In Situ Formation of Nano Ni–Co Oxyhydroxide Enables Water Oxidation Electrocatalysts Durable at High Current Densities

Jehad Abed; Shideh Ahmadi; Laura Laverdure; Ahmed Abdellah; Colin P. O'Brien; Kevin Cole; Pedro Sobrinho; David Sinton; Drew Higgins; Nicholas J. Mosey; Steven J. Thorpe; Edward H. Sargent

doi:10.1002/adma.202103812

In Situ Formation of Nano Ni–Co Oxyhydroxide Enables Water Oxidation Electrocatalysts Durable at High Current Densities

Jehad Abed, Shideh Ahmadi, Laura Laverdure, Ahmed Abdellah, Colin P. O'Brien, Kevin Cole, Pedro Sobrinho, David Sinton, Drew Higgins, Nicholas J. Mosey, Steven J. Thorpe^*, Edward H. Sargent

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

105 Scopus citations

Abstract

The oxygen evolution reaction (OER) limits the energy efficiency of electrocatalytic systems due to the high overpotential symptomatic of poor reaction kinetics; this problem worsens over time if the performance of the OER electrocatalyst diminishes during operation. Here, a novel synthesis of nanocrystalline Ni–Co–Se using ball milling at cryogenic temperature is reported. It is discovered that, by anodizing the Ni–Co–Se structure during OER, Se ions leach out of the original structure, allowing water molecules to hydrate Ni and Co defective sites, and the nanoparticles to evolve into an active Ni–Co oxyhydroxide. This transformation is observed using operando X-ray absorption spectroscopy, with the findings confirmed using density functional theory calculations. The resulting electrocatalyst exhibits an overpotential of 279 mV at 0.5 A cm⁻² and 329 mV at 1 A cm⁻² and sustained performance for 500 h. This is achieved using low mass loadings (0.36 mg cm⁻²) of cobalt. Incorporating the electrocatalyst in an anion exchange membrane water electrolyzer yields a current density of 1 A cm⁻² at 1.75 V for 95 h without decay in performance. When the electrocatalyst is integrated into a CO₂-to-ethylene electrolyzer, a record-setting full cell voltage of 3 V at current density 1 A cm⁻² is achieved.

Original language	English (US)
Article number	2103812
Journal	Advanced Materials
Volume	33
Issue number	45
DOIs	https://doi.org/10.1002/adma.202103812
State	Published - Nov 11 2021

Funding

This work was supported financially by the Natural Sciences and Engineering Research Council (NSERC) of Canada, Vanier Canada Graduate Scholarship, and TOTAL SE. Electron microscopy, scanning transmission electron microscopy, and electron energy loss spectroscopy were performed at the Canadian Centre for Electron Microscopy (CCEM) at McMaster University. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the U.S. DOE under Contract No. DE\u2010AC02\u201006CH11357 and the Canadian Light Source and its funding partners. The authors thank Dr. Tianpin Wu and Dr. George Sterbinsky from 9BM beamline, and Dr. Debora Motta Meira and Dr. Zou Finfrock from 20BM beamline for assistance in collecting the XAS data and at the advanced photo source (APS). DFT calculations were conducted as part of the Engineered Nickel Catalysts for Electrochemical Clean Energy project administered from Queen's University and supported by Grant No. RGPNM 477963\u20102015 under the Natural Sciences and Engineering Research Council of Canada (NSERC) Discovery Frontiers Program. The computational resources were provided by Compute Canada. This work was supported financially by the Natural Sciences and Engineering Research Council (NSERC) of Canada, Vanier Canada Graduate Scholarship, and TOTAL SE. Electron microscopy, scanning transmission electron microscopy, and electron energy loss spectroscopy were performed at the Canadian Centre for Electron Microscopy (CCEM) at McMaster University. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357 and the Canadian Light Source and its funding partners. The authors thank Dr. Tianpin Wu and Dr. George Sterbinsky from 9BM?beamline, and Dr. Debora Motta Meira and Dr. Zou Finfrock from 20BM?beamline for assistance in collecting the XAS data and at the advanced photo source (APS). DFT calculations were conducted as part of the Engineered Nickel Catalysts for Electrochemical Clean Energy project administered from Queen's University and supported by Grant No. RGPNM 477963-2015 under the Natural Sciences and Engineering Research Council of Canada (NSERC) Discovery Frontiers Program. The computational resources were provided by Compute Canada.

Keywords

CO reduction
PGM-free X-ray absorption spectroscopy
cryomilling
oxygen evolution reaction

ASJC Scopus subject areas

General Materials Science
Mechanics of Materials
Mechanical Engineering

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/adma.202103812

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Abed, J., Ahmadi, S., Laverdure, L., Abdellah, A., O'Brien, C. P., Cole, K., Sobrinho, P., Sinton, D., Higgins, D., Mosey, N. J., Thorpe, S. J., & Sargent, E. H. (2021). In Situ Formation of Nano Ni–Co Oxyhydroxide Enables Water Oxidation Electrocatalysts Durable at High Current Densities. Advanced Materials, 33(45), Article 2103812. https://doi.org/10.1002/adma.202103812

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title = "In Situ Formation of Nano Ni–Co Oxyhydroxide Enables Water Oxidation Electrocatalysts Durable at High Current Densities",

abstract = "The oxygen evolution reaction (OER) limits the energy efficiency of electrocatalytic systems due to the high overpotential symptomatic of poor reaction kinetics; this problem worsens over time if the performance of the OER electrocatalyst diminishes during operation. Here, a novel synthesis of nanocrystalline Ni–Co–Se using ball milling at cryogenic temperature is reported. It is discovered that, by anodizing the Ni–Co–Se structure during OER, Se ions leach out of the original structure, allowing water molecules to hydrate Ni and Co defective sites, and the nanoparticles to evolve into an active Ni–Co oxyhydroxide. This transformation is observed using operando X-ray absorption spectroscopy, with the findings confirmed using density functional theory calculations. The resulting electrocatalyst exhibits an overpotential of 279 mV at 0.5 A cm−2 and 329 mV at 1 A cm−2 and sustained performance for 500 h. This is achieved using low mass loadings (0.36 mg cm−2) of cobalt. Incorporating the electrocatalyst in an anion exchange membrane water electrolyzer yields a current density of 1 A cm−2 at 1.75 V for 95 h without decay in performance. When the electrocatalyst is integrated into a CO2-to-ethylene electrolyzer, a record-setting full cell voltage of 3 V at current density 1 A cm−2 is achieved.",

keywords = "CO reduction, PGM-free X-ray absorption spectroscopy, cryomilling, oxygen evolution reaction",

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AU - Ahmadi, Shideh

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AU - Abdellah, Ahmed

AU - O'Brien, Colin P.

AU - Cole, Kevin

AU - Sobrinho, Pedro

AU - Sinton, David

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AB - The oxygen evolution reaction (OER) limits the energy efficiency of electrocatalytic systems due to the high overpotential symptomatic of poor reaction kinetics; this problem worsens over time if the performance of the OER electrocatalyst diminishes during operation. Here, a novel synthesis of nanocrystalline Ni–Co–Se using ball milling at cryogenic temperature is reported. It is discovered that, by anodizing the Ni–Co–Se structure during OER, Se ions leach out of the original structure, allowing water molecules to hydrate Ni and Co defective sites, and the nanoparticles to evolve into an active Ni–Co oxyhydroxide. This transformation is observed using operando X-ray absorption spectroscopy, with the findings confirmed using density functional theory calculations. The resulting electrocatalyst exhibits an overpotential of 279 mV at 0.5 A cm−2 and 329 mV at 1 A cm−2 and sustained performance for 500 h. This is achieved using low mass loadings (0.36 mg cm−2) of cobalt. Incorporating the electrocatalyst in an anion exchange membrane water electrolyzer yields a current density of 1 A cm−2 at 1.75 V for 95 h without decay in performance. When the electrocatalyst is integrated into a CO2-to-ethylene electrolyzer, a record-setting full cell voltage of 3 V at current density 1 A cm−2 is achieved.

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In Situ Formation of Nano Ni–Co Oxyhydroxide Enables Water Oxidation Electrocatalysts Durable at High Current Densities

Abstract

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Keywords

ASJC Scopus subject areas

UN SDGs

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