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

Nesbitt, Nathan T.; Burdyny, Thomas; Simonson, Hunter; Salvatore, Danielle; Bohra, Divya; Kas, Recep; Smith, Wilson A.

doi:10.1021/acscatal.0c03319

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

Journal Article · Wed Nov 18 00:00:00 EST 2020 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.0c03319· OSTI ID:1755734

^[1]; ^[2]; Simonson, Hunter ^[3]; ^[3]; ^[2]; Kas, Recep ^[1]; ^[4]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
Delft Univ. of Technology (Netherlands)
Univ. of Colorado, Boulder, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Delft Univ. of Technology (Netherlands); Univ. of Colorado, Boulder, CO (United States)

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. In this paper 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.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: The Dutch Research Council (NWO); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1755734

Report Number(s):: NREL/JA--5900-77219; MainId:26165; UUID:cb9df62a-2b11-4b34-b3c2-9c529631dcfa; MainAdminID:19062

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 23 Vol. 10; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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