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| 1 | Synthesis of novel nanomaterials and their application in efficient removal of radionuclides显示文摘With the development of nuclear energy, large amounts of radionuclides are inevitably released into the natural environment. It is necessary to eliminate radionuclides from wastewater for the protection of environment. Nanomaterials have been considered as the potential candidates for the effective and selective removal of radionuclides from aqueous solutions under complicated conditions because of their high specific surface area, large amounts of binding sites, abundant functional groups, pore-size controllable and easily surface modification. This review mainly summarized the recent studies for the synthesis, fabrication and surface modification of novel nanomaterials and their applications in the efficient elimination and solidification of radionuclides,and discussed the interaction mechanisms from batch experiments, spectroscopy analysis and theoretical calculations. The sorption capacities with other materials, advantages and disadvantages of different nanomaterials are compared, and at last the perspective of the novel nanomaterials is summarized. | Xiangxue Wang Long Chen Lin Wang Qiaohui Fan Duoqiang Pan Jiaxing Li Fangting Chi Yi Xie Shujun Yu Chengliang Xiao Feng Luo Jun Wang Xiaolin Wang Changlun Chen Wangsuo Wu Weiqun Shi Shuao Wang Xiangke Wang | 2019 | Science China Chemistry2019，62，8： | 20 |
| 2 | Mesoporous silica SBA-15 functionalized with phosphonate and amino groups for uranium uptake显示文摘Mesoporous silicas have a very attractive ability of sorption and enrichment of metal ions due to their huge surface area and facile functionalization by organic ligands.In this work,phosphonate-amino bifunctionalized mesoporous silica SBA-15(PA-SBA-15) as U(VI) sorbent was fabricated through post-grafting method.The obtained mesoporous silica was characterized by SEM,XRD,NMR and nitrogen sorption/desorption experiments,which revealed the existence of ordered mesoporous structure with uniform pore diameter and large surface area.The adsorptivity of PA-SBA-15 for U(VI) from aqueous solution was investigated using batch sorption technique under different experimental conditions.The preliminary results show that the U(VI) sorption by PA-SBA-15 is very quick with equilibrium time of less than 1 h,and the U(VI) uptake is as large as 373 mg/g at pH 5.5 under 95 ℃.The sorption isotherm has been successfully modeled by the Langmuir isotherm,suggesting a monolayer homogeneous sorption of U(VI) in PA-SBA-15.The sorption is pH-dependent due to the pH-dependent charge of sorbent in the aqueous solution.The thermodynamics research shows that the sorption is a feasible and endothermic process.Based on these results,PA-SBA-15 could be a promising solid phase sorbent for highly-efficient removal of U(VI) ions from waste water and enrichment of U(VI) from a solution at a very low level. | WANG XiaoLiang YUANLiYong WANG YanFei LI ZiJie LIU YaLan FENG YiXiao ZHAO YuLiang CHAI ZhiFang SHI WeiQun | 2012 | Science China Chemistry2012，55，9： | 6 |
| 3 | Solvent extraction of U(VI) by trioctylphosphine oxide using a room-temperature ionic liquid显示文摘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. | YUAN LiYong SUN Man LIAO XiangHong ZHAO YuLiang CHAI ZhiFang SHI WeiQun | 2014 | Science China Chemistry2014，57，11： | 4 |
| 4 | Easily prepared and stable functionalized magnetic ordered mesoporous silica for efficient uranium extraction显示文摘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). | Wenlu Guo Changming Nie Lin Wang Zijie Li Lin Zhu Liuzheng Zhu Zhentai Zhu Weiqun Shi Liyong Yuan | 2016 | Science China Chemistry2016，59，5： | 3 |
| 5 | Phosphonate-Decorated Covalent Organic Frameworks for Actinide Extraction: A Breakthrough Under Highly Acidic Conditions显示文摘Although solid-phase extraction is a useful approach for metal ion separation from aqueous solutions,existing sorbents suffer from low extraction effici-encies and/or instability when in contact with strong acidic media.We report here the first study on rational design and fabrication of phosphonate-decorated covalent organic frameworks,COF-IHEP1 and COF-IHEP2,for efficient and selective extraction of of uranium(VI)[U(VI)]and plutonium(IV)[Pu(IV)]from highly acidic solutions. | Jipan Yu Liyong Yuan Shuai Wang Jianhui Lan Lirong Zheng Chao Xu Jing Chen Lin Wang Zhiwei Huang Wuqing Tao Zhirong Liu Zhifang Chai John K.Gibson Weiqun Shi | 2019 | CCS Chemistry2019，1，3： | 3 |
| 6 | Kinetics process of Tb(Ⅲ)/Tb couple at liquid Zn electrode and thermodynamic properties of Tb-Zn alloys formation显示文摘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. | LiXia Luo YaLan Liu Ning Liu Kui Liu JinWen Pang LiYong Yuan ZhiFang Chai WeiQun Shi | 2017 | Science China Chemistry2017，60，6： | 2 |
| 7 | Facile Access to Uranium and Thorium Phosphaethynolate Complexes Supported by Tren: Experimental and Theoretical Study显示文摘The issue of covale nee of acti nide complexes remai ns con troversial to date.The in troducti on of 2-phosphaethy nolate anion into acti・nide complexes is expected to in vestigate the reaction mode and the bon ding property.Herei n,we describe the function alizatio n of An(Tren^(TIPS))CI(1:An=U;2:An=Th)precursors with NaOCP(dioxane)_(2.5) through salt-elimination method leading to the formation of the corresponding uranium and thorium phosphaethynolate species:[U(Tren^(TIPS))(OCP)]⑶and[Th(Tren^(TIPS))(OCP)](4). | Jipan Yu Kang Liu Qunyan Wu Bin Li Xianghe Kong Kongqiu Hu Lei Mei Liyong Yuan Zhifang Chai Weiqun Shi | 2021 | Chinese Journal of Chemistry2021，39，8： | 1 |
| 8 | Design criteria for tetradentate phenanthroline-derived heterocyclic ligands to separate Am(Ⅲ) from Eu(Ⅲ)显示文摘To design novel phenanthroline-derived soft ligands for selectively separating minor actinides from lanthanides, four tetradentate phenanthroline-derived heterocyclic ligands(BTPhen, BPyPhen, BPzPhen, and BBizPhen) were constructed and their complexation behaviors with Am(ⅡI) and Eu(ⅡI) were systematically investigated by density functional theory(DFT) coupled with relativistic small-core pseudopotential. In all the 1:1-type species, the metal ion is in the center of the cavity and coordinates with two nitrogen atoms(N1 and N1′) of the phenanthroline skeleton and the other two nitrogen atoms(N2 and N2′) of the auxiliary groups. The bond lengths of Am–N are comparable to or even shorter than those of Eu–N bonds because the ionic radii of Am(ⅡI) are larger than those of Eu(ⅡI). Additionally, the negative ΔΔGAm/Eu value for the reaction of [M(H2O)4-(NO3)3] + L → ML(NO3)3 + 4H2 O indicates that the complexation reaction of Am(ⅡI) is more energetically favorable than that of Eu(ⅡI); this can be considered as an important design criterion to screen phenanthroline-derived ligands for MA(ⅡI) extraction. According to this criterion, the selectivity of tetradentate phenanthroline-derived ligands for separating Am(ⅡI) over Eu(ⅡI) follows the order of BTPhen > BBizPhen > BPyPhen > BPzPhen. | XIAO ChengLiang WU QunYan WANG CongZhi ZHAO YuLiang CHAI ZhiFang SHI WeiQun | 2014 | Science China Chemistry2014，57，11： | 1 |
| 9 | Efficacious selective separation of U(Ⅵ) over Mo(Ⅵ) using novel 2,9-diamide-1,10-phenanthroline ligands: Liquid-liquid extraction and coordination chemistry显示文摘Uranium and molybdenum are important strategic elements. The production of ^(99)Mo and the hydrometallurgical process of uranium ore face difficult problems of separation of uranium and molybdenum.In this study, the four phenanthroline diamide ligands were synthesized, and extraction and stripping experiments were performed under different conditions to evaluate the potential application of these ligands for separation of U(Ⅵ) over Mo(Ⅵ). With the growth of alkyl chain, the solubility of ligands could be greatly improved, and the separation effect of U(Ⅵ) over Mo(Ⅵ) gradually increased. The SF_(U/Mo) were around 10,000 at 4 mol/L HNO3. Three stripping agents were tested with the stripping efficiency of Na_(2)CO_(3)(5%) > H_(2)O > HNO_(3)(0.01 mol/L). The stripping percentages of the three stripping agents were all close to unity, indicating that the ligands had the potential to be recycled. The chemical stoichiometry of U(Ⅵ) complexes with ligands was evaluated as 1:1 using electrospray ionization mass spectrometry,ultraviolet visible spectroscopy and single-crystal X-ray diffraction. The consistency between theoretical calculation and experimental results further explains the coordination mechanism. | Taoyuan Xiu Simei Zhang Peng Ren Siyan Liu Shuai Wang Hamza Shehzad Jingyang Wang Meng Zhang Guoan Ye Caishan Jiao Qunyan Wu Liyong Yuan Zhifang Chai Weiqun Shi | 2023 | Chinese Chemical Letters2023，34，11： | 1 |
| 10 | A high efficient sorption of U(VI) from aqueous solution using amino-functionalized SBA-15显示文摘 | Yalan Liu Liyong Yuan Yali Yuan Jianhui Lan Zijie Li Yixiao Feng Yuliang Zhao Zhifang Chai Weiqun Shi | 2012 | Journal of Radioanalytical and Nuclear Chemistry2012，，2： | 1 |
| 11 | Uranium(VI) adsorption on graphene oxide nanosheets from aqueous solutions显示文摘 | Zijie Li Fei Chen Liyong Yuan Yalan Liu Yuliang Zhao Zhifang Chai Weiqun Shi | 2012 | Chemical Engineering Journal2012，，： | 1 |
| 12 | Hierarchical and self-supporting honeycomb LaNi_5 alloy on nickel foam for overall water splitting in alkaline media显示文摘Ni-based metallic foams possessing large specific surfaces and open cell structures are of specific interest as catalysts or catalyst carriers for electrolysis of water.Traditional fabrication of Nickel foam limits the element modification choices to several inert transition metals only on polymer foam precursor and subsequent preparation of foam-based catalysts in aqueous solution or organic electrolyte.To expand the modification horizon,molten salt with wide electrochemical window and fast ion diffusion can achieve the reduction of highly active elements.Herein,we reported is a general and facile method to deposit directly of highly reactive element La and prepare hierarchical honeycomb LaNi_(5) alloy on Ni foam(ho-LaNi_(5)/NF).This self-supporting electrode presents excellent electrical coupling and conductivity between the Ni foam and LaNi_(5),which provides a 3D self-supported heterostructure with outstanding electrocatalytic activity and excellent durability for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).It exhibits excellent overpotential(1.86 V)comparable to commercial coupled IrO_(2)//Pt/C(1.85 V)at a high current density of 100 m A cm^(-2).This work may pave the way for fabricating novel 3D self-supported honeycomb alloy that can be applied as electrode for usage of clean energy. | Yanze Wu Yalan Liu Kui Liu Lin Wang Lei Zhang Degao Wang Zhifang Chai Weiqun Shi | 2022 | Green Energy & Environment2022，7，4： | 1 |
| 13 | High performance of phosphonate- functionalized mesoporous silica for U(VI) sorption from aque- ous solution显示文摘 | YUAN Liyong LIU Yalan SHI Weiqun | 2011 | Dalton Trans2011，40，： | 1 |
| 14 | The role of different cues in the brain mechanism on visual spatial attention显示文摘在大脑的视觉空间注意机制被事件相关的潜力(ERP ) 通过 precue 目标的视觉搜索范例在 16 个年轻题目学习技术,与由汉字和区域暗示的不同规模的专心的范围 cued。结果证明汉字暗示的反应时间为小区域暗示特别为区域暗示比那长得多。与外面的干扰,在区域暗示下面的目标刺激识别在汉字暗示下面是比那快得多的。与相比在区域暗示下面,在汉字暗示下面的目标能导致以后的 P1 的增加, N1 减少并且 P2 增加。区域暗示和汉字暗示之间的差别被干扰类型影响,这应该也被注意。在外面的干扰下面,没有重要差别在区域暗示和汉字暗示之间被发现;然而,它不是在干扰下面的原因。就外面的干扰和内部干扰之间的差别而言,我们能断定随在目标识别的困难的增加,在由在二种暗示下面的目标刺激的前面的正面的资源的消费有明显的差别。 | SONG Weiqun LUO Yuejia CHI Song JI Xunming LING Feng ZHAO Lun WANG Maobin SHI Jiannong | 2006 | Progress in Natural Science:Materials International2006，16，10： | 1 |
| 15 | A novel mesoporous material for uranium extraction,dihydroimidazole functionalized SBA-15显示文摘 | Yuan Liyong Shi Weiqun Lan Jianhui | 2012 | J Mater Chem2012，22，17： | 1 |
| 16 | Professor Zhifang Chai:Scientific contributions and achievements显示文摘Prof.Zhifang Chai,born in October 1942,is a radioanalytical chemist working at the Institute of High Energy Physics,Chinese Academy of Sciences and Soochow University.He graduated from Fudan University in 1964.As an Alexander von Humboldt Foundation fellow,he worked at Cologne University,Germany from1980 to 1982. | Yuliang Zhao Chunying Chen Weiyue Feng Zhiyong Zhang Diandou Xu Weiqun Shi Shuao Wang Yu-Feng Li | 2022 | Chinese Chemical Letters2022，33，7： | 1 |
| 17 | Highly delocalized endohedral metal in Gd@C2v(9)-C82 metallofullerenes co-crystallized with α-Se显示文摘 | Cheng Li Xuejiao J. Gao Huanli Yao Huan Huang Rongli Cui Xihong Guo Lele Zhang Bing Liu Binggang Xu Weiqun Shi Jinquan Dong Lai Feng Xingfa Gao Baoyun Sun | 2018 | Nano Research2018，11，4： | 0 |
| 18 | Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(Ⅵ)sequestration显示文摘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 particles.Herein,we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron oxide.The prepared materials exhibited excellent properties for U(VI)ions removal from aqueous solutions under various conditions.The 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 treatment.Compared 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 adsorbent.The findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation. | Jiafeng Ouyang Wenlu Guo Lin Wang Changming Nie Dadong Shao Weiqun Shi Liyong Yuan | 2023 | Frontiers of Chemical Science and Engineering2023，17，12： | 0 |
| 19 | Two tetravalent uranium silicate and germanate crystals with three membered single-ring by molten salt method:K_(2)USi_(3)O_(9)and Cs_(2)UGe_(3)O_(9)显示文摘Two tetravalent uranium silicate and germanate M_(2)U^(Ⅳ)T_(3)O_(9)(M=K,Cs;T=Si,Ge)crystals were crystalized under inert gas by molten salt flux growth method.K_(2)USi_(3)O_(9)(1)crystallizes in the monoclinic space group P1_(21)/n1 with lattice parameters a=7.1076?,b=10.4776?,c=12.2957?,γ=120°and V=915.67?^(3).Cs_(2)UGe_(3)O_(9)(2)crystallizes in a hexagonal space group P-6 with lattice constants of a=7.5138?,b=7.5138?,c=11.0114?,γ=120°and V=538.38?^(3).Bond valence calculations indicate tetravalent uranium in both structures,which contain three-membered single-ring T_(3)O_(9)^(6-) trimers.K_(2)USi_(3)O_(9) is the first uranium silicate that contains the Si_(3)O_(9)^(6-) trimers. | Xu Zhang Lei Zhang Tao Bo Shanen Huang Zhiwei Huang Weiqun Shi | 2022 | Chinese Chemical Letters2022，33，7： | 0 |
| 20 | Hierarchical assembly of uranyl metallacycles involving macrocyclic hosts显示文摘Actinide metallacycles are an emerging class of functional coordination assemblies,but multi-level assembly from metallacycle units toward hierarchical supramolecular structures are still rarely investigated.In this work,we put forward a novel supramolecular inclusion-based method through introducing two macrocyclic hosts,cucurbit[7]uril(CB[7])and cucurbit[8]uril(CB[8])to facilitate hierarchical assembly of uranyl metallacycles with higher complexity,and successfully prepare two different kinds of uranyl metallacycle-based complexes with intriguing hierarchical structures,a CB[7]-based four-member molecular necklace([4]MN)and a CB[8]-involved ring-in-ring supramolecular polymer chain.The results obtained here prove the feasibility of supramolecular inclusion for regulating coordination assembly of uranyl metallacycles and related hierarchical structures.It is believed that this method can be used to achieve the construction of actinide coordination assemblies with higher structural complexity. | Yuanyuan Liang Lei Mei Qiuyan Jin Junshan Geng Jingyang Wang Kang Liu Kongqiu Hu Jipan Yu Weiqun Shi | 2022 | Chinese Chemical Letters2022，33，7： | 0 |
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