Interfacial Adsorbate Competition Regulates Intermediate Stabilization and Onset Potential in Acidic CO2 Electroreduction
Adrián Pinilla-Sánchez, Suraj Panja, Bárbara Polesso, Prathama Haldar, Ranit Ram, Ranga Rohit Seemakurthi, Anku Guha, Núria López, F. Pelayo García de Arquer
TL;DR
This study explores how anions affect CO2 reduction in acidic conditions, showing that sulfate adsorption hinders the process while hydroxyl helps stabilize key reaction steps.
Contribution
The paper introduces a novel understanding of anion effects on CO2R selectivity and performance in acidic environments using in situ spectroscopy and simulations.
Findings
Sulfate adsorption inhibits CO2R at low pH and delays intermediate formation.
Hydroxyl coadsorption enables *CO stabilization and supports multicarbon product formation.
Anion interactions significantly influence CO2R selectivity and overpotentials.
Abstract
Electrochemical CO2 reduction (CO2R) in acid may enable high carbon utilization but faces selectivity challenges, particularly from the Hydrogen Evolution Reaction (HER). While the source of protons and cation concentrations play a role in this balance, the role of anions remains underexplored. Here, we combine in situ surface-enhanced Raman Spectroscopy during CO2R in acid with theoretical simulations to investigate the role of anionic species over copper gas diffusion electrodes at application-relevant current densities (up to 0.2 A·cm–2) and performance. Our observations reveal that sulfate adsorption inhibits CO2R at low pH and delays CO2R intermediate formation, which is enabled by hydroxyl species coadsorption. Such competition regulates *CO stabilization and the balanced *CO coverage needed to favor the formation of multicarbon products. These results shed light on how anion…
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Taxonomy
TopicsCO2 Reduction Techniques and Catalysts · Electrocatalysts for Energy Conversion · Chemical Looping and Thermochemical Processes