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Correlations between experiments and simulations for formic acid oxidation.

Alexander Bagger1, Kim D Jensen1, Maryam Rashedi1,2

  • 1University of Copenhagen, Department of Chemistry Universitetsparken 5 2100 Kbh-Ø Denmark alexander@chem.ku.dk.

Chemical Science
|December 12, 2022
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Summary
This summary is machine-generated.

Electrocatalytic formic acid oxidation is key for renewable energy cycles but faces catalyst poisoning. This study reveals that adsorbed hydrogen (*H) leads to carbon monoxide (CO) formation and surface poisoning, hindering efficiency.

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Area of Science:

  • Electrochemistry
  • Catalysis
  • Renewable Energy

Background:

  • Formic acid oxidation and CO2 reduction are crucial for closed carbon-loop systems powered by renewable energy.
  • Formic acid fuel cells are limited by site-blocking species formed during formic acid oxidation.
  • Understanding CO2 reduction mechanisms provides insights into the reverse reaction: formic acid oxidation.

Purpose of the Study:

  • To investigate the mechanism and catalytic limitations of formic acid oxidation.
  • To correlate simulation data with experimental results on various electrocatalysts.
  • To identify the fundamental factors limiting formic acid oxidation efficiency.

Main Methods:

  • Computational simulations on multiple materials.
  • Experimental electrocatalytic oxidation of formic acid.
  • Correlation of binding energetics and reaction pathways.

Main Results:

  • Formate intermediate exhibits similar binding energetics on Pt, Pd, and Ag catalysts.
  • Silver (Ag) was found to be ineffective as a catalyst for this reaction.
  • Adsorbed hydrogen (*H) on catalyst surfaces promotes *CO formation and poisoning via disproportionation.

Conclusions:

  • The binding energetics of formate do not solely determine catalytic activity.
  • *H adsorption is a critical step leading to catalyst poisoning.
  • Identifying these limitations advances the understanding of formic acid oxidation mechanisms for improved fuel cell performance.