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Geometric Catalyst Utilization in Zero-Gap CO2Electrolyzers

Journal Article (2022)
Author(s)

Siddhartha Subramanian (TU Delft - ChemE/Materials for Energy Conversion and Storage)

Kailun Yang (TU Delft - ChemE/Materials for Energy Conversion and Storage)

Mengran Li (TU Delft - ChemE/Materials for Energy Conversion and Storage)

M. Sassenburg (TU Delft - ChemE/Materials for Energy Conversion and Storage)

M. Abdinejad (TU Delft - ChemE/Materials for Energy Conversion and Storage)

I.E. Irtem (TU Delft - ChemE/Materials for Energy Conversion and Storage)

J. Middelkoop (TU Delft - ChemE/O&O groep)

Thomas Burdyny (TU Delft - ChemE/Materials for Energy Conversion and Storage)

Research Group
ChemE/Materials for Energy Conversion and Storage
Copyright
© 2022 S.S. Subramanian, K. Yang, Mengran Li, M. Sassenburg, M. Abdinejad, I.E. Irtem, J. Middelkoop, T.E. Burdyny
DOI related publication
https://doi.org/10.1021/acsenergylett.2c02194
More Info
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Publication Year
2022
Language
English
Copyright
© 2022 S.S. Subramanian, K. Yang, Mengran Li, M. Sassenburg, M. Abdinejad, I.E. Irtem, J. Middelkoop, T.E. Burdyny
Research Group
ChemE/Materials for Energy Conversion and Storage
Issue number
1
Volume number
8
Pages (from-to)
222-229
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Abstract

The electrochemical reduction of CO2 (CO2RR) on silver catalysts has been demonstrated under elevated current density, longer reaction times, and intermittent operation. Maintaining performance requires that CO2 can access the entire geometric catalyst area, thus maximizing catalyst utilization. Here we probe the time-dependent factors impacting geometric catalyst utilization for CO2RR in a zero-gap membrane electrode assembly. We use three flow fields (serpentine, parallel, and interdigitated) as tools to disambiguate cell behavior. Cathode pressure drop is found to play the most critical role in maintaining catalyst utilization at all time scales by encouraging in-plane CO2 transport throughout the gas-diffusion layer (GDL) and around salt and water blockages. The serpentine flow channel with the highest pressure drop is then the most failure-resistant, achieving a CO partial current density of 205 mA/cm2 at 2.76 V. These findings are confirmed through selectivity measurements over time, double-layer capacitance measurements to estimate GDL flooding, and transport modeling of the spatial CO2 concentration.