natural water systems. Cationic framework materials that can capture those pollutants are highly desirable but scarcely reported. Here we present a mesoporous cationic thorium-based MOF (SCU-8) containing channels with a large inner diameter of 2.2 nm and possessing a high surface area of 1360 m 2 g −1 . The anion-exchange properties of SCU-8 were explored with many anions including small oxo anions like ReO 4
− and Cr 2 O 7
2− as well as anionic organic dyes like methyl blue and the persistent organic pollutant, perfluorooctane sulfonate (PFOS). Both fast uptake kinetics and great sorption selectivity toward PFOS are observed. The underlying sorption mechanism was probed using quantum mechanical and molecular dynamics simulations. These computational results reveal that PFOS anions are immobilized in SCU-8 by driving forces including electrostatic interactions, hydrogen bonds, hydrophobic interactions, and van der Waals interactions at different adsorption stages.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2015
·Vol. 308
·期 1
·251-259
·
IF 1.034
Hu Chen,Liu Hui-jun,Peng Long,Sun Yun-kai,Long Wei
A specialized ethylamine-bridged β-cyclodextrins (EB β-CD) was synthetized. EB β-CD’s adsorption properties of thorium ions were performed. Experimental results show that the adsorption of thorium using the EB β-CD can achieve equilibrium within 60 min at room temperature under the condition of pH 4, the adsorbance is 10.49 mg g −1 . The results of SEM and BET nitrogen adsorption show that, EB β-CD is typical mesoporous material. According to pseudo-second-order kinetics, the adsorption of Th(IV) indicating the influence of textural properties of EB β-CD on the rate of adsorption. The thermodynamic parameters obtained showed that the adsorption process is exothermic, spontaneous process.
研究领域:
化学
·
环境科学
✓ 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）