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Highly concentrated electrolytes enhance carbon monoxide (CO) electroreduction to ethylene (C2H4). Tuning interfacial water structure boosts CO conversion into valuable multi-carbon products, aiding climate change mitigation.

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Area of Science:

  • Electrochemistry
  • Catalysis
  • Materials Science

Background:

  • Growing interest in converting carbon dioxide (CO2) and carbon monoxide (CO) into multi-carbon products for climate change mitigation.
  • Challenges in directing selectivity due to competing reaction pathways in CO electroreduction.

Purpose of the Study:

  • To investigate the effect of interfacial water structure on CO electroreduction selectivity.
  • To enhance the production of ethylene (C2H4) and other multi-carbon products from CO.

Main Methods:

  • Electrochemical reduction of CO in highly concentrated sodium perchlorate (NaClO4) electrolytes.
  • Tuning electrolyte concentration (0.01 to 10 molal) to modify interfacial water structure.
  • Temperature-dependent studies and surface-enhanced Raman spectroscopy (SERS) to analyze reaction mechanisms.

Main Results:

  • A 18-fold increase in CO reduction rate with increasing NaClO4 concentration.
  • Achieved 91% Faradaic efficiency for multi-carbon products at -1.43 V vs. the normal hydrogen electrode.
  • Disordered interfacial water layers, characterized by disrupted hydrogen bonding, correlate with enhanced CO to C2H4 reduction.

Conclusions:

  • Manipulating interfacial water structure through high ionic strength electrolytes is a viable strategy to enhance CO electroreduction.
  • Disruption of hydrogen bonding in interfacial water facilitates the selective formation of C2H4.
  • Findings provide insights for designing catalysts and electrolytes for efficient CO conversion into valuable chemicals.