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Issue 8, 2018
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Two tetranuclear 3d–4f heterometal complexes Mn2Ln2 (Ln = Dy, Gd): synthesis, structure, magnetism, and electrocatalytic reactivity for water oxidation

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Abstract

In this present study, two Mn/Ln clusters, [Mn2Ln2(O2CMe)6(pdmH)2L](NO3)·H2O (Ln = Dy (1), Gd (2)), have been synthesized and experimentally investigated by X-ray crystallography, PXRD, magneto- and electrochemistry. By X-ray analysis, it is shown that the two complexes are isomorphous, both possessing one [MnIIMnIIILnIII23-O)2]6+ core with four metal atoms in one plane arranged in a butterfly conformation. This is the first time that mixed-valent manganese (MnII and MnIII) and LnIII heterometal tetranuclear complexes have been isolated and characterized. Magnetic susceptibility measurements reveal that compounds 1 and 2 both display overall weak ferromagnetic exchanges between the metal ions within the clusters. The temperature dependencies of the out-of-phase (χM′) and in-phase (χM′) ac susceptibility signals exhibit no significant frequency-dependency for compounds 1 and 2, which suggests that the two complexes may not be SMMs. Electrochemical studies indicate that compounds 1 and 2 can both catalyze water oxidation at a potential of ∼1.70 V with an overpotential of ∼880 mV vs. NHE, which could be due to a cooperative catalytic effect between the manganese and lanthanide ions.

Graphical abstract: Two tetranuclear 3d–4f heterometal complexes Mn2Ln2 (Ln = Dy, Gd): synthesis, structure, magnetism, and electrocatalytic reactivity for water oxidation

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Publication details

The article was received on 10 Jan 2018, accepted on 08 Mar 2018 and first published on 09 Mar 2018


Article type: Paper
DOI: 10.1039/C8NJ00149A
Citation: New J. Chem., 2018,42, 5798-5805
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    Two tetranuclear 3d–4f heterometal complexes Mn2Ln2 (Ln = Dy, Gd): synthesis, structure, magnetism, and electrocatalytic reactivity for water oxidation

    T. Lan, W. Gao, C. Chen, H. Wang, M. Wang and Y. Fan, New J. Chem., 2018, 42, 5798
    DOI: 10.1039/C8NJ00149A

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