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

Research output: Contribution to journalArticleResearchpeer review

Authors

  • 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

External Research Organisations

  • Karlsruhe Institute of Technology (KIT)
  • Technische Universität Darmstadt
  • Indian Institute of Technology Madras (IITM)
  • Helmholtz Institute Ulm Electrochemical Energy Storage (HIU)
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Details

Original languageEnglish
Pages (from-to)2433-2442
Number of pages10
JournalEnergy and Environmental Science
Volume12
Issue number8
Early online date2 May 2019
Publication statusPublished - 1 Aug 2019

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.

ASJC Scopus subject areas

Sustainable Development Goals

Cite this

Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries. / Wang, Qingsong; Sarkar, Abhishek; Wang, Di et al.
In: Energy and Environmental Science, Vol. 12, No. 8, 01.08.2019, p. 2433-2442.

Research output: Contribution to journalArticleResearchpeer review

Wang, Q, Sarkar, A, Wang, D, Velasco, L, Azmi, R, Bhattacharya, SS, Bergfeldt, T, Düvel, A, Heitjans, P, Brezesinski, T, Hahn, H & Breitung, B 2019, 'Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries', Energy and Environmental Science, vol. 12, no. 8, pp. 2433-2442. https://doi.org/10.1039/c9ee00368a, https://doi.org/10.15488/10767
Wang, Q., Sarkar, A., Wang, D., Velasco, L., Azmi, R., Bhattacharya, S. S., Bergfeldt, T., Düvel, A., Heitjans, P., Brezesinski, T., Hahn, H., & Breitung, B. (2019). Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries. Energy and Environmental Science, 12(8), 2433-2442. https://doi.org/10.1039/c9ee00368a, https://doi.org/10.15488/10767
Wang Q, Sarkar A, Wang D, Velasco L, Azmi R, Bhattacharya SS et al. Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries. Energy and Environmental Science. 2019 Aug 1;12(8):2433-2442. Epub 2019 May 2. doi: 10.1039/c9ee00368a, 10.15488/10767
Wang, Qingsong ; Sarkar, Abhishek ; Wang, Di et al. / Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries. In: Energy and Environmental Science. 2019 ; Vol. 12, No. 8. pp. 2433-2442.
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title = "Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries",
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.",
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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

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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.

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