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How Buffer Ions Shape Hydrogen Evolution at Non-extreme pH: Operando Insights into Cu-Mo Electrocatalyst Surface

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Adding phosphate anions to a copper-molybdenum oxide catalyst significantly enhances hydrogen evolution reaction (HER) efficiency in non-extreme pH electrolytes. This electrolyte engineering strategy optimizes ion interactions for cost-effective water electrolysis.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Non-extreme pH conditions are desirable for cost-effective water electrolysis using abundant elements.
  • Electrolyte engineering, particularly buffer ion selection and concentration, is critical for high-efficiency water electrolysis.
  • The hydrogen evolution reaction (HER) in carbonate electrolytes at pH 10.5 relies on bicarbonate anions (HCO3-).

Purpose of the Study:

  • To investigate the effect of phosphate anions on the HER efficiency of a copper-molybdenum oxide (MoOx(Cu)) electrocatalyst in a carbonate electrolyte.
  • To elucidate the mechanism by which phosphate anions enhance HER performance.
  • To provide insights into electrolyte engineering for improved electrochemical reactions.

Main Methods:

  • Electrochemical tests (HER measurements) on MoOx(Cu) electrocatalyst in K-carbonate electrolyte with various anion additives.
  • Electrochemical impedance spectroscopy to study double-layer capacitance.
  • Operando Raman, infrared (IR), and X-ray absorption spectroscopies to analyze surface species.
  • Density functional theory (DFT) calculations to model interfacial interactions.

Main Results:

  • Phosphate anions uniquely reduced HER overpotentials on MoOx(Cu) from low current densities to -1 A cm-2.
  • HER enhancement was observed with phosphate but not with borate or sulfate anions.
  • Phosphate addition increased double-layer capacitance and was linked to Cu-phosphate interactions and surface reconstruction.
  • Spectroscopic and DFT studies confirmed phosphate adsorption on the MoOx(Cu) surface, facilitating cation and HCO3- attraction for enhanced HER.

Conclusions:

  • Phosphate anions are crucial for enhancing HER efficiency in carbonate electrolytes with MoOx(Cu) catalysts.
  • Interfacial cation-anion organization, driven by phosphate adsorption, significantly influences HER performance.
  • This study offers valuable insights into electrolyte engineering for optimizing electrochemical reactions involving ionic reactants.