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Unexpected structural complexity of thorium coordination polymers and polyoxo cluster built from simple formate ligands
Li, ZJ; Guo, SY; Lu, HJ; Xu, YJ; Yue, ZH; Weng, LH; Guo, XF; Lin, J; Wang, JQ
2020
Source PublicationINORGANIC CHEMISTRY FRONTIERS
ISSN2052-1553
Volume7Issue:1Pages:260-269
Subtype期刊论文
AbstractA simple binary synthetic approach with variable [HCOOH]/[Th(iv)] ratios and the addition of water resulted in the self-assembly of six novel thorium formate complexes with well-controlled structures ranging from 0D clusters and 2D layered networks to 3D frameworks. Specifically, small [HCOOH]/[Th(iv)] promoted the formation of the hexanuclear Th6O4(OH)(4)(HCOO)(12) core, a secondary building unit for the construction of 3D [Th6Na(mu(3)-O)(4)(mu(3)-OH)(4)(HCOO)(14)]center dot[NH2(CH3)(2)]center dot(DMF)(3)(H2O)(5) (Th-SINAP-1), 2D [Th-6(mu(3)-O)(4)(mu(3)-OH)(4)(HCOO)(12)(DMF)(2)]center dot(H2O)(10) (Th-SINAP-2), and 0D [Th-6(mu(3)-O)(4)(mu(3)-OH)(4)(HCOO)(12)(H2O)(6)]center dot G (Th-SINAP-3). The large [HCOOH]/[Th(iv)] inhibited the olation/oxolation reaction, affording 3D frameworks of [Th-2(HCOO)(9)]center dot[NH2(CH3)(2)]center dot(DMF)(H2O)(2) (Th-SINAP-4), [Th-2(HCOO)(9)]center dot[NH2(CH3)(2)]center dot(DMF)(H2O)(4) (Th-SINAP-5), and [Th-2(HCOO)(8)(H2O)(DMF)]center dot(H2O)(3) (Th-SINAP-6) with monomeric Th(iv) cations as the metal nodes. The addition of water not only affected the hydrolysis of Th(iv) to form nucleophilic hydroxo/oxo-aquo Th species, but also influenced the overall solid-state packing via the competition between H2O, HCOO-, OH-/O2-, and DMF for coordination with Th4+ cations. This unexpected structural complexity of thorium formates opens a new avenue for the targeted design and synthesis of atypical coordination polymers, e.g. open-framework materials of actinides, for applications in diverse fields such as radionuclide adsorption.
KeywordMETAL-ORGANIC FRAMEWORKS OXO CLUSTER HEXANUCLEAR HYDROLYSIS PLUTONIUM DEFECTS UIO-66 SEPARATION MOLECULES CHEMISTRY
DOI10.1039/c9qi01263j
Indexed BySCI
Language英语
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/33254
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Chinese Acad Sci, Shanghai Inst Appl Phys, CAS Key Lab Interfacial Phys & Technol, 2019 Jia Luo Rd, Shanghai 201800, Peoples R China
2.Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China
3.Washington State Univ, Dept Chem, Pullman, WA 99164 USA
Recommended Citation
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Li, ZJ,Guo, SY,Lu, HJ,et al. Unexpected structural complexity of thorium coordination polymers and polyoxo cluster built from simple formate ligands[J]. INORGANIC CHEMISTRY FRONTIERS,2020,7(1):260-269.
APA Li, ZJ.,Guo, SY.,Lu, HJ.,Xu, YJ.,Yue, ZH.,...&Wang, JQ.(2020).Unexpected structural complexity of thorium coordination polymers and polyoxo cluster built from simple formate ligands.INORGANIC CHEMISTRY FRONTIERS,7(1),260-269.
MLA Li, ZJ,et al."Unexpected structural complexity of thorium coordination polymers and polyoxo cluster built from simple formate ligands".INORGANIC CHEMISTRY FRONTIERS 7.1(2020):260-269.
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