Electrodeposition of Complex High Entropy Oxides via Water Droplet Formation and Conversion to Crystalline Alloy Nanoparticles

Percival, Stephen J.; Lu, Ping; Lowry, Daniel R.; Nenoff, Tina M.

doi:10.1021/acs.langmuir.1c03228

Electrodeposition of Complex High Entropy Oxides via Water Droplet Formation and Conversion to Crystalline Alloy Nanoparticles

Journal Article · Wed Jan 26 23:00:00 EST 2022 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.1c03228· OSTI ID:1870445

^[1]; Lu, Ping ^[1]; Lowry, Daniel R. ^[1]; ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

We report that a combination of electrodeposition and thermal reduction methods have been utilized for the synthesis of ligand-free FeNiCo alloy nanoparticles through a high-entropy oxide intermediate. These phases are of great interest to the electrocatalysis community, especially when formed by a sustainable chemistry method. This is successfully achieved by first forming a complex five element amorphous FeNiCoCrMn high-entropy oxide (HEO) phase via electrodeposition from a nanodroplet emulsion solution of the metal salt reactants. The amorphous oxide phase is then thermally treated and reduced at 570–600 °C to form the crystalline FeNiCo alloy with a separate CrMnO_x cophase. The FeNiCo alloy is fully characterized by scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy elemental analysis and is identified as a face-centered cubic crystal with the lattice constant a = 3.52 Å. The unoptimized, ligand-free FeNiCo NPs activity toward the oxygen evolution reaction is evaluated in alkaline solution and found to have an ~185 mV more cathodic onset potential than the Pt metal. Beyond being able to synthesize highly crystalline, ligand-free FeNiCo nanoparticles, the demonstrated and relatively simple two-step process is ideal for the synthesis of tailor-made nanoparticles where the desired composition is not easily achieved with classical solution-based chemistries.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: NA0003525

OSTI ID:: 1870445

Report Number(s):: SAND2022-3545J; 704466

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 5 Vol. 38; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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