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Cited by 713Electrocatalysts for Energy ConversionCO2 Reduction Techniques and CatalystsHydrogen Storage and Materials

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Morphology and surface chemistry engineering toward pH-universal catalysts for hydrogen evolution at high current density

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Luo, Yuting, Tang, Lei, Khan, Usman, Yu, Qiangmin, Cheng, Hui-Ming, Zou, Xiaolong, Liu, Bilu·2019·Nature Communications
DOI 10.1038/s41467-018-07792-9PMC PMC6336864
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Abstract

Large-scale implementation of electrochemical hydrogen production requires several fundamental issues to be solved, including understanding the mechanism and developing inexpensive electrocatalysts that work well at high current densities. Here we address these challenges by exploring the roles of morphology and surface chemistry, and develop inexpensive and efficient electrocatalysts for hydrogen evolution. Three model electrocatalysts are flat platinum foil, molybdenum disulfide microspheres, and molybdenum disulfide microspheres modified by molybdenum carbide nanoparticles. The last catalyst is highly active for hydrogen evolution independent of pH, with low overpotentials of 227 mV in acidic medium and 220 mV in alkaline medium at a high current density of 1000 mA cm−2, because of enhanced transfer of mass (reactants and hydrogen bubbles) and fast reaction kinetics due to surface oxygen groups formed on molybdenum carbide during hydrogen evolution. Our work may guide rational design of electrocatalysts that work well at high current densities.

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Fig. 1 Synthesis and characterization. a Design schematic of the MoS2/Mo2C. b Scanning electron microscopy (SEM) image of the synthesized MoS2/Mo2C. The scale bar is 20 μm. The inset is an enlarged view of the dotted square and is a microsphere of MoS2/Mo2C. The scale bar is 1 μm. c–e High-resolution transmission electron microscopy (HRTEM) images of the MoS2/Mo2C. Insets in (c) and (e) are enlarged views and the corresponding fast Fourier transform (FFT) pattern, respectively. The images (d) and (e) are enlarged views of the squares outlined in red and blue in (c). The scale bars are 5 nm in (c) and 0.5 nm in (d, e). f Raman spectrum of MoS2/Mo2C. Inset shows a spectrum from 1300 to 1600 cm−1, indicating no graphitic carbon materials were produced. g X-ray photoelectron spectroscopy (XPS) spectra of Mo 3d of MoS2 and MoS2/Mo2C. Two peaks originating from Mo2+ appear in the MoS2/Mo2C samples
Fig. 1 Synthesis and characterization. a Design schematic of the MoS2/Mo2C. b Scanning electron microscopy (SEM) image of the synthesized MoS2/Mo2C. The scale bar is 20 μm. The inset is an enlarged view of the dotted square and is a microsphere of MoS2/Mo2C. The scale bar is 1 μm. c–e High-resolution transmission electron microscopy (HRTEM) images of the MoS2/Mo2C. Insets in (c) and (e) are enlarged views and the corresponding fast Fourier transform (FFT) pattern, respectively. The images (d) and (e) are enlarged views of the squares outlined in red and blue in (c). The scale bars are 5 nm in (c) and 0.5 nm in (d, e). f Raman spectrum of MoS2/Mo2C. Inset shows a spectrum from 1300 to 1600 cm−1, indicating no graphitic carbon materials were produced. g X-ray photoelectron spectroscopy (XPS) spectra of Mo 3d of MoS2 and MoS2/Mo2C. Two peaks originating from Mo2+ appear in the MoS2/Mo2C samplesCC BY · PubMed Central
Fig. 2 Electrocatalytic performance of different catalysts at high current densities. a Polarization curves and b Tafel curves after iR compensation for a Pt foil, MoS2, and MoS2/Mo2C in KOH (1 M) at a scan rate of 5 mV s−1. c Ratios of ∆η/∆log|j|, i.e., Rη/j, for the three catalysts in different current density ranges, which can be used as an indicator to evaluate the performance of a catalyst at high current densities. All points were tested three times, and error bars correspond to standard deviations. Source data are provided as a Source Data file. d CAs of a KOH (1 M) droplet on the surfaces of the catalyst. The CAs were measured for at least three times for each sample, and error bars correspond to standard deviations. Source data are provided as a Source Data file. e Photos show sharp contrast during the release of H2 bubbles on the Pt foil and on MoS2/Mo2C surfaces. The scale bars are 1 mm. f Size distributions of H2 bubbles on the surfaces of a Pt foil and MoS2/Mo2C. Source data are provided as a Source Data file
Fig. 2 Electrocatalytic performance of different catalysts at high current densities. a Polarization curves and b Tafel curves after iR compensation for a Pt foil, MoS2, and MoS2/Mo2C in KOH (1 M) at a scan rate of 5 mV s−1. c Ratios of ∆η/∆log|j|, i.e., Rη/j, for the three catalysts in different current density ranges, which can be used as an indicator to evaluate the performance of a catalyst at high current densities. All points were tested three times, and error bars correspond to standard deviations. Source data are provided as a Source Data file. d CAs of a KOH (1 M) droplet on the surfaces of the catalyst. The CAs were measured for at least three times for each sample, and error bars correspond to standard deviations. Source data are provided as a Source Data file. e Photos show sharp contrast during the release of H2 bubbles on the Pt foil and on MoS2/Mo2C surfaces. The scale bars are 1 mm. f Size distributions of H2 bubbles on the surfaces of a Pt foil and MoS2/Mo2C. Source data are provided as a Source Data fileCC BY · PubMed Central
Fig. 3 Performance and surface chemistry of catalysts. a Overpotentials at 1000 mA cm−2 for a Pt foil, MoS2, and MoS2/Mo2C in acidic and alkaline media. Each sample was measured for three times, and error bars correspond to standard deviations. Source data are provided as a Source Data file. b Tafel slopes (at a current density smaller than 50 mA cm−2) for a Pt foil, MoS2, and MoS2/Mo2C in acidic and alkaline media. Each sample was measured for three times, and error bars correspond to standard deviations. Source data are provided as a Source Data file. c Polarization curves of the MoS2/Mo2C catalyst during the initial scan and after 10,000 scans. Inset shows the chronoamperometric responses (i–t) recorded on MoS2/Mo2C for 24 h in both media. d O 1s X-ray photoelectron spectroscopy (XPS) spectra of the MoS2/Mo2C sample before and after 100 cycles in KOH (1.0 M) and H2SO4 (0.5 M) solutions
Fig. 3 Performance and surface chemistry of catalysts. a Overpotentials at 1000 mA cm−2 for a Pt foil, MoS2, and MoS2/Mo2C in acidic and alkaline media. Each sample was measured for three times, and error bars correspond to standard deviations. Source data are provided as a Source Data file. b Tafel slopes (at a current density smaller than 50 mA cm−2) for a Pt foil, MoS2, and MoS2/Mo2C in acidic and alkaline media. Each sample was measured for three times, and error bars correspond to standard deviations. Source data are provided as a Source Data file. c Polarization curves of the MoS2/Mo2C catalyst during the initial scan and after 10,000 scans. Inset shows the chronoamperometric responses (i–t) recorded on MoS2/Mo2C for 24 h in both media. d O 1s X-ray photoelectron spectroscopy (XPS) spectra of the MoS2/Mo2C sample before and after 100 cycles in KOH (1.0 M) and H2SO4 (0.5 M) solutionsCC BY · PubMed Central
Fig. 4 Self-optimized surface oxygen on the (101) surface of β-Mo2C to enable fast kinetics. a X-ray photoelectron spectroscopy (XPS) spectra of β-Mo2C that has undergone the hydrogen reduction reaction at different pH values and potentials. b Models and binding energies of surface oxygenated species, including –OH (blue, 531.6 eV), –O (green, 532.5 eV), and H2O (red, 533.5 eV). c Pourbaix diagram of Mo2C (101) at different pH values and potentials. Here, “Ox” and “Hyd” stand for –O and –OH terminated Mo2C surfaces, while “Mo2C” represents the free surface. d–g DFT calculations showing adsorption energies for d H on –OH terminated, and e disassociated H2O on –O terminated Mo2C (101) as a function of adsorbed species. g, f The top and side views of the corresponding optimized structures, where (dark) green, gray, red, and white spheres represent Mo, C, O, and H atoms, respectively
Fig. 4 Self-optimized surface oxygen on the (101) surface of β-Mo2C to enable fast kinetics. a X-ray photoelectron spectroscopy (XPS) spectra of β-Mo2C that has undergone the hydrogen reduction reaction at different pH values and potentials. b Models and binding energies of surface oxygenated species, including –OH (blue, 531.6 eV), –O (green, 532.5 eV), and H2O (red, 533.5 eV). c Pourbaix diagram of Mo2C (101) at different pH values and potentials. Here, “Ox” and “Hyd” stand for –O and –OH terminated Mo2C surfaces, while “Mo2C” represents the free surface. d–g DFT calculations showing adsorption energies for d H on –OH terminated, and e disassociated H2O on –O terminated Mo2C (101) as a function of adsorbed species. g, f The top and side views of the corresponding optimized structures, where (dark) green, gray, red, and white spheres represent Mo, C, O, and H atoms, respectivelyCC BY · PubMed Central

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Metadata

Authors
Luo, Y., Tang, L., Khan, U., Yu, Q., Cheng, H.-M., Zou, X., & Liu, B.
Affiliations
  • Tsinghua–Berkeley Shenzhen Institute (CN)
  • Chinese Academy of Sciences (CN)
Corresponding author
  • Zou, Xiaolong
  • Liu, Bilu
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2019-01-17
Volume
10
Issue
1
Pages
269-269
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-018-07792-9
PMC
PMC6336864
OpenAlex
W2915424365
Cited by
713
References
53
Citations by year
2026: 49 · 2025: 92 · 2024: 133 · 2023: 117 · 2022: 120 · 2021: 92 · 2020: 67 · 2019: 43
FWCI
17.13
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • Europe PMC (PubMed Central) (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion)
Funders
  • National Natural Science Foundation of China (51722206, JCYJ20170307140956657)
  • Development and Reform Commission of Shenzhen Municipality (JCYJ20170307140956657, 51722206)
  • Shenzhen Fundamental Research Program (JCYJ20170307140956657)
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 › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
Keywords
hydrogen evolution reaction, electrocatalysts, molybdenum carbide nanoparticles, catalyst morphology, surface chemistry, high current density, mass transfer, surface oxygen groups, platinum foil, acidic and alkaline media, electrochemical hydrogen production

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