Issue 42, 2021

Synthesis of (MgCoNiCuZn)O entropy-stabilized oxides using solution-based routes: influence of composition on phase stability and functional properties

Abstract

Formation of the (MgCoNiCuZn)O entropy-stabilized oxide and of the related 4-cation derivatives is achieved using a Pechini route based on cation chelation and subsequent immobilization in a polymer gel. Calcination of the as-obtained resins yields a phase separation into fine-grained oxide precursors, but the extent of this phase separation depends on the formulation. In particular, absence of copper leads to the formation of a multi-element oxide with a rock-salt structure including most of the cations except for Zn at a temperature as low as 450 °C. Starting from these charred resins, the temperature-composition phase diagram of the equimolar mixtures is investigated by in situ powder X-ray diffraction. This study highlights the specific role of copper, with an onset of phase transformation into a phase-pure (MgCoNiZn)O mixed oxide at a temperature 25 °C lower than the one found for the 5-cation reference. Removal of the magnesium and nickel elements has also a pronounced impact on phase stability and lattice distortions after quenching, suggesting a description in terms of site percolation within a (MgNi)O templating network. The optical, dielectric and magnetic properties of the 4-cation compositions with respect to the 5-element high-entropy oxide are discussed in relation with the structural distortions induced at the local scale by the Jahn–Teller Cu2+ ions and at longer range through the destabilization of the rock-salt cubic structure.

Graphical abstract: Synthesis of (MgCoNiCuZn)O entropy-stabilized oxides using solution-based routes: influence of composition on phase stability and functional properties

Supplementary files

Article information

Article type
Paper
Submitted
14 Jul 2021
Accepted
06 Oct 2021
First published
07 Oct 2021

J. Mater. Chem. C, 2021,9, 15121-15131

Synthesis of (MgCoNiCuZn)O entropy-stabilized oxides using solution-based routes: influence of composition on phase stability and functional properties

W. Mnasri, D. Bérardan, S. Tusseau-Nenez, T. Gacoin, I. Maurin and N. Dragoe, J. Mater. Chem. C, 2021, 9, 15121 DOI: 10.1039/D1TC03287A

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