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Diacylhydrazone assembled {Ln11} nanoclusters featuring a “double-boats conformation” topology: synthesis, structures and magnetism

Abstract

A family of novel Ln nanoclusters, namely, [Ln11(ovpho)4(μ-CH3O)2(μ-H2O)2(μ3-OH)6(CH3OH)4(H2O)2(NO3)8](OH)·xH2O·yCH3-OH [Ln = Gd (1), x = 1, y = 3; Ln = Tb (2), x = 1, y = 3; Ln = Dy (3), x = 0, y = 3], were obtained by the solvothermal reactions of Ln(NO3)3 with a diacylhydrazone ligand N,N’-bis(o-vanillidene)pyridine-2,6-dicarbohydrazide N-oxide (H4ovpho). Their isostructural molecular structures are composed of two crystallographically symmetric {Ln6} rings sharing a Ln3+ ion, and display an unprecedented “double boat conformation” topology that had not reported so far as we know. Besides the Ophenol, Oenol and Ooxynitride from ovpho4- ligands, the Omethaol, Oaque and Ohydroxyl also help to biridge the Ln3+ ions. The structural variation between these {Ln11} clusters and a previously reported {Gd18} nanowheel, which are all assembled by H4ovpho under the same synthetic method and reaction condition, is caused only by the change of anions of Ln salts. The magnetic investigations revealed large magnetocaloric effect (MCE) of 1, whose maximum −ΔSm value reaches 30.1 J kg−1 K−1 for ΔH = 50 kOe at 2.0 K. It is also found that 3 shows single-molecule magnets (SMMs) behavior, with an approximated energy barrier Ueff = 6.13 K and pre-exponential factor τ0 = 1.70 × 10-6 s.

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Publication details

The article was received on 28 Aug 2017, accepted on 10 Jan 2018 and first published on 11 Jan 2018


Article type: Paper
DOI: 10.1039/C7DT03179C
Citation: Dalton Trans., 2018, Accepted Manuscript
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    Diacylhydrazone assembled {Ln11} nanoclusters featuring a “double-boats conformation” topology: synthesis, structures and magnetism

    K. Wang, Z. Chen, H. Zou, S. Zhang, Y. Li, X. Zhang, W. Sun and F. Liang, Dalton Trans., 2018, Accepted Manuscript , DOI: 10.1039/C7DT03179C

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