Active Motif Change of Ni-Fe Spinel Oxide by Ir Doping for Highly Durable and Facile Oxygen Evolution Reaction

Sukhwa Hong; Kahyun Ham; Jeemin Hwang; Sinwoo Kang; Min Ho Seo; Young Woo Choi; Byungchan Han; Jaeyoung Lee; Kangwoo Cho

doi:10.1002/adfm.202209543

Active Motif Change of Ni-Fe Spinel Oxide by Ir Doping for Highly Durable and Facile Oxygen Evolution Reaction

Sukhwa Hong, Kahyun Ham, Jeemin Hwang, Sinwoo Kang, Min Ho Seo, Young Woo Choi, Byungchan Han, Jaeyoung Lee, Kangwoo Cho

Department of Chemical and Biomolecular Engineering

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

3 Citations (Scopus)

Abstract

The oxygen evolution reaction (OER) is crucial for producing sustainable energy carriers. Herein, Ir (5 mol.%) doped inverse-spinel NiFe₂O₄ (Ir-NFO) nanoparticles deposited on Ni foam (NF) by scalable solution casting are considered a promising OER electrocatalyst for industrial deployments. The Ir-NFO/NF (with minimal lattice distortion by uniform Ir doping) provides an OER overpotential of 251 mV (intrinsically outperforming NFO/NF and benchmarking IrO₂/NF) and extraordinary robustness over 130 days at 100 mA cm⁻². In situ X-ray absorption spectroscopy reveals oxidation only for Fe on NFO, whereas concurrent generation of higher-valent Ni and Fe occurs on Ir-NFO during OER. Density functional theory calculations further demonstrate that Ir substitutes the sublayer Ni octahedral site and switches the main active reaction center from Fe_Oh Fe_Td bridge site (Fe O Fe) on NFO to Ni_Oh–Fe_Td bridge site (Ni O Fe active motif) on Ir-NFO for a co-catalytic OER. This study sheds new light on precious-metal doped Ni-Fe oxides, which may be applicable to other binary/ternary oxide electrocatalysts.

Original language	English
Article number	2209543
Journal	Advanced Functional Materials
Volume	33
Issue number	1
DOIs	https://doi.org/10.1002/adfm.202209543
Publication status	Published - 2023 Jan 3

Bibliographical note

Funding Information:
S.H., K.H., and J.H. contributed equally to this work. This work was financially supported by National Research Foundation of Korea (NRF) grant funded by the Ministry of Education (2022R1A6A3A13066016) and the Korea government Ministry of Science and ICT (MSIT) (2022R1A2C4001228, 2021M3I3A1084818, and 2021K1A4A8A01079455) and framework of the research and development program of the Korea Institute of Energy Research (C2‐2475).

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Materials Science(all)
Condensed Matter Physics

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10.1002/adfm.202209543

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@article{e6b54424086644e79ecb8a736e20403b,

title = "Active Motif Change of Ni-Fe Spinel Oxide by Ir Doping for Highly Durable and Facile Oxygen Evolution Reaction",

abstract = "The oxygen evolution reaction (OER) is crucial for producing sustainable energy carriers. Herein, Ir (5 mol.%) doped inverse-spinel NiFe2O4 (Ir-NFO) nanoparticles deposited on Ni foam (NF) by scalable solution casting are considered a promising OER electrocatalyst for industrial deployments. The Ir-NFO/NF (with minimal lattice distortion by uniform Ir doping) provides an OER overpotential of 251 mV (intrinsically outperforming NFO/NF and benchmarking IrO2/NF) and extraordinary robustness over 130 days at 100 mA cm−2. In situ X-ray absorption spectroscopy reveals oxidation only for Fe on NFO, whereas concurrent generation of higher-valent Ni and Fe occurs on Ir-NFO during OER. Density functional theory calculations further demonstrate that Ir substitutes the sublayer Ni octahedral site and switches the main active reaction center from FeOh FeTd bridge site (Fe O Fe) on NFO to NiOh–FeTd bridge site (Ni O Fe active motif) on Ir-NFO for a co-catalytic OER. This study sheds new light on precious-metal doped Ni-Fe oxides, which may be applicable to other binary/ternary oxide electrocatalysts.",

author = "Sukhwa Hong and Kahyun Ham and Jeemin Hwang and Sinwoo Kang and Seo, {Min Ho} and Choi, {Young Woo} and Byungchan Han and Jaeyoung Lee and Kangwoo Cho",

note = "Funding Information: S.H., K.H., and J.H. contributed equally to this work. This work was financially supported by National Research Foundation of Korea (NRF) grant funded by the Ministry of Education (2022R1A6A3A13066016) and the Korea government Ministry of Science and ICT (MSIT) (2022R1A2C4001228, 2021M3I3A1084818, and 2021K1A4A8A01079455) and framework of the research and development program of the Korea Institute of Energy Research (C2‐2475). Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH.",

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AU - Hong, Sukhwa

AU - Ham, Kahyun

AU - Hwang, Jeemin

AU - Kang, Sinwoo

AU - Seo, Min Ho

AU - Choi, Young Woo

AU - Han, Byungchan

AU - Lee, Jaeyoung

AU - Cho, Kangwoo

N1 - Funding Information: S.H., K.H., and J.H. contributed equally to this work. This work was financially supported by National Research Foundation of Korea (NRF) grant funded by the Ministry of Education (2022R1A6A3A13066016) and the Korea government Ministry of Science and ICT (MSIT) (2022R1A2C4001228, 2021M3I3A1084818, and 2021K1A4A8A01079455) and framework of the research and development program of the Korea Institute of Energy Research (C2‐2475). Publisher Copyright: © 2022 Wiley-VCH GmbH.

PY - 2023/1/3

Y1 - 2023/1/3

N2 - The oxygen evolution reaction (OER) is crucial for producing sustainable energy carriers. Herein, Ir (5 mol.%) doped inverse-spinel NiFe2O4 (Ir-NFO) nanoparticles deposited on Ni foam (NF) by scalable solution casting are considered a promising OER electrocatalyst for industrial deployments. The Ir-NFO/NF (with minimal lattice distortion by uniform Ir doping) provides an OER overpotential of 251 mV (intrinsically outperforming NFO/NF and benchmarking IrO2/NF) and extraordinary robustness over 130 days at 100 mA cm−2. In situ X-ray absorption spectroscopy reveals oxidation only for Fe on NFO, whereas concurrent generation of higher-valent Ni and Fe occurs on Ir-NFO during OER. Density functional theory calculations further demonstrate that Ir substitutes the sublayer Ni octahedral site and switches the main active reaction center from FeOh FeTd bridge site (Fe O Fe) on NFO to NiOh–FeTd bridge site (Ni O Fe active motif) on Ir-NFO for a co-catalytic OER. This study sheds new light on precious-metal doped Ni-Fe oxides, which may be applicable to other binary/ternary oxide electrocatalysts.

AB - The oxygen evolution reaction (OER) is crucial for producing sustainable energy carriers. Herein, Ir (5 mol.%) doped inverse-spinel NiFe2O4 (Ir-NFO) nanoparticles deposited on Ni foam (NF) by scalable solution casting are considered a promising OER electrocatalyst for industrial deployments. The Ir-NFO/NF (with minimal lattice distortion by uniform Ir doping) provides an OER overpotential of 251 mV (intrinsically outperforming NFO/NF and benchmarking IrO2/NF) and extraordinary robustness over 130 days at 100 mA cm−2. In situ X-ray absorption spectroscopy reveals oxidation only for Fe on NFO, whereas concurrent generation of higher-valent Ni and Fe occurs on Ir-NFO during OER. Density functional theory calculations further demonstrate that Ir substitutes the sublayer Ni octahedral site and switches the main active reaction center from FeOh FeTd bridge site (Fe O Fe) on NFO to NiOh–FeTd bridge site (Ni O Fe active motif) on Ir-NFO for a co-catalytic OER. This study sheds new light on precious-metal doped Ni-Fe oxides, which may be applicable to other binary/ternary oxide electrocatalysts.

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ER -

Active Motif Change of Ni-Fe Spinel Oxide by Ir Doping for Highly Durable and Facile Oxygen Evolution Reaction

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