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Radiation-Assisted Synthesis of Crown Ether-Modified Covalent Organic Frameworks for Lithium Isotope Separation

CCS Chemistry 2024年第10期6卷 2594-2606页

作者： Shouchao Zhong Yue Wang Jianhui Lan Mingshu Xie Yiqian Wu Jiuqiang Li Fujian Liu Lilong Jiang Jing Peng liyong yuan Maolin Zhai Weiqun Shi Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental Science Key Laboratory of Polymer Chemistry and Physics of the Ministry of EducationCollege of Chemistry and Molecular EngineeringBeijing National Laboratory for Molecular SciencesPeking UniversityBeijing 100871 National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou350002 Fujian Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049

γ-ray radiation-induced grafting strategy was first employed to immobilize 4-aminobenzo-15-crown-5 onto a covalent organic framework(COF).This endeavor culminated in the successful synthesis of a class of two-dimensional crown ether-modified COFs(named[15C5]n%-(TzDa-G-x%)),marking the maiden utilization of COFs in the realm of^(6)Li/^(7)Li isotope *** COFs exhibited swifter adsorption kinetics than alternative *** them,[15C5]_(57%)-(TzDa-G-50%)with its excellent crystallinity,porosity,and stability exhibited the best performance in Li+adsorption and^(6)Li/^(7)Li isotope *** Li+adsorption in acetonitrile achieved a capacity of 3.6 mg·g^(−1)within 30 min and a saturation capacity of 7.3 mg·g^(−1).The single-stage separation factor of^(6)Li/^(7)Li isotopes was 1.014±*** results of dynamic adsorption column experiments showed that the packed column made of[15C5]_(57%)-(TzDa-G-50%)maintained stable performance during four cycles of Li+adsorptionelution,with over 99%Li+removal rate in *** crown ether-modified COF has potential application in^(6)Li/^(7)Li isotope separation,and this radiation-assisted synthesis strategy is expected to become universal in the modification of COFs for diverse applications.

关键词： covalent organic framework gamma radiation modification crown ether ^(6)Li/^(7)Li isotope separation adsorption column

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Towards understanding the correlation between UO_2^(2+) extraction and substitute groups in 2,9-diamide-1,10-phenanthroline

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Science China Chemistry 2018年第10期61卷 1285-1292页

作者： Xinrui Zhang liyong yuan Zhifang Chai Weiqun Shi Laboratory of Nuclear Energy Chemistry Institute of High Energy Physics Chinese Academy of Sciences School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions Soochow University

2,9-Diamide-1,10-phenanthroline(DAPhen)ligands represent a new family of tetradentate extractants given their strong affinity to actinides and the CHON *** this family,N,N′-diethyl-N,N′-ditolyl-2,9-diamide-1,10-phenanthroline(Et-TolDAPhen),initially reported by us,exhibits excellent selectivity towards actinides(U,Th,Am,Pu)over lanthanides and thus can be potentially applied in the group actinide extraction(GANEX)process for the group separation of *** this article,by tailoring the lengths of alkyl chains,we synthesized other four DAPhen ligands with different substitute groups in the diamide moieties,and characterized the relationship between properties and substitute groups of DAPhen *** extraction results show that three of the ligands exhibit high performance in UO_2^(2+)extraction from an acidic solution and the extracted UO_2^(2+)can be easily stripped by only using ultrapure *** titration confirms that UO_2^(2+)combined with all the four ligands in 1:1 *** extended X-ray absorption finestructure(EXAFS)study shows that six donor atoms comprise the first equatorial shell of the UO_2^(2+)ions bonded by the DAPhen ligands,among which two nitrogen and two oxygen atoms are from the DAPhen ligand,while other two oxygen atoms are from one nitrate *** article promises to provide basic data for assessing the feasibility of this kind of DAPhen ligands applied in actinides separation from nuclear wastes.

关键词： 2,9-diamide-1,10-phenanthroline UO2^2+ extraction UV-Vis titration EXAFS

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A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications for the "versatility" of these materials as solid sorbents

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1632-1642页

作者： Xiyuan Bu Ming Tian Hongqing Wang Lin Wang liyong yuan Weiqun Shi Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

Although metal–organic frameworks offer a new platform for developing versatile sorption materials,yet coordinating the functionality,structure and component of these materials remains a great *** depends on a comprehensive knowledge of a“real sorption mechanism”.Herein,a ternary mechanism for U(Ⅵ)uptake in metal–organic frameworks was *** MIL-100s(Al,Fe,Cr)were prepared and studied for their ability to sequestrate U(Ⅵ)from aqueous *** a result,MIL-100(Al)performed the best among the tested materials,and MIL-100(Cr)performed the *** nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(Ⅵ)uptake in the three metal–organic frameworks involves different ***,hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s(Al,Fe)by exchanging with hydrogen ions of terminal hydroxyl groups(Al-OH_(2),Fe-OH_(2)),and/or,hydrated uranyl ions are bound directly to Al(Ⅲ)center in MIL-100(Al)through a strong inner-sphere *** MIL-100(Cr),however,the U(Ⅵ)uptake is attributed to electrostatic ***,the sorption mechanism is also pH and ionic strength *** present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism,which helps to construct effective metal–organic frameworks-based sorbents for water purification.

关键词： U(Ⅵ) metal–organic frameworks adsorption mechanism metal node

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Electrochemical properties of gadolinium on liquid gallium electrode in LiCl-KCl eutectic

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Journal of Rare Earths 2018年第6期36卷 656-661页

作者： Bo Li Kui Liu Jingwen Pang liyong yuan Yalan Liu Mingzhang Lin School of Nuclear Science and Technology University of Science and Technology of ChinaHefei230026China Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing100049China

This work presents the electrochemical properties of gadolinium(Gd), a significant rare earth element in spent nuclear fuel(SNF), in the LiCl-KCl eutectic. To explore thermodynamic properties of Gd at the liquid gallium(Ga) electrode, experiments were performed both on the inert tungsten(W) and liquid gallium(Ga) electrode at different temperatures in a range from 723 to 823 K, which show that the Gd metal can be oxidized to Gd(Ⅲ) by exchanging of 3 electrons. Electrochemical techniques including cyclic voltammetry(CV), open circuit potential(OCP), potentiostatic electrolysis and galvanostatic electrolysis were utilized to detect the electrochemical behavior and evaluate standard apparent potential of the Gd(Ⅲ)/Gd couple,and E(Gd(Ⅲ)/Gd)*=-3.456 + 6.2×10-4T(±0.046)( vs Cl2/Cl-) is *** addition, electromotive force(EMF) and coulometric titration were employed to calculate the activity and activity coefficient of Gd in metal Ga. After calculation, the activity is 1.791×10-15at 723 K and function of activity coefficient and temperature is lgγ = 3.485-10927/T(±0.0875).

关键词： LiCl-KCl eutectic Electrochemical properties Gadolinium Liquid Ga Rare earths

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Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(Ⅵ)sequestration

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Frontiers of Chemical Science and Engineering 2023年第12期17卷 2037-2049页

作者： Jiafeng Ouyang Wenlu Guo Lin Wang Changming Nie Dadong Shao Weiqun Shi liyong yuan School of Environmental and Biological Engineering Nanjing University of Science and TechnologyNanjing 210094China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

Although mesoporous silica with magnetically hybridized two-dimensional channel structures has been well studied in recent years,it remains a challenge to fabricate the counterpart with macroporous three-dimensional cubic structures since the highly acidic preparation conditions lead to dissolution of magnetic ***,we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron *** prepared materials exhibited excellent properties for U(VI)ions removal from aqueous solutions under various *** experimental data show that the U(VI)adsorption features fast adsorption kinetics,high adsorption capacity and ideal selectivity toward U(VI).The adsorption process is of spontaneous and endothermic nature and ionic strength independence,and the adsorbents can be easily regenerated by acid *** to pristine KIT-6,the introduction of magnetism does not reduce the efficiency of the material to remove U(VI)while exerting its role as a recovery *** findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation.

关键词： magnetic nanoparticle 3D mesoporous silica amino functionalization adsorption of U(VI) acid resistance

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Solvent extraction of U(VI) by trioctylphosphine oxide using a room-temperature ionic liquid

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Science China Chemistry 2014年第11期57卷 1432-1438页

作者： yuan liyong SUN Man LIAO XiangHong ZHAO YuLiang CHAI ZhiFang SHI WeiQun Key Laboratory of Nuclear Radiation and Nuclear Energy Technology Key Laboratory for Biomedical Effects of Nanomaterials & Nanosafety Institute of High Energy Physics Chinese Academy of Sciences School of Radiological & Interdisciplinary Sciences Soochow University

The unique physical and chemical properties of room-temperature ionic liquids(RTILs) have recently received increasing attention as solvent alternatives for possible application in the field of nuclear industry, particularly in liquid-liquid separations of radioactive nuclides. We investigated solvent extraction of U(VI) from aqueous solutions into a commonly used ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([C4mim][NTf2]) using trioctylphosphine oxide(TOPO) as an extractant. The effects of contact time, TOPO concentration, acidity, and nitrate ions on the U(VI) extraction are discussed in detail. The extraction mechanism was proposed based on slope analysis and UV-Vis measurement. The results clearly show that TOPO/[C4mim][NTf2] provides a highly efficient extraction of U(VI) from aqueous solution under near-neutral conditions. When the TOPO concentration was 10 mmol/L, the extraction of 1 mmol/L U(VI) was almost complete(> 97%). Both the extraction efficiency and distribution coefficient were much larger than in conventional organic solvents such as dichloromethane. Slope analysis confirmed that three TOPO molecules in [C4mim][NTf2] bound with one U(VI) ion and one nitrate ion was also involved in the complexation and formed the final extracted species of [UO2(NO3)(TOPO)3]+. Such a complex suggests that extraction occurs by a cation-exchange mode, which was subsequently evidenced by the fact that the concentration of C4mim+ in the aqueous phase increased linearly with the extraction percent of U(VI) recorded by UV-Vis measurement.

关键词： uranium solvent extraction ionic liquid trioctylphosphine oxide

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Kinetics process of Tb(Ⅲ)/Tb couple at liquid Zn electrode and thermodynamic properties of Tb-Zn alloys formation

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Science China Chemistry 2017年第6期60卷 813-821页

作者： LiXia Luo YaLan Liu Ning Liu Kui Liu JinWen Pang liyong yuan ZhiFang Chai WeiQun Shi Laboratory of Nuclear Energy Chemistry Institute of High Energy Physics Chinese Academy of Sciences Key Laboratory of Radiation Physics and Technology Ministry of Education Institute of Nuclear Science and Technology Sichuan University

Electrochemical properties of rare-earth elements in the LiCl-KCl eutectic are important for the pyrometallurgical recycling process of spent nuclear fuels. In this work, the electrochemical properties of Tb(Ⅲ)/Tb(0) couple were studied by the cyclic voltammetry(CV) at a liquid Zn pool electrode. The results showed that this electrochemical reaction is quasi-reversible with mixed reversible diffusion control and the charge transfer control. The diffusion coefficient of Tb(Ⅲ) was determined to be in the order of ~10.5 cm2 s.1. Moreover, kinetic parameters, such as the standard rate constants(ks) and charge transfer coefficient(α) for the electroreduction of Tb(Ⅲ) to Tb(0) at the liquid Zn electrode, were calculated by the Nicholson method at 873 K. Additionally, it was found that Tb-Zn intermetallic compounds were easily to be formed in the measurements. Hence, the reduction process of Tb(Ⅲ)/Tb(0) couple on the Zn-coated Mo electrode was also studied to obtain more information of the Tb-Zn intermetallic compounds. Electrochemical signals stemming from various intermetallic compounds associated with TbZn12, Tb2Zn17, Tb13Zn58, Tb3Zn11, TbZn3, TbZn2 and TbZn, were observed. The thermodynamic data were thereafter estimated by applying the emf method at 823–923 K. The standard formation Gibbs energies and the standard equilibrium constant of each Tb-Zn intermetallic compounds were also calculated. Finally, enthalpies and entropies of formation and the apparent standard potentials of various Tb-Zn intermetallic compounds were also obtained.

关键词： Tb liquid Zn electrode kinetic parameters thermodynamic properties molten salt

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A Certified Cubic B-Spline Interpolation Method with Tangential Direction Constraints

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Journal of Systems Science & Complexity 2024年第3期37卷 1271-1294页

作者： HE Shitao SHEN liyong WU Qin yuan Chunming School of Mathematical Sciences University of Chinese Academy of SciencesBeijing 100049China KLMM Academy of Mathematics and Systems ScienceChinese Academy of SciencesBeijing 100190China

Curve interpolation with B-spline is widely used in various areas. This problem is classic and recently raised in application scenario with new requirements such as path planning following the tangential vector field under certified error in CNC machining. This paper proposes an algorithm framework to solve Hausdorff distance certified cubic B-spline interpolation problem with or without tangential direction constraints. The algorithm has two stages: The first stage is to find the initial cubic B-spine fitting curve which satisfies the Hausdorff distance constraint;the second stage is to set up and solve the optimization models with certain constraints. Especially, the sufficient conditions of the global Hausdorff distance control for any error bound are discussed, which can be expressed as a series of linear and quadratic constraints. A simple numerical algorithm to compute the Hausdorff distance between a polyline and its B-spline interpolation curve is proposed to reduce our *** results are presented to show the advantages of the proposed algorithms.

关键词： Cubic B-spline Hausdorff distance interpolation tangential direction

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Easily prepared and stable functionalized magnetic ordered mesoporous silica for efficient uranium extraction

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Science China Chemistry 2016年第5期59卷 629-636页

作者： Wenlu Guo Changming Nie Lin Wang Zijie Li Lin Zhu Liuzheng Zhu Zhentai Zhu Weiqun Shi liyong yuan School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China State Key Laboratory of NBC Protection for Civilian Beijing 102205China

Functionalized magnetic Fe_3O_4@SiO_2 composite nanoparticles were prepared by simply embedding iron oxide nanoparticles into MCM-41 through one-step synthesis process, followed by aminopropyls grafting on the mesopore channels, aiming to efficiently and conveniently uptake U(VI) from aqueous solution. The resultant material possesses highly ordered mesoporous structure with large surface area, uniform pore size, excellent thermal stability, quick magnetic response, and desirable acids resistance, confirmed by Fourier transform infrared spectroscopy(FTIR), scanning electron microscopy(SEM), N_2 adsorption/desorption experiments, powder X-ray diffraction(PXRD), and thermogravimetric analysis(TGA). Detailed U(VI) sorption test indicated that this material is indeed an effective U(VI) sorbent with fast sorption kinetics of less than 2 h, large sorption capacity of 160 mg/g at p H 5.0±0.1, and desirable selectivity towards U(VI) ions over a range of competing metal ions. The absorbed U(VI) can be easily desorbed by 0.01 mol/L or more concentrated HNO_3 solution, and the reclaimed sorbent can be reused with no obvious decrease of sorption capacity even after 4 sorption-desorption cycles. The present results suggest the vast opportunities of this kind of magnetic composite on the solid-phase extraction of U(VI).

关键词： aminopropyls magnetic ordered mesoporous silica uranium sorption

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The radiolytic behavior and mechanism of calixarene crown ether under γ-irradiation

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Chinese Science Bulletin 2013年第14期58卷 1663-1669页

作者： AO YinYong PENG Jing ZHANG YouWei yuan liyong YU ChuHong LI JiuQiang ZHAI MaoLin Beijing National Laboratory for Molecular Sciences (BNLMS) Department of Applied Chemistry College of Chemistry and Molecular Engineering Peking University Institute of High Energy Physics Chinese Academy of Sciences

Bis(2-propyloxy)calix[4]crown-6 (BPC6) is an effective separation agent for cesium removing from spent nuclear fuel. The study on radiolytic behavior of BPC6 itself under γ-irradiation was required for evaluating its feasibility of practical application. It was found that BPC6 exhibited excellent radiation stability at dose less than 100 kGy. However, the isopropyl groups in BPC6 under- went oxidation and dealkylation to form carbonyl groups and phenolic hydroxyl groups at dose above 300 kGy, respectively. When the dose was more than 1000 kGy, the ring opening of crown ether structure of BPC6 resulted in the formation of phenolic hydroxyl groups as well. The formation of radiolytic products containing phenolic hydroxyl groups during the irradiation of BPC was confirmed by using FeCl 3 as a probe. Combining with the radiolytic behavior of two model chemicals (1-isopropoxybenzene and benzo-18-crown-6 ether), the radiolytic behavior and mechanism of BPC6 under -irradiation was testified further.

关键词：行为冠醚机制杯芳烃异丙氧基辐射稳定性烷基化反应酚羟基

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