Boosted urea electrooxidation activity by dynamic steady blending CoOOH-Ni(OH)2 nanoclusters for H2 production in a pH-asymmetric electrolyzer

Shih Mao Peng; Shu Ting Chang; Chia Che Chang; Priyadarshini Hn; Chun Chih Chang; Kuan Chang Wu; Yung Hung Huang; Yi Chia Chen; Tsung Rong Kuo; Chih Wen Pao; Jeng Lung Chen; Di Yan Wang

doi:10.1039/d4ta04241g

Boosted urea electrooxidation activity by dynamic steady blending CoOOH-Ni(OH)₂ nanoclusters for H₂ production in a pH-asymmetric electrolyzer

Shih Mao Peng, Shu Ting Chang, Chia Che Chang, Priyadarshini Hn, Chun Chih Chang, Kuan Chang Wu, Yung Hung Huang, Yi Chia Chen, Tsung Rong Kuo, Chih Wen Pao, Jeng Lung Chen, Di Yan Wang

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

Abstract

Electrochemical urea oxidation reaction (UOR) is a promising alternative to the oxygen evolution reaction for reducing the overall potential of the hydrogen evolution reaction during water electrolysis. The theoretical potential for the UOR is only 0.37 V versus reversible hydrogen electrode (RHE). However, the kinetics of the six-electron transfer process involved in the UOR are inherently sluggish, resulting in high overpotential during the reaction. This study designed an active catalyst with a lower kinetic barrier in the UOR by fabricating blending CoOOH-Ni(OH)₂ nanoclusters through the structural transformation of amorphous Co-Ni hydroxide films. This structural transformation was investigated using high-angle annular dark-field scanning transmission electron microscopy, corresponding energy-dispersive X-ray spectroscopy, and in situ X-ray absorption spectra. The blending CoOOH-Ni(OH)₂ nanoclusters exhibited superior electrocatalytic activity in the UOR in an alkaline environment, achieving a low onset potential of 1.24 V (vs. RHE) in 1 M KOH with 0.5 M urea. We employed the CoOOH-Ni(OH)₂ nanoclusters as anodic electrocatalysts in a two-cell electrolyzer for asymmetric electrocatalysis. Hydrogen could be produced at a remarkable current density of 10 mA cm⁻² at a low applied potential of only 0.45 V. Density functional theory calculations revealed that blending CoOOH-Ni(OH)₂ nanoclusters with more oxygen vacancies exhibited a lower Gibbs free energy for the intermediate reaction pathway of NCONH₂ → NCONH, compared with the fine structure of CoNiO_x (x = 2-3). This study lays down a novel pathway for developing new blending electrocatalysts to be used in electrochemical reactions.

Original language	English
Journal	Journal of Materials Chemistry A
DOIs	https://doi.org/10.1039/d4ta04241g
Publication status	Accepted/In press - 2024

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

UN SDGs

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

Access to Document

10.1039/d4ta04241g

Cite this

Peng, S. M., Chang, S. T., Chang, C. C., Hn, P., Chang, C. C., Wu, K. C., Huang, Y. H., Chen, Y. C., Kuo, T. R., Pao, C. W., Chen, J. L., & Wang, D. Y. (Accepted/In press). Boosted urea electrooxidation activity by dynamic steady blending CoOOH-Ni(OH)₂ nanoclusters for H₂ production in a pH-asymmetric electrolyzer. Journal of Materials Chemistry A. https://doi.org/10.1039/d4ta04241g

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title = "Boosted urea electrooxidation activity by dynamic steady blending CoOOH-Ni(OH)2 nanoclusters for H2 production in a pH-asymmetric electrolyzer",

abstract = "Electrochemical urea oxidation reaction (UOR) is a promising alternative to the oxygen evolution reaction for reducing the overall potential of the hydrogen evolution reaction during water electrolysis. The theoretical potential for the UOR is only 0.37 V versus reversible hydrogen electrode (RHE). However, the kinetics of the six-electron transfer process involved in the UOR are inherently sluggish, resulting in high overpotential during the reaction. This study designed an active catalyst with a lower kinetic barrier in the UOR by fabricating blending CoOOH-Ni(OH)2 nanoclusters through the structural transformation of amorphous Co-Ni hydroxide films. This structural transformation was investigated using high-angle annular dark-field scanning transmission electron microscopy, corresponding energy-dispersive X-ray spectroscopy, and in situ X-ray absorption spectra. The blending CoOOH-Ni(OH)2 nanoclusters exhibited superior electrocatalytic activity in the UOR in an alkaline environment, achieving a low onset potential of 1.24 V (vs. RHE) in 1 M KOH with 0.5 M urea. We employed the CoOOH-Ni(OH)2 nanoclusters as anodic electrocatalysts in a two-cell electrolyzer for asymmetric electrocatalysis. Hydrogen could be produced at a remarkable current density of 10 mA cm−2 at a low applied potential of only 0.45 V. Density functional theory calculations revealed that blending CoOOH-Ni(OH)2 nanoclusters with more oxygen vacancies exhibited a lower Gibbs free energy for the intermediate reaction pathway of NCONH2 → NCONH, compared with the fine structure of CoNiOx (x = 2-3). This study lays down a novel pathway for developing new blending electrocatalysts to be used in electrochemical reactions.",

author = "Peng, {Shih Mao} and Chang, {Shu Ting} and Chang, {Chia Che} and Priyadarshini Hn and Chang, {Chun Chih} and Wu, {Kuan Chang} and Huang, {Yung Hung} and Chen, {Yi Chia} and Kuo, {Tsung Rong} and Pao, {Chih Wen} and Chen, {Jeng Lung} and Wang, {Di Yan}",

note = "Publisher Copyright: {\textcopyright} 2024 The Royal Society of Chemistry.",

year = "2024",

doi = "10.1039/d4ta04241g",

language = "English",

journal = "Journal of Materials Chemistry A",

issn = "2050-7488",

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T1 - Boosted urea electrooxidation activity by dynamic steady blending CoOOH-Ni(OH)2 nanoclusters for H2 production in a pH-asymmetric electrolyzer

AU - Peng, Shih Mao

AU - Chang, Shu Ting

AU - Chang, Chia Che

AU - Hn, Priyadarshini

AU - Chang, Chun Chih

AU - Wu, Kuan Chang

AU - Huang, Yung Hung

AU - Chen, Yi Chia

AU - Kuo, Tsung Rong

AU - Pao, Chih Wen

AU - Chen, Jeng Lung

AU - Wang, Di Yan

PY - 2024

Y1 - 2024

N2 - Electrochemical urea oxidation reaction (UOR) is a promising alternative to the oxygen evolution reaction for reducing the overall potential of the hydrogen evolution reaction during water electrolysis. The theoretical potential for the UOR is only 0.37 V versus reversible hydrogen electrode (RHE). However, the kinetics of the six-electron transfer process involved in the UOR are inherently sluggish, resulting in high overpotential during the reaction. This study designed an active catalyst with a lower kinetic barrier in the UOR by fabricating blending CoOOH-Ni(OH)2 nanoclusters through the structural transformation of amorphous Co-Ni hydroxide films. This structural transformation was investigated using high-angle annular dark-field scanning transmission electron microscopy, corresponding energy-dispersive X-ray spectroscopy, and in situ X-ray absorption spectra. The blending CoOOH-Ni(OH)2 nanoclusters exhibited superior electrocatalytic activity in the UOR in an alkaline environment, achieving a low onset potential of 1.24 V (vs. RHE) in 1 M KOH with 0.5 M urea. We employed the CoOOH-Ni(OH)2 nanoclusters as anodic electrocatalysts in a two-cell electrolyzer for asymmetric electrocatalysis. Hydrogen could be produced at a remarkable current density of 10 mA cm−2 at a low applied potential of only 0.45 V. Density functional theory calculations revealed that blending CoOOH-Ni(OH)2 nanoclusters with more oxygen vacancies exhibited a lower Gibbs free energy for the intermediate reaction pathway of NCONH2 → NCONH, compared with the fine structure of CoNiOx (x = 2-3). This study lays down a novel pathway for developing new blending electrocatalysts to be used in electrochemical reactions.

AB - Electrochemical urea oxidation reaction (UOR) is a promising alternative to the oxygen evolution reaction for reducing the overall potential of the hydrogen evolution reaction during water electrolysis. The theoretical potential for the UOR is only 0.37 V versus reversible hydrogen electrode (RHE). However, the kinetics of the six-electron transfer process involved in the UOR are inherently sluggish, resulting in high overpotential during the reaction. This study designed an active catalyst with a lower kinetic barrier in the UOR by fabricating blending CoOOH-Ni(OH)2 nanoclusters through the structural transformation of amorphous Co-Ni hydroxide films. This structural transformation was investigated using high-angle annular dark-field scanning transmission electron microscopy, corresponding energy-dispersive X-ray spectroscopy, and in situ X-ray absorption spectra. The blending CoOOH-Ni(OH)2 nanoclusters exhibited superior electrocatalytic activity in the UOR in an alkaline environment, achieving a low onset potential of 1.24 V (vs. RHE) in 1 M KOH with 0.5 M urea. We employed the CoOOH-Ni(OH)2 nanoclusters as anodic electrocatalysts in a two-cell electrolyzer for asymmetric electrocatalysis. Hydrogen could be produced at a remarkable current density of 10 mA cm−2 at a low applied potential of only 0.45 V. Density functional theory calculations revealed that blending CoOOH-Ni(OH)2 nanoclusters with more oxygen vacancies exhibited a lower Gibbs free energy for the intermediate reaction pathway of NCONH2 → NCONH, compared with the fine structure of CoNiOx (x = 2-3). This study lays down a novel pathway for developing new blending electrocatalysts to be used in electrochemical reactions.

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