Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries

Qingsong Wang; Abhishek Sarkar; Di Wang; Leonardo Velasco; Raheleh Azmi; Subramshu S. Bhattacharya; Thomas Bergfeldt; Andre Düvel; Paul Heitjans; Torsten Brezesinski; Horst Hahn; Ben Breitung

doi:10.1039/C9EE00368A

Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries†

Qingsong Wang,

*^a Abhishek Sarkar,

^ab Di Wang,^ac Leonardo Velasco,

^a Raheleh Azmi,

^d Subramshu S. Bhattacharya,^e Thomas Bergfeldt,^c Andre Düvel,

^f Paul Heitjans,

^f Torsten Brezesinski,

^a Horst Hahn

*^abg and Ben Breitung

*^ac

Author affiliations

* Corresponding authors

^a Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
E-mail: qingsong.wang@kit.edu, horst.hahn@kit.edu, ben.breitung@kit.edu

^b Joint Research Laboratory Nanomaterials – Technische Universität Darmstadt and Karlsruhe Institute of Technology (KIT), Otto-Berndt-Str. 3, 64206 Darmstadt, Germany

^c Karlsruhe Nano Micro Facility (KNMF), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany

^d Institute for Applied Materials, Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany

^e Department of Metallurgical and Materials Engineering, Nano Functional Materials Technology Centre (NFMTC), Indian Institute of Technology Madras, Chennai, India

^f Institute of Physical Chemistry and Electrochemistry, and ZFM – Center for Solid State Chemistry and New Materials, Leibniz University Hannover, Callinstr. 3a, 30167 Hannover, Germany

^g Helmholtz Institute Ulm for Electrochemical Energy Storage, Helmholtzstr. 11, 89081 Ulm, Germany

Abstract

In the present work, a new class of high entropy materials for energy storage applications is introduced. Multi-anionic and -cationic compounds are prepared by facile mechanochemistry using a recently designed multi-cationic transition-metal-based high entropy oxide as the precursor and LiF or NaCl as the reactant, leading to formation of lithiated or sodiated materials. Notably, the Li-containing entropy-stabilized oxyfluoride described herein (Li_x(Co_0.2Cu_0.2Mg_0.2Ni_0.2Zn_0.2)OF_x) exhibits a working potential of 3.4 V vs. Li⁺/Li, enabling its use as a cathode active material. Unlike conventional (non-entropy-stabilized) oxyfluorides, this new material shows enhanced Li storage properties due to entropy stabilization, which, in general, facilitates tailoring the cycling performance by varying the constituent elements in yet unprecedented ways. In addition, we demonstrate that the concept of entropy stabilization is also applicable to Na-containing oxychlorides with a rock-salt structure, thus paving the way toward development of (next-generation) post-Li battery technologies.

Energy & Environmental Science

Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries†

Abstract

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Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries

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