Na2FePO4F/multi-walled carbon nanotubes for lithium-ion batteries: Operando Mössbauer study of spray-dried composites

Magali Brisbois; Sébastien Caes; Moulay T. Sougrati; Bénédicte Vertruyen; Audrey Schrijnemakers; Rudi Cloots; Nicolas Eshraghi; Raphaël P. Hermann; Abdelfattah Mahmoud; Frédéric Boschini

doi:10.1016/j.solmat.2015.09.005

Na₂FePO₄F/multi-walled carbon nanotubes for lithium-ion batteries: Operando Mössbauer study of spray-dried composites

Magali Brisbois, Sébastien Caes, Moulay T. Sougrati, Bénédicte Vertruyen, Audrey Schrijnemakers, Rudi Cloots, Nicolas Eshraghi, Raphaël P. Hermann, Abdelfattah Mahmoud, Frédéric Boschini

Research output: Contribution to journal › Article › peer-review

28 Scopus citations

Abstract

In order to favor electronic conductivity in sodium iron fluorophosphate electrodes for lithium- or sodium-ion batteries, composites of Na₂FePO₄F with multi-walled carbon nanotubes (CNTs) were prepared by pilot-scale spray drying. Addition of multi-walled CNTs in the solution results in an excellent dispersion of the CNTs within the volume of Na₂FePO₄F and not only at the surface of the particles. Following a heat treatment at 600 °C in argon in order to reach crystallization, X-ray diffraction and ex situ Mössbauer spectroscopy revealed the presence of significant amounts of Fe(III) and maghemite (γ-Fe₂O₃) in the powder. However, Na₂FePO₄F/CNTs composites exhibit good electrochemical performance when cycling against lithium, with a discharge capacity of 104 mA h g^-1 at C/10 rate and 90 mA h g^-1 at 1C rate. Therefore, operando ⁵⁷Fe transmission Mössbauer spectroscopy analyses were carried out in order to investigate the evolution of the iron oxidation state during cycling. During the first discharge, all the Fe(III) is reduced to Fe(II), explaining the good electrochemical performance.

Original language	English
Pages (from-to)	67-72
Number of pages	6
Journal	Solar Energy Materials and Solar Cells
Volume	148
DOIs	https://doi.org/10.1016/j.solmat.2015.09.005
State	Published - Apr 1 2016
Externally published	Yes

Funding

M.B. is grateful to the Belgian “ Fonds pour la Formation à la Recherche dans l’Industrie et l’Agriculture (FRIA) ” for financial support (Grant no. 1.E056.11 ). Part of this work was supported by the Walloon Region under the “PE Plan Marshall 2.vert” program (BATWAL – 1318146 ). A. Mahmoud acknowledges the Forschungszentrum Jülich for an international postdoctoral grant.

Funders	Funder number
Walloon Region
Fonds pour la Formation à la Recherche dans l’Industrie et dans l’Agriculture	E056.11
Forschungszentrum Jülich

Keywords

Carbon nanotubes
Lithium-ion batteries
Mössbauer
NaFePOF
Spray-drying

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.solmat.2015.09.005

Cite this

Brisbois, M., Caes, S., Sougrati, M. T., Vertruyen, B., Schrijnemakers, A., Cloots, R., Eshraghi, N., Hermann, R. P., Mahmoud, A., & Boschini, F. (2016). Na₂FePO₄F/multi-walled carbon nanotubes for lithium-ion batteries: Operando Mössbauer study of spray-dried composites. Solar Energy Materials and Solar Cells, 148, 67-72. https://doi.org/10.1016/j.solmat.2015.09.005

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abstract = "In order to favor electronic conductivity in sodium iron fluorophosphate electrodes for lithium- or sodium-ion batteries, composites of Na2FePO4F with multi-walled carbon nanotubes (CNTs) were prepared by pilot-scale spray drying. Addition of multi-walled CNTs in the solution results in an excellent dispersion of the CNTs within the volume of Na2FePO4F and not only at the surface of the particles. Following a heat treatment at 600 °C in argon in order to reach crystallization, X-ray diffraction and ex situ M{\"o}ssbauer spectroscopy revealed the presence of significant amounts of Fe(III) and maghemite (γ-Fe2O3) in the powder. However, Na2FePO4F/CNTs composites exhibit good electrochemical performance when cycling against lithium, with a discharge capacity of 104 mA h g-1 at C/10 rate and 90 mA h g-1 at 1C rate. Therefore, operando 57Fe transmission M{\"o}ssbauer spectroscopy analyses were carried out in order to investigate the evolution of the iron oxidation state during cycling. During the first discharge, all the Fe(III) is reduced to Fe(II), explaining the good electrochemical performance.",

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AU - Caes, Sébastien

AU - Sougrati, Moulay T.

AU - Vertruyen, Bénédicte

AU - Schrijnemakers, Audrey

AU - Cloots, Rudi

AU - Eshraghi, Nicolas

AU - Hermann, Raphaël P.

AU - Mahmoud, Abdelfattah

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