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Issue 7, 2018
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Diacylhydrazone-assembled {Ln11} nanoclusters featuring a “double-boats conformation” topology: synthesis, structures and magnetism

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Abstract

A family of novel Ln nanoclusters, namely, [Ln11(ovpho)4(μ-CH3O)2(μ-H2O)23-OH)6(CH3OH)4(H2O)2(NO3)8](OH)·xH2yCH3OH [Ln = Gd (1), x = 1, y = 3; Ln = Tb (2), x = 1, y = 3; Ln = Dy (3), x = 0, y = 3], was obtained via 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, to our knowledge, has not yet been reported. Ophenol, Oenol and Ooxynitride from ovpho4− ligands, as well as Omethanol, Owater and Ohydroxyl help to bridge the Ln3+ ions. The structural variation between these {Ln11} clusters and a previously reported {Gd18} nanowheel, both of which are assembled by H4ovpho under the same synthetic method and reaction conditions, is caused only by changing the anions of Ln salts. Magnetic investigations revealed a 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. Additionally, it was 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.

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

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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., 2018,47, 2337-2343
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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, 47, 2337
    DOI: 10.1039/C7DT03179C

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