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H2O2 Synthesis with Molecular Electrocatalysts Enables Substantial Current Densities in a Flow Cell Using Gas

Phebe H van Langevelde1, Nathalie E G Ligthart2, Pim G J van Duren1

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Molecular catalysts for two-electron oxygen reduction reaction (ORR) to generate hydrogen peroxide (H2O2) were tested in gas diffusion electrodes (GDEs). This configuration significantly enhanced catalytic currents and revealed new selectivity trends compared to rotating disk electrodes (RDEs).

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Copper ComplexesGas Diffusion ElectrodesHomogeneous CatalysisHydrogen PeroxideRotating Ring Disk Electrodes

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Area of Science:

  • Electrochemistry
  • Catalysis
  • Materials Science

Background:

  • Molecular catalysts for the two-electron oxygen reduction reaction (ORR) producing hydrogen peroxide (H2O2) are of significant interest.
  • Previous studies were limited to rotating disk electrode (RDE) setups, hindering evaluation in industrially relevant configurations.
  • Mass transport limitations in RDEs restrict the assessment of true catalytic currents for molecular ORR catalysts.

Purpose of the Study:

  • To evaluate the performance of a copper-based molecular ORR catalyst, Cu-(tmpa), in a gas diffusion electrode (GDE) cell configuration.
  • To identify factors influencing catalytic current and H2O2 generation in a GDE setup.
  • To assess the potential of molecular catalysts in industrially relevant reactor configurations.

Main Methods:

  • Utilized a readily assembled GDE cell to test the Cu-(tmpa) catalyst.
  • Investigated the impact of buffer concentration, catalyst concentration, and GDE composition on catalytic current.
  • Operated the Cu-(tmpa) catalyst in a GDE flow cell for extended periods.

Main Results:

  • Cu-(tmpa) demonstrated sustained H2O2 generation over multiple hours in the GDE flow cell.
  • Achieved a Faradaic efficiency of 50% and a production rate of 0.11 mmol cm⁻² h⁻¹ at -20 mA/cm².
  • GDE configuration increased current density by nearly 10 times compared to RDE, with altered selectivity trends favoring H2O2 at higher currents.

Conclusions:

  • The GDE setup enables a comprehensive assessment of molecular ORR catalyst potential beyond idealized RDE conditions.
  • Cu-(tmpa) shows promise as an H2O2-generating catalyst in a GDE configuration, suitable for practical applications.
  • Well-defined active sites of molecular catalysts can be effectively utilized in emerging H2O2 production technologies.