Electrodeposition of atmosphere-sensitive ternary sodium transition metal oxide films for sodium-based electrochemical energy storage

Arghya Patra, Jerome Davis, Saran Pidaparthy, Manohar H. Karigerasi, Beniamin Zahiri, Ashish A. Kulkarni, Michael A. Caple, Daniel P. Shoemaker, Jian Min Zuo, Paul V. Braun

Research output: Contribution to journalArticlepeer-review


We introduce an intermediate-temperature (350 °C) dry molten sodium hydroxide-mediated binder-free electrodeposition process to grow the previously electrochemically inaccessible air- and moisture-sensitive layered sodium transition metal oxides, NaxMO2(M = Co, Mn, Ni, Fe), in both thin and thick film form, compounds which are conventionally synthesized in powder form by solid-state reactions at temperatures ≥700 °C. As a key motivation for this work, several of these oxides are of interest as cathode materials for emerging sodium-ion-based electrochemical energy storage systems. Despite the low synthesis temperature and short reaction times, our electrodeposited oxides retain the key structural and electrochemical performance observed in high-temperature bulk synthesized materials. We demonstrate that tens of micrometers thick >75%dense NaxCoO2and NaxMnO2can be deposited in under 1 h. When used as cathodes for sodium-ion batteries, these materials exhibit near theoretical gravimetric capacities, chemical diffusion coefficients of Na+ions (~10-12cm2·s-1), and high reversible areal capacities in the range ~0.25 to 0.76 mA·h·cm-2, values significantly higher than those reported for binder-free sodium cathodes deposited by other techniques. The method described here resolves longstanding intrinsic challenges associated with traditional aqueous solution-based electrodeposition of ceramic oxides and opens a general solution chemistry approach for electrochemical processing of hitherto unexplored air- and moisture-sensitive high valent multinary structures with extended frameworks.

Original languageEnglish (US)
Article numbere2025044118
JournalProceedings of the National Academy of Sciences of the United States of America
Issue number22
StatePublished - Jun 1 2021


  • Electrosynthesis
  • Secondary battery
  • Sodium ion cathode
  • Transition metal oxide

ASJC Scopus subject areas

  • General


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