Elucidating the Best-Fit Tandem Approach for the Upscaled Electroconversion of CO2 to C2H4
VSRK Tandava a, Andrés Alberto García a, Martí Biset-Peiró a, Joan Ramón Morante a, Sebastián Murcia-López a
a Catalonia Institute for Energy Research (IREC), Sant Adrià de Besos, 08930, Barcelona, Spain.
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
#MatInter - Materials and Interfaces for emerging electrocatalytic reactions
Barcelona, Spain, 2024 March 4th - 8th
Organizers: Marta Costa Figueiredo and María Escudero-Escribano
Poster, VSRK Tandava, 496
Publication date: 18th December 2023

Anthropogenic carbon cycle closure is aimed at achieving a tangible reality with the successful implementation of electrochemical CO2 reduction powered by renewable electricity. Despite significant progress in obtaining carbon products, such as CO and Formate, multi-carbon products have been a distant reality in reaching the potential industrial scale. Practical limitations, such as poor selectivity for multi-carbon products in compliance with sluggish kinetics lead to electrocatalysts suffering from high overpotentials while directly converting CO2 to C2+ products. Over the years, mimicking cascade catalytic processes with multiple reaction intermediates has been a dream of the research community inspired by nature. Several attempts have been made to mimic nature’s cascade processes in electrochemical CO2 reduction as an alternative route to modulate product generation from CO2 to CO and further reduce CO to C2+ products resembling a tandem approach. Considerable tandem approaches have been extensively investigated for multiple reaction steps involving tandem electrocatalysts to tandem devices. While most of these yield a noteworthy multi-carbon product formation, the product distribution varies in the range of products such as ethylene, ethanol, and propanol, including acetates. Therefore, it is highly important to investigate the most suitable approach for steering the major selectivity towards a single multi-carbon product. Herein, we have carried out a systematic approach to elucidate the best-fit tandem approach starting from tandem electrocatalysts and tandem electrodes, followed by tandem devices. To understand the product selectivity, we chose to operate with a Ni-N-C single-atom catalyst and CuxO-C-based cathodic materials. Initial investigations began with tandem electrocatalysts with Ni-N-C and CuxO-C with varying compositions in the ink formulations and deposited on the gas diffusion layers. A wide range of product distributions were observed with C2H4 being the dominant product. We further executed the tandem electrode design with layer-by-layer deposition of the catalysts followed by a segmented electrode which further enhanced the selectivity towards C2H4. Finally, we incorporated a tandem device in which CO2 is converted to CO in the first cell and CO is sequentially converted to multi-carbon products in the second. When the unreacted CO2 is trapped using an absorption chamber between these two electrolyzers, an exponential surge in the faradaic efficiency towards C2H4 (˃ 70%) thus accounting for more than 85 ± 2% towards multi-carbon product faradaic efficiency at an average current density of -150 mA·cm-2. This approach was found to be highly efficient not only in terms of faradaic efficiency but also energetically thus aiding the cascade approach with a tandem device setup reaching the potential industrial scale.

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