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Accelerated interfacial proton transfer for promoting electrocatalytic activity.

Kai-Chao Deng1, Zhi-Xuan Lu1, Juan-Juan Sun1

  • 1State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University Xiamen 361005 China bren@xmu.edu.cn sartimm@outlook.com.

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Researchers developed a new method to control interfacial pH for enhanced electrocatalysis. By using 4-mercaptopyridine (4MPy) molecules, they improved proton transfer, doubling the activity for formic acid oxidation reactions.

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Area of Science:

  • Electrochemistry
  • Surface Science
  • Catalysis

Background:

  • Interfacial pH is crucial for proton-coupled electron transfer (PCET) electrocatalytic reactions.
  • Slow proton transfer at interfaces leads to pH variations, hindering optimal catalyst activity.

Purpose of the Study:

  • To develop a general strategy for regulating interfacial pH to enhance electrocatalytic activity.
  • To investigate the role of proton transfer promotion in maintaining optimal interfacial pH.

Main Methods:

  • Adsorption of bifunctional 4-mercaptopyridine (4MPy) molecules onto catalyst surfaces.
  • Utilizing the pyridyl group of 4MPy as a proton acceptor/donor.
  • Employing *in situ* electrochemical surface-enhanced Raman spectroscopy (EC-SERS) for quantitative analysis.

Main Results:

  • 4MPy effectively promoted proton transfer at the Pt catalyst interface.
  • Interfacial proton transfer remained thermoneutral during formic acid oxidation reaction (FAOR) at high current densities.
  • The Pt@4MPy catalyst exhibited twice the apparent current density compared to pristine Pt for FAOR.

Conclusions:

  • Promoting interfacial proton transfer is a viable strategy for effective interfacial pH regulation.
  • The 4MPy-modified catalyst offers enhanced electrocatalytic activity for FAOR.
  • This work presents a general approach to improve electrocatalytic performance by controlling interfacial pH.