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Cited by 427Electrocatalysts for Energy ConversionCatalytic Processes in Materials ScienceCO2 Reduction Techniques and Catalysts

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Iridium single atoms incorporated in Co3O4 efficiently catalyze the oxygen evolution in acidic conditions

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Zhu, Yiming, Wang, Jiaao, Koketsu, Toshinari, Kroschel, Matthias, Chen, Jin-Ming, Hsu, Su-Yang, Henkelman, Graeme, Hu, Zhiwei, Strasser, Peter, Ma, Jiwei·2022·Nature Communications
DOI 10.1038/s41467-022-35426-8PMC PMC9751110
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Abstract

Abstract Designing active and stable electrocatalysts with economic efficiency for acidic oxygen evolution reaction is essential for developing proton exchange membrane water electrolyzers. Herein, we report on a cobalt oxide incorporated with iridium single atoms (Ir-Co 3 O 4 ), prepared by a mechanochemical approach. Operando X-ray absorption spectroscopy reveals that Ir atoms are partially oxidized to active Ir >4+ during the reaction, meanwhile Ir and Co atoms with their bridged electrophilic O ligands acting as active sites, are jointly responsible for the enhanced performance. Theoretical calculations further disclose the isolated Ir atoms can effectively boost the electronic conductivity and optimize the energy barrier. As a result, Ir-Co 3 O 4 exhibits significantly higher mass activity and turnover frequency than those of benchmark IrO 2 in acidic conditions. Moreover, the catalyst preparation can be easily scaled up to gram-level per batch. The present approach highlights the concept of constructing single noble metal atoms incorporated cost-effective metal oxides catalysts for practical applications.

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Crossref · 10.1038/s41467-022-35426-8

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Figures

Fig. 1 Structural characterizations of Ir-Co3O4. a SEM, (b) TEM, (c) AFM and (d) HR-TEM images of Ir-Co3O4. Inset in (c) is the height profile of Ir-Co3O4 along the dashed line. e AC HAADF-STEM image and the corresponding FFT image (inset) of Ir-Co3O4. f The enlarged area in (e), with the Ir single atoms marked in circles, and (g) intensity profiles along the dashed rectangles. h 3D atom-overlapping Gaussian function fitting mapping of the selected area in (e). i AC HAADF-STEM image and the corresponding elemental mappings of Ir-Co3O4.
Fig. 1 Structural characterizations of Ir-Co3O4. a SEM, (b) TEM, (c) AFM and (d) HR-TEM images of Ir-Co3O4. Inset in (c) is the height profile of Ir-Co3O4 along the dashed line. e AC HAADF-STEM image and the corresponding FFT image (inset) of Ir-Co3O4. f The enlarged area in (e), with the Ir single atoms marked in circles, and (g) intensity profiles along the dashed rectangles. h 3D atom-overlapping Gaussian function fitting mapping of the selected area in (e). i AC HAADF-STEM image and the corresponding elemental mappings of Ir-Co3O4.CC BY · PubMed Central
Fig. 2 Electronic and atomic structure analysis of Ir-Co3O4. a Ir 4f XPS spectra of Ir-Co3O4 and IrO2. b Co 2p XPS spectra and (c) O 1 s XPS spectra of Ir-Co3O4 and Co3O4. d XANES spectra of Ir-L3 edge on Ir-Co3O4, Ir foil and IrO2. d The normalized Ir-L3 edge XANES spectra of Ir-Co3O4, Ir foil and IrO2. e Ir-L3 edge EXAFS spectra and (f) corresponding wavelet-transformed k3-weighted EXAFS spectra of Ir-Co3O4, Ir foil and IrO2. g The normalized Co-K edge XANES spectra and (h) Co-K edge XANES spectra of Ir-Co3O4 and Co3O4.
Fig. 2 Electronic and atomic structure analysis of Ir-Co3O4. a Ir 4f XPS spectra of Ir-Co3O4 and IrO2. b Co 2p XPS spectra and (c) O 1 s XPS spectra of Ir-Co3O4 and Co3O4. d XANES spectra of Ir-L3 edge on Ir-Co3O4, Ir foil and IrO2. d The normalized Ir-L3 edge XANES spectra of Ir-Co3O4, Ir foil and IrO2. e Ir-L3 edge EXAFS spectra and (f) corresponding wavelet-transformed k3-weighted EXAFS spectra of Ir-Co3O4, Ir foil and IrO2. g The normalized Co-K edge XANES spectra and (h) Co-K edge XANES spectra of Ir-Co3O4 and Co3O4.CC BY · PubMed Central
Fig. 3 Electrochemical OER of Ir-Co3O4. a Polarization curves of Ir-Co3O4, IrO2, Co3O4 and C-Co3O4 in 0.5 M H2SO4 at a scanning rate of 5 mV s−1. b Tafel plots derived from the polarization curves in (a). c Corresponding specific activities of Ir-Co3O4, IrO2, Co3O4 and C-Co3O4; TOF values of Ir-Co3O4 and IrO2 at the overpotential of 300 mV. d Comparison of overpotentials and Tafel plots in reported Ir-based OER electrocatalysts. e Comparison of the mass activities normalized to Ir mass on Ir-Co3O4 and IrO2. f EIS Nyquist plots and fitting curves of samples recorded at the 1.43 V vs. RHE. g Chronopotentiometric measurements of Ir-Co3O4, IrO2, Co3O4 and C-Co3O4 at 10 mA cm−2, carbon paper was used as the catalyst support. h Dissolved Ir (left-y axis) and Co (right-y axis) ion concentrations measured for Ir-Co3O4, IrO2, Co3O4 and C-Co3O4 in the electrolyte by ICP-OES. i Generated O2 amount and corresponding Faradaic efficiency over a range of overpotentials on Ir-Co3O4. Note: error bars represent the standard deviation of three independent measurements.
Fig. 3 Electrochemical OER of Ir-Co3O4. a Polarization curves of Ir-Co3O4, IrO2, Co3O4 and C-Co3O4 in 0.5 M H2SO4 at a scanning rate of 5 mV s−1. b Tafel plots derived from the polarization curves in (a). c Corresponding specific activities of Ir-Co3O4, IrO2, Co3O4 and C-Co3O4; TOF values of Ir-Co3O4 and IrO2 at the overpotential of 300 mV. d Comparison of overpotentials and Tafel plots in reported Ir-based OER electrocatalysts. e Comparison of the mass activities normalized to Ir mass on Ir-Co3O4 and IrO2. f EIS Nyquist plots and fitting curves of samples recorded at the 1.43 V vs. RHE. g Chronopotentiometric measurements of Ir-Co3O4, IrO2, Co3O4 and C-Co3O4 at 10 mA cm−2, carbon paper was used as the catalyst support. h Dissolved Ir (left-y axis) and Co (right-y axis) ion concentrations measured for Ir-Co3O4, IrO2, Co3O4 and C-Co3O4 in the electrolyte by ICP-OES. i Generated O2 amount and corresponding Faradaic efficiency over a range of overpotentials on Ir-Co3O4. Note: error bars represent the standard deviation of three independent measurements.CC BY · PubMed Central
Fig. 4 Operando XANES analysis and energetic properties of Ir-Co3O4 for OER. a The Ir L3-edge XANES and (b) the Co K-edge XANES of Ir-Co3O4 measured in 0.5 M H2SO4 under pristine state, OCP, OER operating condition of 1.6 V and OCP after OER operation. Ir L3-edge XANES of Ir foil and IrO2, and Co K-edge XANES of Co3O4 are used as references. c The white line positions and the absorption edge positions of all measured XANES. d The top and side panels of charge density difference on Ir-Co3O4. e Comparison of the d-band center of Ir-Co3O4 and Co3O4. Corresponding Co 3d, O 2p and Ir 5d pDOS spectra of (f) Ir-Co3O4 and (g) Co3O4. h The Gibbs free energy diagrams of the four-electron OER process on the Ir sites and Co sites of these catalysts under the applied overpotentials of 1.23 V vs. RHE, respectively.
Fig. 4 Operando XANES analysis and energetic properties of Ir-Co3O4 for OER. a The Ir L3-edge XANES and (b) the Co K-edge XANES of Ir-Co3O4 measured in 0.5 M H2SO4 under pristine state, OCP, OER operating condition of 1.6 V and OCP after OER operation. Ir L3-edge XANES of Ir foil and IrO2, and Co K-edge XANES of Co3O4 are used as references. c The white line positions and the absorption edge positions of all measured XANES. d The top and side panels of charge density difference on Ir-Co3O4. e Comparison of the d-band center of Ir-Co3O4 and Co3O4. Corresponding Co 3d, O 2p and Ir 5d pDOS spectra of (f) Ir-Co3O4 and (g) Co3O4. h The Gibbs free energy diagrams of the four-electron OER process on the Ir sites and Co sites of these catalysts under the applied overpotentials of 1.23 V vs. RHE, respectively.CC BY · PubMed Central

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Research works printed but not linked: 2

  1. Zhang, L. et al. Facet dependent oxygen evolution activity of spinel cobalt oxides. J. Electrochem. 28, 2108481 (2022).
  2. Agrestini, S. et al. Nature of the magnetism of iridium in the double perovskite Sr2CoIrO6. Phys. Rev. B 100, 014443 (2019). · DOI

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Metadata

Authors
Zhu, Y., Wang, J., Koketsu, T., Kroschel, M., Chen, J.-M., Hsu, S.-Y., Henkelman, G., Hu, Z., Strasser, P., & Ma, J.
Affiliations
  • Tongji University (CN)
  • The University of Texas at Austin (US)
  • Technische Universität Berlin (DE)
  • National Synchrotron Radiation Research Center (TW)
  • Max Planck Institute for Chemical Physics of Solids (DE)
Corresponding author
  • Hu, Zhiwei
  • Strasser, Peter
  • Ma, Jiwei
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2022-12-14
Volume
13
Issue
1
Pages
7754-7754
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-022-35426-8
PMC
PMC9751110
OpenAlex
W4311441455
Cited by
420
References
74
Citations by year
2026: 98 · 2025: 140 · 2024: 128 · 2023: 54
FWCI
14.50
Type
journal article
Language
en
Update notices
correction (2024-02-15)
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DepositOnce (submittedVersion, cc-by)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • Technische Universität Berlin – Universitätsbibliothek (cc-by)
Funders
  • Welch Foundation (F-1841)
  • Deutsche Forschungsgemeinschaft (STR 596/11-1)
  • National Natural Science Foundation of China (22179098)
  • Bundesministerium für Bildung und Forschung (H2Giga)
  • Pohang University of Science and Technology
  • Fundamental Research Funds for the Central Universities
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords
iridium single atoms, Co3O4, oxygen evolution reaction, acidic electrocatalysts, mechanochemical synthesis, proton exchange membrane water electrolysis, operando X-ray absorption spectroscopy, electronic conductivity, energy barrier, mass activity, turnover frequency

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