Mechanochemical synthesis: route to novel rock-salt-structured high-entropy oxides and oxyfluorides
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Mechanochemical synthesis: route to novel rock-saltstructured high-entropy oxides and oxyfluorides Ling Lin1 , Kai Wang2, Raheleh Azmi3 , Junbo Wang1 , Abhishek Sarkar1,4 , Miriam Botros1 , Saleem Najib5, Yanyan Cui1, David Stenzel1 , Parvathy Anitha Sukkurji1 Qingsong Wang1 , Horst Hahn1,4,6 , Simon Schweidler1,* , and Ben Breitung1,*
,
1
Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany 2 Department of Materials and Earth Sciences, Technische Universität Darmstadt, Alarich-Weiss-Str. 2, 64287 Darmstadt, Germany 3 Institute for Applied Materials, Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany 4 Joint Research Laboratory Nanomaterials, Technische Universität Darmstadt and Karlsruhe Institute of Technology (KIT), OttoBerndt-Str. 3, 64206 Darmstadt, Germany 5 Faculty of Engineering, University of Waterloo, 200 University Avenue West, Waterloo, ON N2L 3G1, Canada 6 Helmholtz Institute Ulm for Electrochemical Energy Storage, Helmholtzstr. 11, 89081 Ulm, Germany
Received: 9 June 2020
ABSTRACT
Accepted: 29 August 2020
A facile mechanochemical reaction at ambient temperature was successfully applied to synthesize novel single-phase rock-salt-structured high-entropy oxides, containing five, six and seven metal elements in equiatomic amounts. This synthesis approach overcomes the limitations of the commonly known synthesis procedures, which would result in multiple-phase compounds. Redox-sensitive elements, such as Fe2? and Mn2?, can now be considered. The corresponding single-phase Li-containing high-entropy oxyfluorides were obtained by introducing LiF into the lattice using the same strategy. All materials show single-phase rock-salt structures with lattice parameters depending on the incorporated ion sizes. Solid solution states result in high configurational entropies, and all elements appear homogenously distributed over the whole cationic and anionic sublattice. The straightforward synthesis technique, combined with utilized simple binary oxide precursors, paves the way for a multitude of novel high-entropy oxide and oxyfluoride compounds. The compounds were studied by means of X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy and Mo¨ssbauer spectroscopy.
Published online: 14 September 2020
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The Author(s) 2020
Handling Editor: M. Grant Norton.
Address correspondence to E-mail: [email protected]; [email protected]
https://doi.org/10.1007/s10853-020-05183-4
16880
J Mater Sci (2020) 55:16879–16889
Introduction In recent years, a new class of materials enjoys rising popularity, which is based on an entropy stabilization of the crystal structure and related to the socalled high-entropy materials (HEMs) [1]. These HEMs utilize a promising concept to form singlephase compounds composed of a multitude of different elements. This variety of elements leads to a high configurational entropy, which counteracts
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