MATERIALS & DESIGN
·
2020
·
IF 6.289
Ruixi Bai,Fan Yang,Lingyi Meng,Zhigang Zhao,Wanghuan Guo,Chunqing Cai,Yang Zhang
A polyethylenimine (PEI)-scaffolded and functionalized graphene aerogel, PEI-GO-AG, was prepared and utilized as a highly selective adsorbent for the extraction of thorium (Th) (IV) from three lanthanides (Ln) (III) elements. The three dimensional (3D)-porous structure of the adsorbent was established by the cross-linking effect of PEI via a one-step hydrothermal strategy and preserved by a freeze-drying treatment to avoid the collapse of the structure. The extractive efficiency of PEI-GO-AG displayed a sensitive dependence on the beginning mass ratio of PEI/graphene oxide (GO) in the hydrothermal step because of its significant influence on the hydrophilicity and the amounts of introduced binding sites of the adsorbent.. Besides, a density function theory (DFT)-based theoretical calculation was performed, confirming the higher stability of Th (IV)-PEI-GO-AG than that of Ln (III)-PEI-GO-AG. Ascribed to these contributions, the as-prepared adsorbent showed high selectivity towards Th (IV) among three Ln (III) elements. The separation factor ( SF ) values of Th (IV) to lanthanum (La) (III), europium (Eu) (III), and lutetium (Lu) (III) were SF Th/La = 114.41, SF Th/Eu = 52.75, and SF Th/Lu = 107.81, respectively.
研究领域:
材料科学
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环境科学
·
核化学
✓ 已验证
产品关联
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
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2015
·Vol. 305
·期 2
·543-549
·
IF 1.034
Wang Youjia,Wu Lei,Yang Yunchang,Feng Wen,Yuan Lihua
A novel design based on condensation of a simple bifunctional monomer led to hydrogen-bonded oligoaramide extractant 1 that could segregate Th(IV) from rare earths(III) [REs(III)] and U(VI) under strongly acidic conditions in a highly efficient and selective fashion by solvent extraction process. The extractant demonstrated a high extractability of 94.5–99.0 % and selectivity for extraction of Th(IV) from REs in 2.0–6.0 M HNO 3 . Particularly, REs were extracted only in <9 % in a simulated multi-component mixture in 4.0 M HNO 3 , which contrasts sharply with 88 % extraction of Th(IV). The presence of NaNO 3 as the salting-out agent significantly improved the extraction selectivity of Th(IV).
研究领域:
化学
·
核化学与放射化学
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DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 2
·1472-1478
·
IF 8.897
Feng Han,Xiong Xiaohong,Gong Lele,Zhang Huiping,Xu Ying,Feng Xuefeng,Luo Feng
The reticular chemistry strategy presents a powerful molecule-design tool to tailor the physical and chemical properties of metal-organic framework (MOF). In this work, we for the first time investigated the effect of organic ligands on the radionuclide sequestration (TcO 4 − ) of thorium-organic framework. Through a coordination modulation technique, two novel isoreticular thorium-organic frameworks, namely Th-MOF-67 and Th-MOF-68, were obtained. Relative to the antetype MOF of Th-MOF-66 that shows extremely low uptake of ReO 4 − (a chemical surrogate of radioactive TcO 4 − ), the isoreticular MOFs of Th-MOF-67 and Th-MOF-68 enable ultrahigh uptake of ReO 4 − , giving an impressively 36.8-fold or 56-fold enhancement, respectively. The adsorption capacity of Th-MOF-68 is as high as 560 mg/g, exceeding most reported adsorbents for such use. The mechanism for such exceptional outstanding performance, as unveiled by both the single crystal X-ray diffraction and theoretical calculation, is due to coordination interaction for Th-MOF-67, when a tetrazolate ligand was used, or a combined effect from both coordination interaction and anion-exchange for Th-MOF-68, if using a triazolate ligand.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 22
·10093-10103
·
IF 2.7
Chunpei Yan,Qihang Peng,Linshan Peng,Zhirong Liu,Yong Qian,Tianxiang Jin
This study introduces UiO-66-PO3, a novel functionalized metal–organic framework (MOF) tailored for efficient thorium separation and enrichment from wastewater. UiO-66-PO3 was synthesized by amination reaction between UiO-66-NH2 and 2-carboxyethylphosphonic acid. Comprehensive characterization techniques confirmed its successful synthesis and revealed its unique properties. UiO-66-PO3 exhibited a remarkable theoretical maximum adsorption capacity of 320.0 mg g−1 for Th(IV) under optimized conditions. Its exceptional hydrophilicity significantly enhanced the adsorption capacity compared to UiO-66-NH2. Furthermore, UiO-66-PO3 retained over 89% of its initial adsorption capacity for Th(IV) after five adsorption–desorption cycles, highlighting excellent regeneration capabilities. UiO-66-PO3 emerges as a promising adsorbent for thorium separation due to its high adsorption capacity, regeneration performance, and tunable properties.
研究领域:
材料科学
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环境科学
·
放射化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2019
·Vol. 321
·期 2
·733-745
·
IF 1.186
Hu Peizhuo,Nan Yu,Tai Wenya,Shan Qiang,Zhong Yi,Lei Zhiwei,Liu Tonghuan,Chen Suwen,Qian Lijuan
Modification of silica gel by butanedioic anhydride (SiO 2 –BDAH) results in efficient adsorbents for removal of U(VI), Th(IV), and Eu(III) from aqueous solutions. SiO 2 –BDAH was characterized by Fourier Transform infrared spectroscopy, elemental analysis, N 2 adsorption–desorption isotherms, thermogravimetic analysis, and potentiometric titration. The effect of contact time, pH, and initial concentration of radioactive solutions and temperature on the adsorption capacity of the sorbent was investigated. The sorption equilibrium times of U(VI), Th(IV), and Eu(III) onto SiO 2 –BDAH were 1.5, 2, and about 10 h. The sorption percentages of U(VI), Th(IV), and Eu(III) increased with increased pH from 1 to 5. The sorption process of U(VI), Th(IV), and Eu(III) can be described by the Langmuir model, with sorption capacities of 5.10 × 10 −5 , 5.06 × 10 −5 , and 3.44 × 10 −5 mol/L, respectively. The enthalpy and entropy changes were all positive, whereas the free energy changes were negative. This study indicated that SiO 2 –BDAH can remove U(VI) and Th(IV) at the same time in the presence of multiple ions from waste water quickly.
研究领域:
环境科学
·
放射化学
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 70
·17586-17594
·
IF 5.236
Zi-Jian Li,Yu Ju,Zeya Zhang,Huangjie Lu,Yongxin Li,Ningjin Zhang,Xian-Long Du,Xiaofeng Guo,Zhi-Hui Zhang,Yuan Qian,Ming-Yang He,Jian-Qiang Wang,Jian Lin
Graphical The extraordinary coordination versatility of Th 4+ cation and the unexpected bridging role of formate allow polymorphism control of thorium-organic frameworks (TOFs) with five distinct phases, wherein the highest degree of interpenetration and porosity for TOFs have been achieved. The resulting TOFs exhibit considerably different adsorption behaviors toward organic dyes, thus suggesting that TOFs represent an excellent platform for structure-property relationship study. Polymorphism control of metal-organic frameworks is highly desired for elucidating structure-property relationships, but remains an empirical process and is usually done in a trial-and-error approach. We adopted the rarely used actinide cation Th 4+ and a ditopic linker to construct a series of thorium-organic frameworks (TOFs) with a range of polymorphs. The extraordinary coordination versatility of Th 4+ cations and clusters, coupled with synthetic modulation, gives five distinct phases, wherein the highest degree of interpenetration (threefold) and porosity (75.9 %) of TOFs have been achieved. Notably, the O atom on the capping site of the nine-coordinated Th 4+ cation can function as a bridging unit to interconnect neighboring secondary building units (SBUs), affording topologies that are undocumented for other tetravalent-metal-containing MOFs. Furthermore, for the first time HCOOH has been demonstrated as a bridging unit of SBUs to further induce structural complexity. The resulting TOFs exhibit considerably different adsorption behaviors toward organic dyes, thus suggesting that TOFs represent an exceptional and promising platform for structure-property relationship study.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Shulin Zheng,Hongqing Wang,Qinghua Hu,Yuyuan Wang,Jiangke Hu,Fenfen Zhou,Pengying Liu
A fluorescent sensor Hn based on β-diketone derivative for Th 4+ ions was designed and investigated, which showed high selectivity in the present of other metal ions even UO 2 2+ in CH 3 OH:H 2 O (v/v = 2:8, pH = 7.2) solution. Meanwhile, the binding mode of the sensor Hn with Th 4+ ions was found to be 1:1 with association constant of 2.46 × 10 4 M −1 . And there was linear relationship between the fluorescent intensity of Hn -Th 4+ and the concentration of Th 4+ ions covering a range of 0.06 μM–1.0 μM and the detection limit was 0.0344 μM. At the same time, the interaction properties between the sensor Hn and Th 4+ ions and the fluorescent mechanism were investigated by IR, 1 HNMR and DFT. Most importantly, this fluorescent sensor was successfully utilized for the fluorescent imaging of Th 4+ ions in living cells.
研究领域:
分析化学
·
生物无机化学
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分子影像学
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环境毒理学
·
细胞生物学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2018
·Vol. 319
·期 3
·869-880
·
IF 1.181
Ding Hanlin,Luo Xuegang,Zhang Xiaonuo,Yang Hao
In this work, a modified biomass material was successfully prepared by immobilization and inactivation method based on Aspergillus niger , and the obtained environmentally friendly Alginate-immobilized Aspergillus niger microsphere (AAM) exhibited a superior Th(IV) biosorption performance. The sorption kinetics and thermodynamic analysis were studied and showed that the sorption process is spontaneous and endothermic under the experimental conditions. Additionally, the maximum biosorption capacity of AAMs for Th(IV) can be of 303.95 mg g −1 at 313.15 K, which exhibited a superior biosorption capacity than the most reported other biomass materials. The results illustrated the biomaterial had good recyclability through immobilization and inactivation.
研究领域:
环境科学
·
微生物学
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产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2015
·Vol. 308
·期 1
·287-295
·
IF 1.034
Jing P. F.,Liu H. J.,Zhang Q.,Hu S. Y.,Hu C.,Peng L.,Lei L. L.
The adsorption of thorium(IV) [Th(IV)] was studied using a novel 6-o-monotosyl-deoxy-β-cyclodextrin inclusion complex of dibenzoyl (inclusion complex), which was acquired by the reaction of dibenzoyl and 6-OTs-β-CD with the mole ratio of 1:2. The adsorption of Th(IV) onto inclusion complex were investigated as a function of pH value, contact time, temperature, interfering ions and Th(IV) concentration using batch adsorption technique. The maximum adsorption of Th(IV) and the equilibrium adsorption capacity were found to be 89 ± 1 % and 17.83 mg g −1 respectively at pH 3.0, equilibrium time 20 min and initial Th(IV) concentration 20 mg L −1 . Adsorption kinetics, adsorption isotherm and thermodynamics were carried out.
研究领域:
化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2017
·
IF 3.981
Kai Lv,Chu-Ting Yang,Jun Han,Sheng Hu,Xiao-Lin Wang
Combining the merits of soft-templating and perchlorate oxidation methods, the first-case investigation of niobium alkylphosphonates has uncovered their unique morphology, backbone composition, thermal behavior and huge potentiality as radioanalytical separation materials. These hierarchically porous solids are random aggregates of densely stacked nanolayers perforated with worm-like holes or vesicular voids, manifesting the massif-, tower-like “polymer brush” elevated up to ∼ 150 nm driven by the minimal surface free energy principle. These coordination polymers consist of distorted niobium (V) ions strongly linked with tetrahedral alkylphosphonate building units, exposing uncoordinated phosphonate moieties and defective metal sites. Despite the amorphous features, they demonstrate multimodal porosity covering continuous micropores, segregated mesopores and fractional macropores, beneficial for the sequestration by active Lewis acid-base center. Evidenced by the maximum distribution coefficients of thorium, lanthanides reaching 9.0 × 10 4 , 9.5 × 10 4 mLg −1 and large separation factor at pH ≤ 1 20-element cocktail, this category of niobium alkylphosphonates are capable of harvesting thorium, lanthanides directly from the radionuclide surrogate, comparable to or even surpass the performance of the metal (IV) arylphosphonates counterparts. They also display appreciable SF Eu/Sm ∼20 in 1 molL −1 HNO 3 , shedding light on dual approaches to achieve the isolation of americium from curium. A combinatorial radioanalytical separation protocol has been proposed to enrich thorium and europium, revealing facile utilization of these highly stable, phosphonated hybrids in sustainable development of radioanalytical separation.
研究领域:
材料科学
·
放射化学
·
核能技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Jun Liao,Ting Xiong,Zhibo Zhao,Ling Ding,Wenkun Zhu,Yong Zhang
The development and utilization of nuclear energy produced a large amount of uranium(VI)/thorium(IV)-containing wastewater, which would be harmful to the environment. The enrichment of the radioactive ions from wastewater using a green and environmentally friendly technology was great important to the protection of water environment and the resource utilization of energy materials. In this work, a novel cow manure-derived biocarbon-based composite was prepared by impregnation-carbonization technology for the separation of thorium(IV) and uranium(VI) from water. The composite could efficiently separate the target ions under acidic condition (pH = 4.5) with high saturated separation capacities (675.1 mg/g for uranium(VI) and 710.4 mg/g for thorium(IV)), high removal percentages (97.5% for uranium(VI) and 99.8% for thorium(IV)), fast separation rates in the initial stage of separation process (10.3 mg/(g·min) for thorium(IV) and 4.6 mg/(g·min) for uranium(VI) and good reusability after five cycles. Even in 1.0 g/L of NaCl solution, the removal efficiencies still exceeded 88.4% for uranium(VI) and 93.1% for thorium(IV). These results exposed the perfect performance of the cow manure-derived biochar-based composite in thorium(IV) and uranium(VI) separation. Moreover, various models were used to fit the experimental data, which revealed that the uranium(VI)/thorium(IV) separation on the biocarbon composite was monolayer chemical adsorption and the complexation was mainly the way for capturing uranium(VI) and thorium(IV). This work might offer a new perspective for the resource management of animal manure and a prospect for the practical application of biochar in thorium(IV) and uranium(VI) recovery.
研究领域:
环境科学
·
材料科学
✓ 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）