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Issue 12, 2017
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EuNi5InH1.5−x (x = 0–1.5): hydrogen induced structural and magnetic transitions

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Abstract

The new quaternary hydride EuNi5InH1.5 has been obtained by hydrogenation of the intermetallic parent EuNi5In under extremely mild conditions, hence, at room temperature and low hydrogen pressure. Hydrogenation at slightly elevated temperatures and pressures allows for the growth of large crystals, which is a rare observation for intermetallic hydrides. EuNi5InH1.5 crystallizes in its own structure type (hP17, P[6 with combining macron]m2, a = 4.9437(6), c = 10.643(1) Å) with a unique arrangement of the intermetallic host. The hydrogen atoms prefer Ni-surrounded positions, occupying {EuNi3} and {Eu2Ni2} tetrahedral voids in the structure. Upon hydrogenation of EuNi5In an anisotropic volume expansion accompanied with a decrease of symmetry is observed. Magnetic measurements reveal antiferromagnetic ordering in the hydride below 4 K and indicate an intermediate +II/+III oxidation state for Eu both in the intermetallic phase and the hydride. X-ray photoemission spectroscopy confirms the existence of the two different oxidation states of Eu. The hydrogenation does not affect the oxidation state of Eu and the type of magnetic ordering, but exerts a strong influence on the transition temperature, crystal structure, mechanical and electrical properties. Crystallographic analysis suggests that Eu(II) and Eu(III) do not order but rather mix homogeneously on crystallographic sites. Electronic structure calculations reveal the metallic character of the hydride with several different types of chemical bonding interactions being present in the compound ranging from the formally ionic Eu–H to covalent Ni–H and delocalized metal–metal. Geometry optimization confirm the thermodynamic instability of the intermetallic host lattice for the hydride and supports a transformation into the parental structure as observed experimentally.

Graphical abstract: EuNi5InH1.5−x (x = 0–1.5): hydrogen induced structural and magnetic transitions

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Publication details

The article was received on 09 Jan 2017, accepted on 27 Jan 2017 and first published on 30 Jan 2017


Article type: Paper
DOI: 10.1039/C7TC00121E
Citation: J. Mater. Chem. C, 2017,5, 2994-3006
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    EuNi5InH1.5−x (x = 0–1.5): hydrogen induced structural and magnetic transitions

    I. Bigun, V. Smetana, Y. Mudryk, I. Hlova, M. Dzevenko, L. Havela, Y. Kalychak, V. Pecharsky and A. Mudring, J. Mater. Chem. C, 2017, 5, 2994
    DOI: 10.1039/C7TC00121E

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