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

authored by
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
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 (Lix(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)OFx) 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.

Organisation(s)
Institute of Physical Chemistry and Electrochemistry
Center for Solid State Chemistry and New Materials (ZFM)
External Organisation(s)
Karlsruhe Institute of Technology (KIT)
Technische Universität Darmstadt
Indian Institute of Technology Madras (IITM)
Helmholtz Institute Ulm Electrochemical Energy Storage (HIU)
Type
Article
Journal
Energy and Environmental Science
Volume
12
Pages
2433-2442
No. of pages
10
ISSN
1754-5692
Publication date
01.08.2019
Publication status
Published
Peer reviewed
Yes
ASJC Scopus subject areas
Environmental Chemistry, Renewable Energy, Sustainability and the Environment, Nuclear Energy and Engineering, Pollution
Sustainable Development Goals
SDG 7 - Affordable and Clean Energy
Electronic version(s)
https://doi.org/10.1039/c9ee00368a (Access: Open)
https://doi.org/10.15488/10767 (Access: Open)