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Boosting Interface Dynamics via Axial Coordination Engineering to Enhance Photoelectrochemical Water Splitting

Kunlin Hai1, Shengya Zhang1, Ze Wang1

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Researchers developed a novel cobalt porphyrin (CoPy@I-2-C) interface activator to enhance photoelectrode performance for water splitting. This material improves charge transfer and catalytic activity, leading to higher photocurrents and stability.

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axial coordinationcharge separationcobalt porphyrinimidazole-2-carbaldehydein situ characterizationsurface catalysis

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Efficient photoelectrodes are crucial for water splitting, requiring optimized semiconductor/transition-metal oxyhydroxide/electrolyte (SC/TMOOH/ELC) interfaces.
  • Simultaneously controlling charge separation and catalytic activity across diverse timescales (10-6 to 100 s) presents a significant challenge.

Purpose of the Study:

  • To engineer an active interface that concurrently regulates interfacial charge transfer and surface catalytic reaction dynamics.
  • To develop a novel interface material for enhancing photoanode performance in water splitting applications.

Main Methods:

  • Axial coordination engineering using cobalt porphyrin (CoPy) coordinated with imidazole-2-carbaldehyde (CoPy@I-2-C) as an interfacial layer.
  • Fabrication and characterization of BiVO4/CoPy@I-2-C/FeNiOOH and TiO2/CoPy@I-2-C/FeNiOOH photoanodes.
  • In situ scanning photoelectrochemical microscopy and density functional theory (DFT) calculations.

Main Results:

  • The optimized BiVO4 photoanode achieved a photocurrent density of 6.40 mA/cm2 at 1.23 VRHE with excellent stability.
  • CoPy@I-2-C acted as an 'interface activator', modulating both SC/TMOOH and TMOOH/ELC interfaces.
  • DFT calculations and microscopy confirmed the role of the electron-rich porphyrin ring and shifted d-band center in enhancing performance.
  • The interface engineering strategy demonstrated universality by application to a TiO2-based photoanode.

Conclusions:

  • CoPy@I-2-C effectively regulates interfacial charge transfer and catalytic dynamics, significantly boosting photoanode efficiency and stability.
  • This work provides a new strategy for active interface modulation to construct high-performance photoanodes for solar water splitting.