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Support-Accelerated Proton Transfer for Enhanced Oxygen Evolution Catalysis.

Wenrui Li1, Jianning Lv1, Xianchun Chen1

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Catalyst supports can actively accelerate reactions. Functionalized supports with hydroxyl groups enhance proton transfer in oxygen evolution reactions (OER), significantly boosting catalytic efficiency.

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Area of Science:

  • Electrochemistry and Materials Science

Background:

  • Catalyst supports are traditionally viewed as inert materials for dispersing active species.
  • Engineering catalyst supports to actively participate in reactions, particularly proton transfer, remains an underexplored area.

Purpose of the Study:

  • To demonstrate that catalyst supports can be engineered to actively participate in catalytic reactions.
  • To investigate the role of functionalized supports in accelerating interfacial proton transfer during the oxygen evolution reaction (OER).

Main Methods:

  • Synthesis of iridium oxide (IrO2) clusters on hydroxyl- and methyl-functionalized zirconium phosphate supports (IrO2/OH-ZrP and IrO2/CH3-ZrP).
  • In-situ spectroscopy, electrochemical measurements, and theoretical calculations to elucidate reaction mechanisms.
  • Rotation-dependent OER activity studies and local pH measurements to provide evidence for support-mediated proton transfer.

Main Results:

  • The hydroxyl groups on the IrO2/OH-ZrP support directly participate in OER by lowering the OOH deprotonation barrier, facilitating proton transfer.
  • This leads to a Support-Accelerated Proton Transfer mechanism (SAEM), distinct from the conventional adsorbate evolution mechanism (AEM) observed for IrO2/CH3-ZrP.
  • IrO2/OH-ZrP exhibits a turnover frequency 2.99 times higher than IrO2/CH3-ZrP at 300 mV overpotential.

Conclusions:

  • Catalyst supports can be actively engineered to enhance catalytic performance by facilitating proton transfer.
  • Support engineering is crucial for proton-transfer limited reactions, offering a new paradigm beyond active site optimization.
  • The SAEM mechanism highlights the potential of functionalized supports in advancing electrocatalyst design for OER and other reactions.