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

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

Journal Article · Tue Oct 16 00:00:00 EDT 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];

^[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.

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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, Vol. 8, Issue 11; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 80 works

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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
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
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
Facile Synthesis of IrCu Microspheres Based on Polyol Method and Study on Their Electro-Catalytic Performances to Oxygen Evolution Reaction Liu, Xuan; Li, Zichao; Zhou, Luming Nanomaterials, Vol. 9, Issue 8 https://doi.org/10.3390/nano9081145	journal	August 2019
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

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