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Cited by 230Electrocatalysts for Energy ConversionSurface Modification and SuperhydrophobicityMinerals Flotation and Separation Techniques

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Superaerophilic/superaerophobic cooperative electrode for efficient hydrogen evolution reaction via enhanced mass transfer

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Zhang, Chunhui, Xu, Zhe, Han, Nana, Tian, Ye, Kallio, Tanja, Yu, Cunming, Jiang, Lei·2023·Science Advances
DOI 10.1126/sciadv.add6978PMC PMC9848275
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Abstract

Hydrogen evolution reaction (HER), as an effective method to produce green hydrogen, is greatly impeded by inefficient mass transfer, i.e., bubble adhesion on electrode, bubble dispersion in the vicinity of electrode, and poor dissolved H 2 diffusion, which results in blocked electrocatalytic area and large H 2 concentration overpotential. Here, we report a superaerophilic/superaerophobic (SAL/SAB) cooperative electrode to efficiently promote bubble transfer by asymmetric Laplace pressure and accelerate dissolved H 2 diffusion through reducing diffusion distance. Benefiting from the enhanced mass transfer, the overpotential for the SAL/SAB cooperative electrode at −10 mA cm −2 is only −19 mV, compared to −61 mV on the flat Pt electrode. By optimizing H 2 SO 4 concentration, the SAL/SAB cooperative electrode can achieve ultrahigh current density (−1867 mA cm −2 ) at an overpotential of −500 mV. We can envision that the SAL/SAB cooperative strategy is an effective method to improve HER efficiency and stimulate the understanding of various gas-involved processes.

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Figures

Fig. 1. The SAL/flat Pt electrode with intensified HER through mass transfer enhancement. (A) Optical image of the SAL/flat Pt electrode composed of SAL stripes and Pt. A glass vessel was placed above the electrode as an H2 collector. (B) SEM image and wettability characterization of the SAL/flat Pt electrode, showing superaerophilicity of the SAL stripe with a bubble contact angle of ~0° and aerophobicity of Pt with a bubble contact angle of 121.4° ± 5.0°. (C) High-magnification SEM image of the SAL stripe, which is composed of numerous SAL SiO2 nanoparticles. (D) Schematic of the SAL/flat Pt electrode with enhanced mass transfer. The H2 bubbles generating on Pt region can be transported to the H2 collector (indicated by yellow arrows) through SAL stripes. (E) First, H2 bubbles are not making contact with the SAL stripe, and the dissolved H2 can diffuse out the reaction system (indicated by green arrows) through gas cushion on the SAL stripe. (F) As they grow, H2 bubbles will contact the SAL stripes and be timely transferred through SAL stripes. (G) In situ optical observation of bubble transfer (indicated by red arrows) on the SAL/flat Pt electrode. First, H2 bubble 1 makes contact with the left SAL stripe (i) and starts to merge into the SAL stripe (ii). Then, the gas channel at the SAL stripe turns to an ON state (iii), whereby the H2 bubble can be transferred into a gas collector (iv). After that, the gas channel turns off (v) and the SAL/flat Pt electrode revives the Pt region to continue HER (vi). With a similar process, H2 bubble 2 is also successfully transferred into the gas collector through the right SAL stripe (iii to vi).
Fig. 1. The SAL/flat Pt electrode with intensified HER through mass transfer enhancement. (A) Optical image of the SAL/flat Pt electrode composed of SAL stripes and Pt. A glass vessel was placed above the electrode as an H2 collector. (B) SEM image and wettability characterization of the SAL/flat Pt electrode, showing superaerophilicity of the SAL stripe with a bubble contact angle of ~0° and aerophobicity of Pt with a bubble contact angle of 121.4° ± 5.0°. (C) High-magnification SEM image of the SAL stripe, which is composed of numerous SAL SiO2 nanoparticles. (D) Schematic of the SAL/flat Pt electrode with enhanced mass transfer. The H2 bubbles generating on Pt region can be transported to the H2 collector (indicated by yellow arrows) through SAL stripes. (E) First, H2 bubbles are not making contact with the SAL stripe, and the dissolved H2 can diffuse out the reaction system (indicated by green arrows) through gas cushion on the SAL stripe. (F) As they grow, H2 bubbles will contact the SAL stripes and be timely transferred through SAL stripes. (G) In situ optical observation of bubble transfer (indicated by red arrows) on the SAL/flat Pt electrode. First, H2 bubble 1 makes contact with the left SAL stripe (i) and starts to merge into the SAL stripe (ii). Then, the gas channel at the SAL stripe turns to an ON state (iii), whereby the H2 bubble can be transferred into a gas collector (iv). After that, the gas channel turns off (v) and the SAL/flat Pt electrode revives the Pt region to continue HER (vi). With a similar process, H2 bubble 2 is also successfully transferred into the gas collector through the right SAL stripe (iii to vi).CC BY-NC · PubMed Central
Fig. 2. Influence of SAL width (SW) and Pt electrode width (EW) on bubble transfer and H2 diffusion. (A) Schematic of the influence of SW on bubble transfer from the Pt electrode to the SAL stripe. (B) Optical images of bubble pinning on the electrode with an SW of 250 μm and bubble transferring on the electrode with an SW of 750 μm (indicated by red dashed circles and red arrows). (C) Statistics of the transfer time of H2 bubbles with different diameters on the SAL stripes with various SWs. On the SAL stripe with an SW of 250 μm, lots of H2 bubbles will spend much time (>50 ms) to transfer or pin on SAL stripes. (D) Schematic of the influence of EW on bubble growing and transferring. (E) Optical images of H2 bubbles on the blank electrode (without SAL stripe) and the SAL/flat Pt electrode with an EW of 500 μm. H2 bubbles cannot be timely removed on the blank electrode, while the SAL/flat Pt electrode is capable of transferring H2 bubble timely (indicated by red dashed circles and red arrows). (F) Variation of the current density of the SAL/flat Pt electrodes with various EWs at an overpotential of −350 mV. (G) Simulation of H2 diffusion on the blank Pt electrode. The maximal H2 concentration at the Pt interface can reach as high as ~0.66 M. (H) Simulation of H2 diffusion on the SAL/flat Pt electrode. The H2 concentration can be lowered to ~0.29 M, showing enhanced H2 diffusion. (I) Simulation of H2 diffusion on the SAL/flat Pt electrodes with various EWs. The SAL/flat Pt electrode with minor EW is favorable for dissolved H2 diffusion.
Fig. 2. Influence of SAL width (SW) and Pt electrode width (EW) on bubble transfer and H2 diffusion. (A) Schematic of the influence of SW on bubble transfer from the Pt electrode to the SAL stripe. (B) Optical images of bubble pinning on the electrode with an SW of 250 μm and bubble transferring on the electrode with an SW of 750 μm (indicated by red dashed circles and red arrows). (C) Statistics of the transfer time of H2 bubbles with different diameters on the SAL stripes with various SWs. On the SAL stripe with an SW of 250 μm, lots of H2 bubbles will spend much time (>50 ms) to transfer or pin on SAL stripes. (D) Schematic of the influence of EW on bubble growing and transferring. (E) Optical images of H2 bubbles on the blank electrode (without SAL stripe) and the SAL/flat Pt electrode with an EW of 500 μm. H2 bubbles cannot be timely removed on the blank electrode, while the SAL/flat Pt electrode is capable of transferring H2 bubble timely (indicated by red dashed circles and red arrows). (F) Variation of the current density of the SAL/flat Pt electrodes with various EWs at an overpotential of −350 mV. (G) Simulation of H2 diffusion on the blank Pt electrode. The maximal H2 concentration at the Pt interface can reach as high as ~0.66 M. (H) Simulation of H2 diffusion on the SAL/flat Pt electrode. The H2 concentration can be lowered to ~0.29 M, showing enhanced H2 diffusion. (I) Simulation of H2 diffusion on the SAL/flat Pt electrodes with various EWs. The SAL/flat Pt electrode with minor EW is favorable for dissolved H2 diffusion.CC BY-NC · PubMed Central
Fig. 3. H2 bubble behaviors and electrochemical tests on the flat Pt electrode, the SAB Pt electrode, the SAL/flat Pt electrode, and the SAL/SAB Pt electrode. (A to D) Optical images and schematics of H2 bubble behaviors on these four electrodes. Serious H2 bubble adhesion can be observed on the flat Pt electrode (A), while H2 bubbles can timely detach from the nanostructured SAB Pt electrode (B). Introducing SAL stripes can facilitate H2 bubble transfer on the SAL/flat Pt electrode (C). SAL stripes, coupled with superaerophobicity of nanostructured Pt, further promote bubble transfer on the SAL/SAB Pt electrode, which can achieve ultrafast bubble transfer in 2 ms (D). (E and F) HER polarization curves (E) and current densities of these four electrodes at −50, −100, −300, and −500 mV versus RHE (F). The SAL/SAB Pt electrode exhibits the best HER performance. (G) Tafel plots of these four electrodes.
Fig. 3. H2 bubble behaviors and electrochemical tests on the flat Pt electrode, the SAB Pt electrode, the SAL/flat Pt electrode, and the SAL/SAB Pt electrode. (A to D) Optical images and schematics of H2 bubble behaviors on these four electrodes. Serious H2 bubble adhesion can be observed on the flat Pt electrode (A), while H2 bubbles can timely detach from the nanostructured SAB Pt electrode (B). Introducing SAL stripes can facilitate H2 bubble transfer on the SAL/flat Pt electrode (C). SAL stripes, coupled with superaerophobicity of nanostructured Pt, further promote bubble transfer on the SAL/SAB Pt electrode, which can achieve ultrafast bubble transfer in 2 ms (D). (E and F) HER polarization curves (E) and current densities of these four electrodes at −50, −100, −300, and −500 mV versus RHE (F). The SAL/SAB Pt electrode exhibits the best HER performance. (G) Tafel plots of these four electrodes.CC BY-NC · PubMed Central
Fig. 4. The Ti-based SAL/SAB cooperative electrode with excellent HER performance. (A) Schematic of the Ti-based SAL/SAB electrode. The SAL stripes and SAB Pt are introduced on the Ti substrate. (B) SEM image of the electrodeposited Pt cluster on the Ti substrate. (C) Bubble transfer on the Ti-based SAL/SAB Pt electrode; H2 bubble can be timely transferred in 2 ms. (D and E) HER polarization curves and current densities at various overpotentials. The Ti-based SAL/SAB Pt electrode exhibits better HER performance than the Ti-based SAB Pt. (F) Tafel plots of the Ti-based SAL/SAB electrode and the Ti-based SAB Pt electrode in 0.5 M H2SO4. (G) Comparison of overpotential at 10 mA cm−2 (red columns, left y axis) and Tafel slope (blue columns, right y axis) for various efficient HER catalysts in 0.5 M H2SO4 solution. Values were plotted from references (table S1) (46–55). (H) HER polarization curves of the Ti-based SAL/SAB electrode in solutions with various H2SO4 concentration, which exhibits the best HER performance in 4 M H2SO4. (I) Comparison of the current densities of the Ti-based SAL/SAB Pt electrode with various 2D materials, single atoms, or Pt-based HER catalysts under different potentials. Values were plotted from references (table S2) (40, 42, 48–50, 59–64). (J) Stability test of the Ti-based SAL/SAB Pt electrode in 4 M H2SO4 at −500 mA cm−2, which exhibits a stable HER performance over 10 hours with ~31 mV potential change.
Fig. 4. The Ti-based SAL/SAB cooperative electrode with excellent HER performance. (A) Schematic of the Ti-based SAL/SAB electrode. The SAL stripes and SAB Pt are introduced on the Ti substrate. (B) SEM image of the electrodeposited Pt cluster on the Ti substrate. (C) Bubble transfer on the Ti-based SAL/SAB Pt electrode; H2 bubble can be timely transferred in 2 ms. (D and E) HER polarization curves and current densities at various overpotentials. The Ti-based SAL/SAB Pt electrode exhibits better HER performance than the Ti-based SAB Pt. (F) Tafel plots of the Ti-based SAL/SAB electrode and the Ti-based SAB Pt electrode in 0.5 M H2SO4. (G) Comparison of overpotential at 10 mA cm−2 (red columns, left y axis) and Tafel slope (blue columns, right y axis) for various efficient HER catalysts in 0.5 M H2SO4 solution. Values were plotted from references (table S1) (46–55). (H) HER polarization curves of the Ti-based SAL/SAB electrode in solutions with various H2SO4 concentration, which exhibits the best HER performance in 4 M H2SO4. (I) Comparison of the current densities of the Ti-based SAL/SAB Pt electrode with various 2D materials, single atoms, or Pt-based HER catalysts under different potentials. Values were plotted from references (table S2) (40, 42, 48–50, 59–64). (J) Stability test of the Ti-based SAL/SAB Pt electrode in 4 M H2SO4 at −500 mA cm−2, which exhibits a stable HER performance over 10 hours with ~31 mV potential change.CC BY-NC · PubMed Central

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Metadata

Authors
Zhang, C., Xu, Z., Han, N., Tian, Y., Kallio, T., Yu, C., & Jiang, L.
Affiliations
  • Chinese Academy of Sciences (CN)
  • Beihang University (CN)
  • Aalto University (FI)
Corresponding author
  • Yu, Cunming
  • Jiang, Lei
ORCID
Venue
Science Advances
Publisher
American Association for the Advancement of Science (AAAS)
Published
2023-01-20
Volume
9
Issue
3
Pages
eadd6978-eadd6978
ISSN
2375-2548 (ISSN-L)
DOI
10.1126/sciadv.add6978
PMC
PMC9848275
OpenAlex
W4317254717
Cited by
230
References
66
Citations by year
2026: 70 · 2025: 66 · 2024: 63 · 2023: 31
FWCI
10.99
Type
journal article
Language
en
Open access
Licence
cc-by-nc
Locations
  • Science Advances (publishedVersion, cc-by-nc)
  • PubMed Central (publishedVersion, cc-by-nc)
  • PubMed (publishedVersion)
  • Aaltodoc (Aalto University) (submittedVersion, cc-by-nc)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Materials Science › Surfaces, Coatings and Films › Surface Modification and Superhydrophobicity
  • Physical Sciences › Chemical Engineering › Filtration and Separation › Minerals Flotation and Separation Techniques
Keywords
hydrogen evolution reaction, superaerophobic surfaces, bubble adhesion, bubble dispersion, Laplace pressure, hydrogen diffusion, mass transfer enhancement, green hydrogen production, electrocatalysis, sulfuric acid electrolyte

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