Electrochemical reduction and oxidation of Ruddlesden–Popper-type La2NiO3F2 within fluoride-ion batteries

kerstin wissel, roland Schoch, tobias vogel, Manuel Donzelli, Galina Matveeva, Ute Kolb, Matthias Bauer, Peter Slater, Oliver Clemens

Research output: Contribution to journalArticlepeer-review

Abstract

Within this article, it is shown that an electrochemical defluorination and additional fluorination of Ruddlesden–Popper-type La2NiO3F2 is possible within all-solid-state fluoride-ion batteries. Structural changes within the reduced and oxidized phases have been examined by X-ray diffraction studies at different states of charging and discharging. The synthesis of the oxidized phase La2NiO3F2+x proved to be successful by structural analysis using both X-ray powder diffraction and automated electron diffraction tomography techniques. The structural reversibility on re-fluorinating and re-defluorinating is also demonstrated. Moreover, the influence of different sequences of consecutive reduction and oxidation steps on the formed phases has been investigated. The observed structural changes have been compared to changes in phases obtained via other topochemical modification approaches such as hydride-based reduction and oxidative fluorination using F2 gas, highlighting the potential of such electrochemical reactions as alternative synthesis routes. Furthermore, the electrochemical routes represent safe and controllable synthesis approaches for novel phases, which cannot be synthesized via other topochemical methods. Additionally, side reactions, occurring alongside the desired electrochemical reactions, have been addressed and the cycling performance has been studied.
Original languageEnglish
Pages (from-to)499–512
Number of pages14
JournalChemistry of Materials
Volume33
Issue number2
Early online date6 Jan 2021
DOIs
Publication statusPublished - 26 Jan 2021

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