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  • Title: Construction of Hybrid Bimetallic Uranyl Compounds Based on a Preassembled Terpyridine Metalloligand.
    Author: Kong X, Hu K, Mei L, Wu Q, Huang Z, Liu K, Chai Z, Nie C, Shi W.
    Journal: Chemistry; 2021 Jan 26; 27(6):2124-2130. PubMed ID: 33151581.
    Abstract:
    Six hybrid uranyl-transition metal compounds [UO2 Ni(cptpy)2 (HCOO)2 (DMF)(H2 O)] (1), [UO2 Ni(cptpy)2 (BTPA)2 ] (2), [UO2 Fe(cptpy)2 (HCOO)2 (DMF)(H2 O)] (3), [UO2 Fe(cptpy)2 (BTPA)2 ] (4), [UO2 Co(cptpy)2 (HCOO)2 (DMF)(H2 O)] (5), and [UO2 Co(cptpy)2 (BTPA)2 ] (6), based on bifunctional ligand 4'-(4-carboxyphenyl)-2,2':6',2''-terpyridine (Hcptpy) are reported (H2 BTPA = 4,4'-biphenyldicarboxylic acid). Single-crystal XRD revealed that all six compounds feature similar metalloligands, which consist of two cptpy- anions and one transition metal cation. The metalloligand M(cptpy)2 can be considered to be an extended linear dicarboxylic ligand with length of 22.12 Å. Compounds 1, 3, and 5 are isomers, and all of them feature 1D chain structures. The adjacent 1D chains are connected together by hydrogen bonds and π-π interactions to form a 3D porous structure, which is filled with solvent molecules and can be exchanged with I2 . Compounds 2, 4, and 6 are also isomers, and all of them feature 2D honeycomb (6,3) networks with hexagonal units of dimensions 41.91×26.89 Å, which are the largest among uranyl compounds with honeycomb networks. The large aperture allows two sets of equivalent networks to be entangled together to result in a 2D+2D→3D polycatenated framework. Remarkably, these uranyl compounds exhibit high catalytic activity for cycloaddition of carbon dioxide. Moreover, the geometric and electronic structures of compounds 1 and 2 are systematically discussed on the basis of DFT calculations.
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