Along the Channel Gradients Impact on the Spatioactivity of Gas Diffusion Electrodes at High Conversions during CO2 Electroreduction

Kas, Recep; Star, Andrew G.; Yang, Kailun; Van Cleve, Tim; Neyerlin, Kenneth C.; Smith, Wilson A.

doi:10.1021/acssuschemeng.0c07694

Along the Channel Gradients Impact on the Spatioactivity of Gas Diffusion Electrodes at High Conversions during CO₂ Electroreduction

Journal Article · Thu Jan 14 00:00:00 EST 2021 · ACS Sustainable Chemistry & Engineering

DOI:https://doi.org/10.1021/acssuschemeng.0c07694· OSTI ID:1764930

^[1]; Star, Andrew G. ^[2]; Yang, Kailun ^[3]; ^[2]; ^[2]; ^[4]

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

Results of a 2-D transport model for a gas diffusion electrode performing CO₂ reduction to CO with a flowing catholyte are presented, including the concentration gradients along the flow cell, spatial distribution of the current density and local pH in the catalyst layer. The model predicts that both the concentration of CO₂ and the buffer electrolyte gradually diminish along the channels for a parallel flow of gas and electrolyte as a result of electrochemical conversion and nonelectrochemical consumption. At high single-pass conversions, significant concentration gradients exist along the flow channels leading to large local variations in the current density (>150 mA/cm²), which becomes prominent when compared to ohmic losses. In addition, concentration overpotentials change dramatically with CO₂ flow rate, which results in significant differences in outlet concentrations at high conversions. The outlet concentration of CO attains a maximum of 80% along with 5% CO₂ and 15% H₂, although the maximum single-pass conversion is limited to below 60% due to homogeneous consumption by the electrolyte. Fundamental and practical implications of our findings on electrochemical CO₂ reduction are discussed with a focus on the trade-off between high current density operation and high single-pass conversion efficiency.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1764930

Report Number(s):: NREL/JA--5900-78079; MainId:31988; UUID:7a56bf80-7e9c-4463-b0dc-b77dfdf235be; MainAdminID:19281

Journal Information:: ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 3 Vol. 9; ISSN 2168-0485

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Along the Channel Gradients Impact on the Spatioactivity of Gas Diffusion Electrodes at High Conversions during CO2 Electroreduction

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Along the Channel Gradients Impact on the Spatioactivity of Gas Diffusion Electrodes at High Conversions during CO₂ Electroreduction