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CO residence time modulates multi-carbon formation rates in a zero-gap Cu based CO2 electrolyzer

Journal Article (2024)
Author(s)

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

J.J. Kok (TU Delft - ChemE/Materials for Energy Conversion and Storage)

P.V. Gholkar (TU Delft - ChemE/Catalysis Engineering)

A. Sajeev Kumar (TU Delft - Large Scale Energy Storage)

H. P. Iglesias van Montfort (TU Delft - ChemE/Materials for Energy Conversion and Storage)

Ruud Kortlever (TU Delft - Large Scale Energy Storage)

Atsushi Urakawa (TU Delft - ChemE/Catalysis Engineering)

Bernard Dam (TU Delft - ChemE/Materials for Energy Conversion and Storage)

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

Research Group
ChemE/Materials for Energy Conversion and Storage
DOI related publication
https://doi.org/10.1039/d4ee02004a
More Info
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Publication Year
2024
Language
English
Research Group
ChemE/Materials for Energy Conversion and Storage
Issue number
18
Volume number
17
Pages (from-to)
6728-6738
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Abstract

Carbon dioxide (CO2) electrolysis on copper (Cu) catalysts has attracted interest due to its direct production of C2+ feedstocks. Using the knowledge that CO2 reduction on copper is primarily a tandem reaction of CO2 to CO and CO to C2+ products, we show that modulating CO concentrations within the liquid catalyst layer allows for a C2+ selectivity of >80% at 200 mA cm−2 under broad conversion conditions. The importance of CO pooling is demonstrated through residence time distribution curves, varying flow fields (serpentine/parallel/interdigitated), and flow rates. While serpentine flow fields require high conversions to limit CO selectivity and maximize C2+ selectivity, the longer CO residence times of parallel flow fields achieve similar selectivity over broad flow rates. Critically, we show that parts of the catalyst area predominantly reduce CO instead of CO2 as supported by CO reduction experiments, transport modelling, and achieving a CO2 utilization efficiency greater than the theoretical limit of 25% for C2+ products.