Journal
CHEMISTRY OF MATERIALS
Volume 26, Issue 11, Pages 3391-3402Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm5005104
Keywords
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Funding
- Ministerio de Educacion y Ciencia [MAT2010-19442]
- Gobierno Vasco/Eusko Jaurlaritza [Etortek CICEnergigune-10, SAIO-TEK-12-ENERGIBA, IT570-13]
- AINSE Ltd.
- University of Basque Country [UFI11/53]
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Ambient temperature sodium-ion batteries are emerging as an exciting alternative to commercially dominant lithium-ion batteries for larger scale stationary applications. In order to realize such a sodium-ion battery, electrodes need to be developed, understood, and improved. Here, Na3V2O2(PO4)(2)F is investigated from the perspective of sodium. Reaction mechanisms for this cathode during battery function include the following: a region comprising at least three phases with subtly varying sodium compositions that transform via two two-phase reaction mechanisms, which appears at the lower potential plateau-like region during both charge and discharge; an extended solid solution region for majority of the cycling process, including most of the higher potential plateau; and a second two-phase region near the highest charge state during charge and between the first and second plateau-like regions during discharge. Notably, the distinct asymmetry in the reaction mechanism, lattice, and volume evolution on charge relative to discharge manifests an interesting question: Is such an asymmetry beneficial for this cathode? These reaction mechanisms are inherently related to sodium evolution, which shows complex behavior between the two sodium crystallographic sites in this compound that in turn mediate the lattice and reaction evolution. Thus, this work relates atomic-level sodium perturbations directly with electrochemical cycling.
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