Exploiting the Oxygen Redox Reaction and Crystal-Preferred Orientation in a P3-Type Na2/3Mg1/3Mn2/3O2Thin-Film Electrode

Yiman Zhang, Nathan D. Phillip, Bohang Song, Robert L. Sacci, Jue Liu, Nancy J. Dudney

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

Abstract

The anionic redox reaction (ARR) can be used to enhance the capacity of cathode materials. Understanding how ARR proceeds along with transition metal redox electrochemistry is crucial for designing the next-generation high-energy-density cathodes. In this study, we use a Na2/3Mg1/3Mn2/3O2 (NMMO) thin film as a model cathode material for Na-ion batteries to study the oxygen redox reaction. We are able to control the orientation of the thin film using a pre-conditioning step of the Pt current collector layer and, thus, tune the cathode electrolyte interphase (CEI). Preferential orientation along the (001) direction prevents the extraction of Na+ ions from the lattice during charge. However, the randomly oriented NMMO thin films perform similar to the slurry electrode from powder. The characteristics of the electrode surface from XPS illustrate the evolution of CEI at different states of charge in the randomly oriented thin-film electrode. Our results show that the crystalline orientation can drastically affect the availability of the electrochemical reaction.

Original languageEnglish
Pages (from-to)7692-7699
Number of pages8
JournalEnergy and Fuels
Volume34
Issue number6
DOIs
StatePublished - Jun 18 2020

Funding

This manuscript has been authored in part by UT-Battelle LLC, under Contract DE-AC05-00OR22725 with the United States Department of Energy (DOE). This research was supported by the Center for Mesoscale Transport Properties, an Energy Frontier Research Center supported by the Basic Energy Sciences, Office of Science, DOE, under Award DE-SC0012673. This manuscript has been authored in part by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the United States Department of Energy (DOE). This research was supported by the Center for Mesoscale Transport Properties, an Energy Frontier Research Center supported by the Basic Energy Sciences, Office of Science, DOE, under Award DE-SC0012673.

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