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| 1 | 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 |
| 2 | 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 |
| 3 | 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 |
| 4 | Boron rings containing planar octacoordinate iron and cobalt显示文摘The boron rings containing planar octacoordinate transition metals, D8h FeB82-, CoB8- and CoB83+, C2v FeB8, D2h CoB8+ and CoB8, are optimized with all real vibrational frequencies at the B3LYP/6-311+G* level of the theory. The D8h FeB82- and CoB8- isomers are global minima, while D8h CoB83+ is only local minimum. The electronic structure character of these systems is revealed by natural bond orbital (NBO) analysis, showing that the boron rings containing planar octacoordinate transition metals have stability and aromaticity with six π electrons. The aromaticity is confirmed by nucleus independent chemical shifts (NICS) calculations. | WU QunYan TANG YuPeng ZHANG XiuHui | 2009 | Science China Chemistry2009，52，3： | 1 |
| 5 | Trans-dimensional Bayesian geoacoustic inversion in shallow water显示文摘To deal with the inversion problem when the spatial structure of seaffoor sediments is unknown, a trans-dimensional particle filter method is proposed, where the cross-spectral density of the pressure field is used to estimate the sediment layering structure and geoacoustic parameters. The simulation results show that the number of sediment layers and geoacoustic parameters can be effectively estimated using the proposed method, and the parallel particle calculation makes this method more efficient than reversible jump Monte Carlo Markov chain(rjMCMC) sampling. A linear frequency-modulated signal received by a vertical line array in the South China Sea is processed using the proposed trans-dimensional particle filter. The inversion results of the sediment layers and geoacoustic parameters are similar to those acquired by rjMCMC inversion. The number of sediment layers and the posterior probability density of parameters can be effectively estimated using this method. | WU Weiwen REN Qunyan LU Licheng Guo Shengming MA Li | 2023 | Chinese Journal of Acoustics2023，42，4： | 0 |
| 6 | Theoretical investigation on the solution behaviors of Ba and Zr in uranium dinitride显示文摘The in-pile performance of ceramic fuels is significantly affected by the fission products. In this work, we have performed first-principles density functional theoretical calculations to study the interaction between metallic fission products(barium and zirconium) and the uranium dinitride UN2 matrix. The thermodynamic properties and bonding nature of Ba and Zr atoms in different incorporation configurations indicate that Zr is more soluble in UN2 matrix than Ba. With increasing the concentration of the impurity atoms, Zr-doped UN2 exhibits a slight tendency to contract, while Ba-doped UN2 tends to swell. Based on the competition between steric effect and chemical interaction, various incorporation trends for Ba and Zr in UN2 as well as in UN have been understood. | Yujuan Zhang Jianhui Lan Qunyan Wu Congzhi Wang Tao Bo Zhifang Chai Weiqun Shi | 2015 | Science China(Information Sciences)2015，58，12： | 0 |
| 7 | Theoretical studies on the complexation of Eu(Ⅲ) and Am(Ⅲ) with HDEHP: structure, bonding nature and stability显示文摘Separation of trivalent lanthanides(Ln(Ⅲ)) and actinides(An(Ⅲ)) is a key issue in the advanced spent nuclear fuel reprocessing. In the well-known trivalent actinide lanthanide separation by phosphorus reagent extraction from aqueous komplexes(TALSPEAK) process, the organophosphorus ligand HDEHP(di-(2-ethylhexyl) phosphoric acid) has been used as an efficient reagent for the partitioning of Ln(Ⅲ) from An(Ⅲ) with the combination of a holdback reagent in aqueous lactate buffer solution. In this work, the structural and electronic properties of Eu^(3+) and Am^(3+) complexes with HDEHP in nitric acid solution have been systematically explored by using scalar-relativistic density functional theory(DFT). It was found that HDEHP can coordinate with M(Ⅲ)(M=Eu, Am) cations in the form of hydrogen-bonded dimers HL_2^-(L=DEHP), and the metal ions prefer to coordinate with the phosphoryl oxygen atom of the ligand. For all the extraction complexes, the metal-ligand bonds are mainly ionic in nature. Although Eu(Ⅲ) complexes have higher interaction energies, the HL_2^- dimer shows comparable affinity for Eu(Ⅲ) and Am(Ⅲ) according to thermodynamic analysis, which may be attributed to the higher stabilities of Eu(Ⅲ) nonahydrate. It is expected that this work could provide insightful information on the complexation of An(Ⅲ) and Ln(Ⅲ) with HDEHP at the molecular level. | juan luo congzhi wang jianhui lan qunyan wu yuliang zhao zhifang chai changming nie weiqun shi | 2016 | Science China Chemistry2016，59，3： | 0 |
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