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Summary
This summary is machine-generated.

This study reveals how coordinating anions in cobalt phosphate electrocatalysts improve the oxygen evolution reaction (OER) by optimizing proton transfer. This work enhances understanding of structure-activity relationships for designing efficient catalysts.

Keywords:
cobalt phosphateelectrocatalysisoxygen evolution reactionproton transfersurface reconstruction

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Rational design of efficient electrocatalysts requires understanding atomic-level structure-activity correlations.
  • The influence of coordination environment on the oxygen evolution reaction (OER) remains unclear.

Purpose of the Study:

  • To investigate the role of coordination engineering in regulating proton transfer for water oxidation.
  • To explore the use of HPO4^2- anions as proton-coupled electron transfer (PCET) induction groups in cobalt-based catalysts.

Main Methods:

  • Theoretical calculations (pH-dependent OER properties, deuterium kinetic isotope effects).
  • Operando electrochemical impedance spectroscopy (EIS) and Raman spectroscopy.
  • Synthesis and characterization of Co3(PO4)2 and CoHPO4 catalysts.

Main Results:

  • CoHPO4 effectively reduces proton hopping energy barriers and modulates high-valent cobalt species formation.
  • The HPO4^2- anion acts as an effective PCET induction group due to its intermediate pKa.
  • Enhanced OER activity was observed for the CoHPO4 catalyst.

Conclusions:

  • Tuning the local coordination environment by incorporating specific anions is a promising strategy to optimize PCET steps and electrocatalytic activity.
  • The findings provide insights into structure-efficiency relationships applicable to both artificial and natural photosynthetic systems.