Liquid-Solid Boundaries Dominate Activity of CO2 Reduction on Gas-Diffusion Electrodes

Nathan Nesbitt, Thomas Burdyny, Hunter Simonson, Danielle Salvatore, Divya Bohra, Recep Kas, Wilson Smith

Research output: Contribution to journalArticlepeer-review

124 Scopus Citations


Electrochemical CO2 electrolysis to produce hydrocarbon fuels or material feedstocks offers a renewable alternative to fossilized carbon sources. Gas-diffusion electrodes (GDEs), composed of solid electrocatalysts on porous supports positioned near the interface of a conducting electrolyte and CO2 gas, have been able to demonstrate the substantial current densities needed for future commercialization. These higher reaction rates have often been ascribed to the presence of a three-phase interface, where solid, liquid, and gas provide electrons, water, and CO2, respectively. Conversely, mechanistic work on electrochemical reactions implicates a fully two-phase reaction interface, where gas molecules reach the electrocatalyst's surface by dissolution and diffusion through the electrolyte. Because the discrepancy between an atomistic three-phase versus two-phase reaction has substantial implications for the design of catalysts, gas-diffusion layers, and cell architectures, the nuances of nomenclatures and governing phenomena surrounding the three-phase-region require clarification. Here we outline the macro, micro, and atomistic phenomena occurring within a gas-diffusion electrode to provide a focused discussion on the architecture of the often-discussed three-phase region for CO2 electrolysis. From this information, we comment on the outlook for the broader CO2 electroreduction GDE cell architecture.

Original languageAmerican English
Pages (from-to)14093-14106
Number of pages14
JournalACS Catalysis
Issue number23
StatePublished - 4 Dec 2020

Bibliographical note

Publisher Copyright:

NREL Publication Number

  • NREL/JA-5900-77219


  • COelectrolysis
  • COreduction
  • double-phase boundary
  • gas-diffusion electrode
  • triple-phase boundary


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