TY - JOUR

T1 - Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries

AU - Wang, Qingsong

AU - Sarkar, Abhishek

AU - Wang, Di

AU - Velasco, Leonardo

AU - Azmi, Raheleh

AU - Bhattacharya, Subramshu S.

AU - Bergfeldt, Thomas

AU - Düvel, Andre

AU - Heitjans, Paul

AU - Brezesinski, Torsten

AU - Hahn, Horst

AU - Breitung, Ben

N1 - Funding Information: Q. W. acknowledges financial support by EnABLES. This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement no. 730957. H. H. and A. S. acknowledge financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, under contract HA 1344/43-1). P. H. is grateful to Niedersächsisches Ministerium für Wissenschaft und Kultur (MWK) for a Niedersachsen Professorship (VWZN3095) and A. D. acknowledges financial support by DFG (DU 1668/3-1). The K-Alpha+ was financially supported by the Federal Ministry of Economics and Energy (BMWi). Dr Julia Maibach (from IAM-ESS, KIT) is acknowledged for access to XPS laboratory.

PY - 2019/8/1

Y1 - 2019/8/1

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85070996920&partnerID=8YFLogxK

U2 - 10.1039/c9ee00368a

DO - 10.1039/c9ee00368a

M3 - Article

AN - SCOPUS:85070996920

VL - 12

SP - 2433

EP - 2442

JO - Energy and Environmental Science

JF - Energy and Environmental Science

SN - 1754-5692

IS - 8

ER -