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La2CoO4: a new intercalation based cathode material for fluoride ion batteries with improved cycling stability

Nowroozi, Mohammad Ali and Ivlev, Sergei and Rohrer, Jochen and Clemens, Oliver (2018):
La2CoO4: a new intercalation based cathode material for fluoride ion batteries with improved cycling stability.
In: Journal of Materials Chemistry A, Royal Society of Chemistry, pp. 4658-4669, 6, (11), ISSN 2050-7488,
DOI: 10.1039/c7ta09427b,
[Online-Edition: https://doi.org/10.1039/c7ta09427b],
[Article]

Abstract

In this study, we report on the electrochemical cycling behavior of La2CoO4 (against a composite of Pb/PbF2 as the anode material) for use as an intercalation-based cathode material for fluoride ion batteries (FIBs). The material can intercalate approximately 1.2 fluoride ions per formula under the formation of La2CoO4F1.2 resulting in a strong increase of the cell volume, confirmed by means of ex situ X-ray diffraction studies at various charging capacities and additional complementary chemical fluorination experiments. Furthermore, by only regulating the cut-off capacity we were able to remarkably avoid unwanted side reactions which were previously assumed to be a major problem for achieving high cycling numbers of LaSrMnO4. In this respect, electrochemical impedance spectroscopy was used to determine an initial critical specific charge capacity of ∼65 mA h g−1. By carefully designing the charging process, a discharge capacity as high as 32 mA h g−1 could be obtained, which is the highest capacity for an intercalation based cathode material reported so far, with a capacity retention of ∼25% of the initial discharge capacity after 50 cycles. In addition, we discuss why avoiding the cross-reactivity of the carbon additive is more difficult for fluoride ion batteries than for lithium ion batteries, showing that this is an important challenge for the successful implementation of high voltage cathode materials.

Item Type: Article
Erschienen: 2018
Creators: Nowroozi, Mohammad Ali and Ivlev, Sergei and Rohrer, Jochen and Clemens, Oliver
Title: La2CoO4: a new intercalation based cathode material for fluoride ion batteries with improved cycling stability
Language: English
Abstract:

In this study, we report on the electrochemical cycling behavior of La2CoO4 (against a composite of Pb/PbF2 as the anode material) for use as an intercalation-based cathode material for fluoride ion batteries (FIBs). The material can intercalate approximately 1.2 fluoride ions per formula under the formation of La2CoO4F1.2 resulting in a strong increase of the cell volume, confirmed by means of ex situ X-ray diffraction studies at various charging capacities and additional complementary chemical fluorination experiments. Furthermore, by only regulating the cut-off capacity we were able to remarkably avoid unwanted side reactions which were previously assumed to be a major problem for achieving high cycling numbers of LaSrMnO4. In this respect, electrochemical impedance spectroscopy was used to determine an initial critical specific charge capacity of ∼65 mA h g−1. By carefully designing the charging process, a discharge capacity as high as 32 mA h g−1 could be obtained, which is the highest capacity for an intercalation based cathode material reported so far, with a capacity retention of ∼25% of the initial discharge capacity after 50 cycles. In addition, we discuss why avoiding the cross-reactivity of the carbon additive is more difficult for fluoride ion batteries than for lithium ion batteries, showing that this is an important challenge for the successful implementation of high voltage cathode materials.

Journal or Publication Title: Journal of Materials Chemistry A
Volume: 6
Number: 11
Publisher: Royal Society of Chemistry
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Fachgebiet Materialdesign durch Synthese
11 Department of Materials and Earth Sciences > Material Science > Materials Modelling
Date Deposited: 20 Jun 2018 09:03
DOI: 10.1039/c7ta09427b
Official URL: https://doi.org/10.1039/c7ta09427b
Funders: This work was funded by the German Research Foundation (DFG) within the Emmy Noether program (Grant No. CL551/2-1)., Computational time was made available at the Lichtenberg-Cluster at TU Darmstadt, Germany., We thank Prof. Dr Florian Kraus (Philipps-Universit ̈ at Marburg) for his kind support., The authors further acknowledge Mr Aamir Iqbal Waidha for providing iodometric titration on La 2 CoO 4 .
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