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EuNi2P4, the first magnetic unconventional clathrate prepared via a mechanochemically assisted route

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Abstract

For the first time, a magnetic unconventional clathrate EuNi2P4 has been prepared from the elements via a combined mechanochemical and solid-state route. Its crystal and electronic structure, magnetic and transport properties as well as lattice dynamics were elucidated. It crystallizes in the orthorhombic space group Fddd (Z = 8) with unit cell parameters a = 5.1852(1) Å, b = 9.4834(1) Å, and c = 18.9893(2) Å, V = 933.78(1) Å3 at room temperature. Its crystal structure can be described as a covalent Ni–P framework forming a twisted Kelvin cell with Eu2+ guest cations occupying the voids of this framework, which is supported by chemical bonding analysis based on the electron localization function topology. Eu2+ guests sit inside the oversized cages with a coordination number of 24 and exhibit strong rattling, which manifests in both thermodynamic properties and Raman spectra. The compound is metallic and exhibits a rather low thermal conductivity of ∼4 W K−1 m−1 at high temperature along with a positive Seebeck coefficient. The magnetism of EuNi2P4 is predetermined by Eu2+ (4f7) with dominant antiferromagnetic interactions. According to the magnetic susceptibility, heat capacity and resistivity measurements, EuNi2P4 undergoes three phase transitions at ∼2.5 K, 6.1 K and 11.3 K in zero magnetic field.

Graphical abstract: EuNi2P4, the first magnetic unconventional clathrate prepared via a mechanochemically assisted route

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Article information


Submitted
01 Dec 2019
Accepted
19 Jan 2020
First published
20 Jan 2020

Inorg. Chem. Front., 2020, Advance Article
Article type
Research Article

EuNi2P4, the first magnetic unconventional clathrate prepared via a mechanochemically assisted route

I. V. Plokhikh, N. Khan, A. A. Tsirlin, A. N. Kuznetsov, D. O. Charkin, A. V. Shevelkov and A. Pfitzner, Inorg. Chem. Front., 2020, Advance Article , DOI: 10.1039/C9QI01566C

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