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Cited by 306Electrocatalysts for Energy ConversionCO2 Reduction Techniques and CatalystsFuel Cells and Related Materials

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Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation

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Gao, Xintong, Bai, Xiaowan, Wang, Pengtang, Jiao, Yan, Davey, Kenneth, Zheng, Yao, Qiao, Shi-Zhang·2023·Nature Communications
DOI 10.1038/s41467-023-41588-wPMC PMC10511637
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Abstract

Renewable energy-based electrocatalytic oxidation of organic nucleophiles (e.g.methanol, urea, and amine) are more thermodynamically favourable and, economically attractive to replace conventional pure water electrooxidation in electrolyser to produce hydrogen. However, it is challenging due to the competitive oxygen evolution reaction under a high current density (e.g., >300 mA cm−2), which reduces the anode electrocatalyst’s activity and stability. Herein, taking lower energy cost urea electrooxidation reaction as the model reaction, we developed oxyanion-engineered Nickel catalysts to inhibit competing oxygen evolution reaction during urea oxidation reaction, achieving an ultrahigh 323.4 mA cm−2 current density at 1.65 V with 99.3 ± 0.4% selectivity of N-products. In situ spectra studies reveal that such in situ generated oxyanions not only inhibit OH− adsorption and guarantee high coverage of urea reactant on active sites to avoid oxygen evolution reaction, but also accelerate urea’s C − N bond cleavage to form CNO − intermediates for facilitating urea oxidation reaction. Accordingly, a comprehensive mechanism for competitive adsorption behaviour between OH− and urea to boost urea electrooxidation and dynamic change of Ni active sites during urea oxidation reaction was proposed. This work presents a feasible route for high-efficiency urea electrooxidation reaction and even various electrooxidation reactions in practical applications.

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Figures

Fig. 1 Activation of NiS2 to Ni-SOX under anodic potential. HRTEM image of a NiS2 and b Ni-SOX catalyst. c EDX elemental mapping (upper) and linear scan (lower) for Ni-SOX. d S 2p XPS curves for NiS2 and Ni-SOX catalyst.
Fig. 1 Activation of NiS2 to Ni-SOX under anodic potential. HRTEM image of a NiS2 and b Ni-SOX catalyst. c EDX elemental mapping (upper) and linear scan (lower) for Ni-SOX. d S 2p XPS curves for NiS2 and Ni-SOX catalyst.CC BY · PubMed Central
Fig. 2 Electrocatalytic UOR performance for Ni-SOX and NiOX. a ECSA-normalized LSV curves in 1 M KOH solution with (solid line), or without (dash line) 0.33 M urea. b Comparison of current density on Ni-SOX with reported powder catalysts under a 1.50 − 1.65 V potential zone for UOR. c In situ evaluation of O2 on Ni-SOX and NiOX using RRDE in 1 M KOH with 0.33 M urea. d Multi-step chronopotentiometric test at different potentials from 1.30 to 1.70 V. e Long-term chronopotentiometric stability determined at current density 50 mA cm −2. f Comparison of Ni3+ reduction peaks for Ni-SOX and NiOX in 1 M KOH with (solid line) or without (dash line) 0.33 M urea.
Fig. 2 Electrocatalytic UOR performance for Ni-SOX and NiOX. a ECSA-normalized LSV curves in 1 M KOH solution with (solid line), or without (dash line) 0.33 M urea. b Comparison of current density on Ni-SOX with reported powder catalysts under a 1.50 − 1.65 V potential zone for UOR. c In situ evaluation of O2 on Ni-SOX and NiOX using RRDE in 1 M KOH with 0.33 M urea. d Multi-step chronopotentiometric test at different potentials from 1.30 to 1.70 V. e Long-term chronopotentiometric stability determined at current density 50 mA cm −2. f Comparison of Ni3+ reduction peaks for Ni-SOX and NiOX in 1 M KOH with (solid line) or without (dash line) 0.33 M urea.CC BY · PubMed Central
Fig. 3 UOR /OER selectivity quantification. In situ detection of the representative gaseous products of UOR (N2) and OER (O2) via DEMS (upper) and the corresponding current acquired in 1 M KOH with 0.33 M urea (lower, without iR correction) on a Ni-SOX and b NiOX. FEs for different UOR /OER products under different potentials on c Ni-SOX and d NiOX. Error bars correspond to the standard deviation of three independent measurements.
Fig. 3 UOR /OER selectivity quantification. In situ detection of the representative gaseous products of UOR (N2) and OER (O2) via DEMS (upper) and the corresponding current acquired in 1 M KOH with 0.33 M urea (lower, without iR correction) on a Ni-SOX and b NiOX. FEs for different UOR /OER products under different potentials on c Ni-SOX and d NiOX. Error bars correspond to the standard deviation of three independent measurements.CC BY · PubMed Central
Fig. 4 Dynamic state change of Ni during UOR. a In situ Ni K-edge XANES spectra for Ni-SOX under varying potential during UOR. Inset, magnified absorption edge region. In situ Raman spectra for Ni-SOX electrode in 1 M KOH b with, and c without, 0.33 M urea at applied potentials. d In situ Raman spectra for NiOX electrode in 1 M KOH with 0.33 M urea.
Fig. 4 Dynamic state change of Ni during UOR. a In situ Ni K-edge XANES spectra for Ni-SOX under varying potential during UOR. Inset, magnified absorption edge region. In situ Raman spectra for Ni-SOX electrode in 1 M KOH b with, and c without, 0.33 M urea at applied potentials. d In situ Raman spectra for NiOX electrode in 1 M KOH with 0.33 M urea.CC BY · PubMed Central
Fig. 5 UOR mechanism analyses. a–d In situ ATR-IR spectra in potential window 1.20 to 1.60 V for Ni-SOX and for NiOX in different ranges. e, f Schematic for competing adsorption of urea and hydroxyl on Ni-SOX and NiOX surfaces.
Fig. 5 UOR mechanism analyses. a–d In situ ATR-IR spectra in potential window 1.20 to 1.60 V for Ni-SOX and for NiOX in different ranges. e, f Schematic for competing adsorption of urea and hydroxyl on Ni-SOX and NiOX surfaces.CC BY · PubMed Central
Fig. 6 UOR /OER competition mechanism. a RRDE curves for NiOX obtained in different concentration of KOH with 0.33 M urea. b RRDE curves for NiOX obtained in 1 M KOH with different concentrations of urea. c Representation for UOR mechanism on Ni-SOX accompanying adsorption of reactants and dynamic evolution of active sites under high potential (>1.50 V). d Representation of UOR and OER mechanism on NiOX accompanying adsorption of reactants and dynamic evolution of active sites under high potential (>1.50 V).
Fig. 6 UOR /OER competition mechanism. a RRDE curves for NiOX obtained in different concentration of KOH with 0.33 M urea. b RRDE curves for NiOX obtained in 1 M KOH with different concentrations of urea. c Representation for UOR mechanism on Ni-SOX accompanying adsorption of reactants and dynamic evolution of active sites under high potential (>1.50 V). d Representation of UOR and OER mechanism on NiOX accompanying adsorption of reactants and dynamic evolution of active sites under high potential (>1.50 V).CC BY · PubMed Central

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Metadata

Authors
Gao, X., Bai, X., Wang, P., Jiao, Y., Davey, K., Zheng, Y., & Qiao, S.-Z.
Affiliations
The University of Adelaide (AU)
Corresponding author
  • Zheng, Yao
  • Qiao, Shi-Zhang
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2023-09-20
Volume
14
Issue
1
Pages
5842-5842
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-023-41588-w
PMC
PMC10511637
OpenAlex
W4386887861
Cited by
306
References
43
Citations by year
2026: 74 · 2025: 125 · 2024: 102 · 2023: 5
FWCI
14.62
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)
  • Adelaide Research & Scholarship (AR&S) (University of Adelaide) (submittedVersion, cc-by)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders
  • Australian Nuclear Science and Technology Organisation
  • Australian Synchrotron
  • University of Adelaide
  • China Scholarship Council
  • Australian Research Council (FT200100062, DP190103472, DP220102596, LP210301397, FL170100154)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
Keywords
urea electrooxidation, nickel-based electrocatalysts, competitive adsorption, hydroxide adsorption, C–N bond cleavage, electrocatalytic hydrogen production, anode catalysts

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