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Luminescence and magnetocaloric effect of Ln4 clusters (Ln = Eu, Gd, Tb, Er) bridged by CO32− deriving from the spontaneous fixation of carbon dioxide in the atmosphere

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Abstract

The synthesis and characterization of a new family of neutral tetranuclear Ln(III) complexes, [Eu4L4(CO3)(acac)2(H2O)2(CH3OH)2]·5H2O·2CH3OH (1), [Gd4L4(CO3)(acac)2 (CH3OH)4]·2CH3OH·CH2Cl2 (2), [Tb4L4(CO3)(acac)2(H2O)2(CH3OH)2]·3H2O·CH3OH (3), and [Er4L4(CO3)(acac)2(H2O)2(CH3OH)(DMF)]·H2O·CH3OH (4) (where acac is acetylacetonate, H2L is 2-(hydroxyimino)-2-[(5-methyl-2-hydroxyphenyl)methylene]hydrazide and DMF = N,N-dimethyl formamide) are reported. For complexes 1–4, by absorbing and fixing CO2 spontaneously under atmospheric conditions, with CO32− as a bridging tetradentate ligand, the four LnIII ions are bridged by two μ2-O oxygen atoms from CO32− to form a Ln4 cluster. X-ray diffraction data reveal that the non-centrosymmetric (1, 3 and 4) or centrosymmetric (2) unit has two distinct LnIII ions, nine-coordinated LnIII ions in distorted spherical capped square antiprism geometry and eight-coordinated LnIII ions in distorted triangular dodecahedron geometry. Magnetic study indicates that complex 2 can act as a cryogenic magnetic refrigerant and the magnetocaloric effect (MCE) was detected with the magnetic entropy change of −ΔSm = 21.43 J kg−1 K−1 at ΔH = 7 T and 5 K. Furthermore, the fluorescence properties of complexes 1 and 3 were also investigated. The results prove that complex 3 can show TbIII characteristic emission peaks, while for complex 1, EuIII typical emission peaks were not observed.

Graphical abstract: Luminescence and magnetocaloric effect of Ln4 clusters (Ln = Eu, Gd, Tb, Er) bridged by CO32− deriving from the spontaneous fixation of carbon dioxide in the atmosphere

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Publication details

The article was received on 21 Oct 2017, accepted on 11 Dec 2017 and first published on 14 Dec 2017


Article type: Research Article
DOI: 10.1039/C7QI00658F
Citation: Inorg. Chem. Front., 2018, Advance Article
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    Luminescence and magnetocaloric effect of Ln4 clusters (Ln = Eu, Gd, Tb, Er) bridged by CO32− deriving from the spontaneous fixation of carbon dioxide in the atmosphere

    H. Chen, W. Wang, X. Li, X. Chu, Y. Nie, Z. Liu, S. Huang, H. Shen, J. Cui and H. Gao, Inorg. Chem. Front., 2018, Advance Article , DOI: 10.1039/C7QI00658F

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