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Unexpected Roles of Alkali-Metal Cations in the Assembly of Low-Valent Uranium Sulfate Molecular Complexes
Yue, ZH; Guo, XF; Feng, ML; Lin, YJ; Ju, Y; Lin, X; Zhang, ZH; Guo, XJ; Lin, J; Huang, YY; Wang, JQ
2020
Source PublicationINORGANIC CHEMISTRY
ISSN0020-1669
Volume59Issue:4Pages:2348-2357
Subtype期刊论文
AbstractThe directing effect of coordinating ligands in the formation of uranium molecular complexes has been well established, but the role of counterions in metal-ligand interactions remains ambiguous and requires further investigation. In this work, we describe the targeted isolation, through the choice of alkali-metal ions, of a family of tetravalent uranium sulfates, showing the influence of the overall topology and, unexpectedly, the U-IV nuclearity upon the inclusion of such countercations. Analyses of the structures of uranium(IV) oxo/hydroxosulfate oligomeric species isolated from consistent synthetic conditions reveal that the incorporation of Na+ and Rb+ promotes the crystallization of OD discrete clusters with a hexanuclear [U6O4(OH)(4)(H2O)(4)](12+) core, whereas the larger Cs+ ion allows for the isolation of a 2D-layered oligomer with a less condensed trinuclear [U-3(O)](10+) center. This finding expands the prevalent view that counterions play an innocent role in molecular complex synthesis, affecting only the overall packing but not the local oligomerization. Interestingly, trends in nuclearity appear to correlate with the hydration enthalpies of alkali-metal cations, such that the alkali-metal cations with larger hydration enthalpies correspond to more hydrated complexes and cluster cores. These findings afford new insights into the mechanism of nucleation of U-IV, and they also open a new path for the rational design and synthesis of targeted molecular complexes.
KeywordSTATE STRUCTURAL CHEMISTRY DIMENSIONAL REDUCTION CRYSTAL-STRUCTURE FISSION-PRODUCTS CLUSTER HEXANUCLEAR COORDINATION SPECIATION HYDROLYSIS SELENITES
DOI10.1021/acs.inorgchem.9b03182
Indexed BySCI
Language英语
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/33252
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
4.Washington State Univ, Dept Chem, Pullman, WA 99164 USA
5.Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
6.Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
7.Changzhou Univ, Jiangsu Key Lab Adv Catalyt Mat & Technol, Changzhou 213164, Jiangsu, Peoples R China
8.Shanghai Normal Univ, Educ Minist, Key Lab Resource Chem, Shanghai 200234, Peoples R China
9.Shanghai Normal Univ, Dept Chem & Chem Engn, Shanghai Key Lab Rare Earth Funct Mat, Shanghai 200234, Peoples R China
Recommended Citation
GB/T 7714
Yue, ZH,Guo, XF,Feng, ML,et al. Unexpected Roles of Alkali-Metal Cations in the Assembly of Low-Valent Uranium Sulfate Molecular Complexes[J]. INORGANIC CHEMISTRY,2020,59(4):2348-2357.
APA Yue, ZH.,Guo, XF.,Feng, ML.,Lin, YJ.,Ju, Y.,...&Wang, JQ.(2020).Unexpected Roles of Alkali-Metal Cations in the Assembly of Low-Valent Uranium Sulfate Molecular Complexes.INORGANIC CHEMISTRY,59(4),2348-2357.
MLA Yue, ZH,et al."Unexpected Roles of Alkali-Metal Cations in the Assembly of Low-Valent Uranium Sulfate Molecular Complexes".INORGANIC CHEMISTRY 59.4(2020):2348-2357.
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