Self-Supported Hydrous Iridium–Nickel Oxide Two-Dimensional Nanoframes for High Activity Oxygen Evolution Electrocatalysts

Godínez-Salomón, Fernando; Albiter, Luis; Alia, Shaun M.; Pivovar, Bryan S.; Camacho-Forero, Luis E.; Balbuena, Perla B.; Mendoza-Cruz, Rubén; Arellano-Jimenez, M. Josefina; Rhodes, Christopher P.

doi:10.1021/acscatal.8b02171

Self-Supported Hydrous Iridium–Nickel Oxide Two-Dimensional Nanoframes for High Activity Oxygen Evolution Electrocatalysts

Journal Article · Tue Oct 16 00:00:00 UTC 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b02171· OSTI ID:1475525

Godínez-Salomón, Fernando ^[1]; Albiter, Luis ^[1]; ^[2]; Pivovar, Bryan S. ^[2]; ^[3]; ^[3]; ^[4]; Arellano-Jimenez, M. Josefina ^[4]; ^[1]

Texas State Univ., San Marcos, TX (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Texas A & M Univ., College Station, TX (United States)
Univ. of Texas, San Antonio, TX (United States)

Oxygen evolution reaction (OER) electrocatalysts with high activity, high stability, and low costs are needed for proton-exchange membrane (PEM) electrolyzers. Based on the high cost and limited supply of iridium, approaches that result in iridium-based OER catalysts with increased catalytic activity are of significant interest. Here, we report a carbon-free, self-supported hydrous iridium-nickel oxide two-dimensional nanoframe structure synthesized by thermal treatment of iridium-decorated nickel oxide nanosheets under reducing conditions and subsequent chemical leaching in acid. The catalyst nanoarchitecture contains an interconnected network of metallic iridium-nickel alloy domains with hydrous iridium oxide and nickel oxide located in the surface region. The electrochemical oxidation step maintains the three-dimensional nanoarchitecture and results in a thin (~5 A) oxide/hydroxide surface layer. The temperature used for thermal reduction was found to strongly affect the catalyst surface structure and OER activity. Utilizing a lower thermal reduction temperature of 200 degrees C was determined to provide a higher relative surface concentration of hydroxides and nickel oxide and result in higher OER activities compared with materials treated at 300 degrees C. The 200 degrees C-treated hydrous iridium-nickel oxide electrocatalyst showed 15 times higher initial OER mass activity than commercial IrO₂, and the activity remained 10 times higher than IrO₂ after accelerated durability testing. Density functional theory (DFT) calculations and analysis of the experimental Tafel slopes support that the second electron transfer step is the rate-limiting step for the reaction. The DFT calculations demonstrate that Ni substitution on the IrO₂ surface lowers the activation energy for adsorbed intermediates of the second electron transfer step of the OER reaction. This work establishes that noble metal-decorated metal oxide nanosheets can be transformed into high surface area, carbon-free electrocatalyst nanostructures with high catalytic activities and molecular accessibility and reveals the importance of using controlled thermal reduction temperatures to alter the surface structure and OER activity.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1475525

Report Number(s):: NREL/JA-5900-72511

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 11 Vol. 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Relationship Between OER Activity and Annealing Temperature of Sputter-Deposited Flat IrO2 Thin Films Tachikawa, Takashi; Beniya, Atsushi; Shigetoh, Keisuke Catalysis Letters, Vol. 150, Issue 7 https://doi.org/10.1007/s10562-020-03105-2	journal	January 2020
Highly scattered Ir oxides on TiN as an efficient oxygen evolution reaction electrocatalyst in acidic media Zhang, Kaikai; Mai, Wanshan; Li, Jin Journal of Materials Science, Vol. 55, Issue 8 https://doi.org/10.1007/s10853-019-04201-4	journal	November 2019
One-pot synthesis of copper–nickel sulfide nanowires for overall water splitting in alkaline media Cao, Dong; Cheng, Daojian Chemical Communications, Vol. 55, Issue 56 https://doi.org/10.1039/c9cc02977j	journal	January 2019
Iridium Oxygen Evolution Activity and Durability Baselines in Rotating Disk Electrode Half-Cells Alia, Shaun M.; Anderson, Grace C. Journal of The Electrochemical Society, Vol. 166, Issue 4 https://doi.org/10.1149/2.0731904jes	journal	January 2019
The Roles of Oxide Growth and Sub-Surface Facets in Oxygen Evolution Activity of Iridium and Its Impact on Electrolysis Alia, Shaun M.; Ha, Mai-Anh; Anderson, Grace C. Journal of The Electrochemical Society, Vol. 166, Issue 15 https://doi.org/10.1149/2.0771915jes	journal	January 2019

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77 NANOSCIENCE AND NANOTECHNOLOGY
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