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DOE OSTI · 3391244

Progress and Perspectives: Zirconium Electrodeposition from Different Electrolytes

Watkins, Nicholas Bret [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000172519387)·De Silva, Umanga Handi Umanga Iroshini [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000300295868)·Janusz, Jordyn Nevada [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000177884754)·McBride, Michael Anthony [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000252747275)·Mirabal, Alex James [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000245017602)·Jones, Benjamin Jesse [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000181850311)·Stull, Jamie Ann [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000204647456)
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Abstract

Zirconium (Zr) possesses outstanding properties, including exceptional chemical resistance and a high melting point, and is therefore desirable for use in a wide variety of challenging environments, such as in nuclear reactors and the chemical processing industry. To minimize the amount of Zr required for any given application, developing methods for generating metallic Zr coatings is highly advantageous. Owing to Zr’s highly negative reduction potential, electrodeposition in traditional solvents at near ambient temperatures remains challenging and thus not well understood. Due to the extreme conditions required to deposit this metal, extensive work has been conducted in molten salt electrolytes, however the broad applicability of this methodology is limited due to its corrosivity. The primary focus of this article is to present an overview of Zr’s electrochemical behavior and to consolidate the efforts of researchers in exploring electrodeposition techniques for Zr involving aqueous, organic, ionic liquid, deep eutectic, and molten salt solvents. With this information, we highlight trends across solvent systems and opportunities for future research.

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42 ENGINEERINGZirconiumelectrodepositionelectroplatingreview

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Watkins, Nicholas Bret [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000172519387), De Silva, Umanga Handi Umanga Iroshini [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000300295868), Janusz, Jordyn Nevada [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000177884754), McBride, Michael Anthony [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000252747275), Mirabal, Alex James [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000245017602), Jones, Benjamin Jesse [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000181850311), Stull, Jamie Ann [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000204647456). 2026-06-01. Progress and Perspectives: Zirconium Electrodeposition from Different Electrolytes. https://doi.org/10.1149/1945-7111/ae6d79

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DOE OSTI2023

Electrolyte-Induced Restructuring of Acid-Stable Oxygen Evolution Catalysts

Crystalline metal oxide catalysts operating under oxygen evolution reaction (OER) conditions invariably restructure, resulting in active sites with hydroxo/oxo species in an amorphous environment. An increase in the population of terminal hydroxo/oxo species (i.e., edge sites) facilitates proton-coupled electron-transfer (PCET) kinetics for oxygen generation and thus improves catalyst competency. While amorphous films benefit from a greater density of active sites, they suffer from diminished charge transport as compared to that of extended crystalline lattices. Managing this amorphous–crystalline dichotomy is essential when designing OER catalysts, which we highlight with the examination of electrodeposited PbO x materials, which historically are very poor OER catalysts. Along these lines, the presence of phosphate during PbO x electrodeposition truncates the growth of an extended lattice owing to its strong bonding to oxide surfaces to afford an amorphous catalyst film (A-PbO x ) with significant charge-transfer resistance (138 ± 42 Ω) and poor OER kinetics (420 ± 105 mV dec –1 Tafel slope). Conversely, electrodeposition of Pb 2+ in the presence of less coordinating electrolytes such as nitrate affords crystalline β-PbO2 with improved charge-transfer resistance (42.6 ± 1.1 Ω), though still poor OER kinetics (134 ± 36 mV dec –1 Tafel slope). By operating amorphous A-PbOx in less coordinating electrolytes, however, a new partially crystalline material can be generated (μc-PbO x ) with further reduced charge-transfer resistance (33.0 ± 1.4 Ω) and improved OER kinetics (70 ± 15 mV dec –1 Tafel slope). The enhanced OER activity of μc-PbO x is the result of coupling the high edge-site population of an amorphous PbOx phase with crystalline-like charge transport properties. Finally, the ability to use an electrolyte to induce OER activity in an inactive amorphous form of PbO x highlights the benefits of optimizing the amorphous–crystalline phase compositions in the design of active OER catalysts.

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