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Cited by 369Electrocatalysts for Energy ConversionFuel Cells and Related MaterialsCO2 Reduction Techniques and Catalysts

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Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis

Open access
Li, Lu, Zhang, Gengwei, Zhou, Chenhui, Lv, Fan, Tan, Yingjun, Han, Ying, Luo, Heng, Wang, Dawei, Liu, Youxing, Shang, Changshuai, Zeng, Lingyou, Huang, Qizheng, Zeng, Ruijin, Ye, Na, Luo, Mingchuan, Guo, Shaojun·2024·Nature Communications
DOI 10.1038/s41467-024-49281-2PMC PMC11166638
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Abstract

Precisely modulating the Ru-O covalency in RuO x for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d -valence electrons, which were doped into or alloyed with RuO x , are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5 s /5 p orbitals. Theoretical calculations confirm that the durability of Ln-RuO x following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuO x , Er-RuO x is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO 2 . Particularly, the Er-RuO x -based device requires only 1.837 V to reach 3 A cm −2 and shows a long-term stability at 500 mA cm −2 for 100 h with a degradation rate of mere 37 μV h −1 .

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Crossref · 10.1038/s41467-024-49281-2

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Figures

Fig. 1 Prediction of the OER performance utilizing DFT calculations. a The qualitative molecular orbital diagram obtained from [RuO6] and [LnO6]. b The ΔGO vacancy and (c) ΔGRu vacancy as a function of -ICOHP for Ln-RuOx. The upshift values of ICOHP indicate lower Ru–O covalency. d The reaction paths on Er-RuOx and RuO2 at 1.23 V. e Volcano plot for different electrocatalysts and corresponding structures.
Fig. 1 Prediction of the OER performance utilizing DFT calculations. a The qualitative molecular orbital diagram obtained from [RuO6] and [LnO6]. b The ΔGO vacancy and (c) ΔGRu vacancy as a function of -ICOHP for Ln-RuOx. The upshift values of ICOHP indicate lower Ru–O covalency. d The reaction paths on Er-RuOx and RuO2 at 1.23 V. e Volcano plot for different electrocatalysts and corresponding structures.CC BY · PubMed Central
Fig. 2 Atomic-scale structure characterization of Er-RuOx. a HAADF-STEM and b surface plot of Er-RuOx along [001] zone axes, scale bar: 2 nm. c Atomic STEM image along [001] zone axes and structural model (inset) of Er-RuOx, scale bar: 2 Å. d HAADF-STEM (scale bar: 2 nm) and (e) atomic STEM images (scale bar: 2 Å) of Er-RuOx along [110] zone axes. f EDS line scan of O, Ru, and Er signal recorded from the green line OO’ in (d). HAADF-STEM image and corresponding element mapping images of Er-RuOx along the (g–k) [110] and (l–p) [001] zone axes, scale bar: 2 nm. q Schematic illustration of Er-RuOx.
Fig. 2 Atomic-scale structure characterization of Er-RuOx. a HAADF-STEM and b surface plot of Er-RuOx along [001] zone axes, scale bar: 2 nm. c Atomic STEM image along [001] zone axes and structural model (inset) of Er-RuOx, scale bar: 2 Å. d HAADF-STEM (scale bar: 2 nm) and (e) atomic STEM images (scale bar: 2 Å) of Er-RuOx along [110] zone axes. f EDS line scan of O, Ru, and Er signal recorded from the green line OO’ in (d). HAADF-STEM image and corresponding element mapping images of Er-RuOx along the (g–k) [110] and (l–p) [001] zone axes, scale bar: 2 nm. q Schematic illustration of Er-RuOx.CC BY · PubMed Central
Fig. 3 Electrocatalytic performance of the as-prepared catalysts. a OER polarization curves of home-made RuO2, Er-RuOx and commercial RuO2 with iR-corrected (95%), where R was measured to be 1.1 ± 0.1 Ω. b Tafel plots of home-made RuO2, Er-RuOx and commercial RuO2. c Polarization curves of Er-RuOx and commercial RuO2 before (solid line) and after (dash line) 30,000 CV cycles. d The CP curves of Er-RuOx and commercial RuO2 at 10 mA cm−2. e Schematic diagram of the PEMWE electrolyzer. f Polarization curves of the Er-RuOx and commercial RuO2-based PEMWE at 80 °C. g The CP curves of Er-RuOx-based PEMWE electrolyzer operated at 200, 500, and 1000 mA cm−2, respectively.
Fig. 3 Electrocatalytic performance of the as-prepared catalysts. a OER polarization curves of home-made RuO2, Er-RuOx and commercial RuO2 with iR-corrected (95%), where R was measured to be 1.1 ± 0.1 Ω. b Tafel plots of home-made RuO2, Er-RuOx and commercial RuO2. c Polarization curves of Er-RuOx and commercial RuO2 before (solid line) and after (dash line) 30,000 CV cycles. d The CP curves of Er-RuOx and commercial RuO2 at 10 mA cm−2. e Schematic diagram of the PEMWE electrolyzer. f Polarization curves of the Er-RuOx and commercial RuO2-based PEMWE at 80 °C. g The CP curves of Er-RuOx-based PEMWE electrolyzer operated at 200, 500, and 1000 mA cm−2, respectively.CC BY · PubMed Central
Fig. 4 Structural characterization of Er-RuOx and RuO2. a Ru K-edge XANES spectra of Ru foil, RuO2, and Er-RuOx. b EXAFS spectra of Ru foil, RuO2, and Er-RuOx. In situ Raman spectra obtained under various applied potential on (c) RuO2 and (d) Er-RuOx. e Ru K-edge XANES spectra of Er-RuOx with different applied bias. f The variation trend of Ru oxidation states in RuO2 and Er-RuOx under different potentials. WT-EXAFS of (g) Ru foil, (h) RuO2, and (i) Er-RuOx.
Fig. 4 Structural characterization of Er-RuOx and RuO2. a Ru K-edge XANES spectra of Ru foil, RuO2, and Er-RuOx. b EXAFS spectra of Ru foil, RuO2, and Er-RuOx. In situ Raman spectra obtained under various applied potential on (c) RuO2 and (d) Er-RuOx. e Ru K-edge XANES spectra of Er-RuOx with different applied bias. f The variation trend of Ru oxidation states in RuO2 and Er-RuOx under different potentials. WT-EXAFS of (g) Ru foil, (h) RuO2, and (i) Er-RuOx.CC BY · PubMed Central
Fig. 5 Analysis of adsorption behavior. a The calculated PDOS of Ru d, O p, and Er f orbitals of Er-RuOx. b The PDOS of Ru dz² orbital of RuO2 and Er-RuOx. c Schematic diagram of orbital hybridization between dz² orbital of RuO2 and Er-RuOx and the *OH bonding orbitals. d Charge density difference of *OH-adsorbed Er-RuOx (left) and RuO2 (right). Yellow and blue iso-surfaces represent charge accumulation and depletion, respectively. Polarization curves of (e) RuO2 and (f) Er-RuOx in 0.5 M H2SO4 solution with (dashed lines) and without (solid lines) 1 M methanol. g Current difference between the polarization curves in 0.5 M H2SO4 solution with and without 1.0 M methanol for Er-RuOx and RuO2. ATR-SEIRAS analysis of (h) commercial RuO2 and (i) Er-RuOx.
Fig. 5 Analysis of adsorption behavior. a The calculated PDOS of Ru d, O p, and Er f orbitals of Er-RuOx. b The PDOS of Ru dz² orbital of RuO2 and Er-RuOx. c Schematic diagram of orbital hybridization between dz² orbital of RuO2 and Er-RuOx and the *OH bonding orbitals. d Charge density difference of *OH-adsorbed Er-RuOx (left) and RuO2 (right). Yellow and blue iso-surfaces represent charge accumulation and depletion, respectively. Polarization curves of (e) RuO2 and (f) Er-RuOx in 0.5 M H2SO4 solution with (dashed lines) and without (solid lines) 1 M methanol. g Current difference between the polarization curves in 0.5 M H2SO4 solution with and without 1.0 M methanol for Er-RuOx and RuO2. ATR-SEIRAS analysis of (h) commercial RuO2 and (i) Er-RuOx.CC BY · PubMed Central

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Authors
Li, L., Zhang, G., Zhou, C., Lv, F., Tan, Y., Han, Y., Luo, H., Wang, D., Liu, Y., Shang, C., Zeng, L., Huang, Q., Zeng, R., Ye, N., Luo, M., & Guo, S.
Affiliations
  • Peking University (CN)
  • Kunming University of Science and Technology (CN)
Corresponding author
Guo, Shaojun
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2024-06-11
Volume
15
Issue
1
Pages
4974-4974
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-024-49281-2
PMC
PMC11166638
OpenAlex
W4399539823
Cited by
368
References
37
Citations by year
2026: 121 · 2025: 206 · 2024: 41
FWCI
24.53
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion)
Funders
  • Salt Science Research Foundation (BL14W1)
  • National Natural Science Foundation of China (52261135633, 52303363, 22105007, 22309004, 52333010, 22205010, 52025133)
  • China Postdoctoral Science Foundation (2022M710187, 2020M670018, 2023M730051, 2023M730029, 2022M720225)
  • China National Petroleum Corporation (2021DQ02-1002)
  • Peking University (2021DQ02-1002)
  • National Postdoctoral Program for Innovative Talents (BX20220009)
  • Beijing Synchrotron Radiation Facility (BL14W1)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords
lanthanide doping, acidic oxygen evolution reaction, proton exchange membrane water electrolysis, catalyst stability, coordination environment, volcano plot, electrocatalyst degradation

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