Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.239
Publication date: 18th July 2023
The electrochemical conversion of CO2 (CO2RR) into value-added chemicals using renewable energy sources is seen as one of the most promising approaches to achieve defossilization of the chemical industry.[1] The main targets are the direct production of multicarbon products such as ethylene and ethanol and the generation of syngas (CO+H2), a feedstock in the Fischer Tropsch process. However, even though the CO2RR process has been extensively investigated for the last 30 years,[2] its industrial application still faces significant challenges. To meet the industrial requirements, many operational parameters must be optimized besides the catalyst material such as the electrode configuration, the reaction microenvironment, and the electrolyzer design.[3] The state-of-the-art CO2RR setups, which consist of gas diffusion electrodes (GDEs) in flow cells and membrane electrode assembly (MEA) electrolyzers, already achieve relevant current densities (≥ 200 mA/cm2) but further research is needed to enhance the GDEs stability during long-term operation.
In this contribution, we present the synthesis of Ni and Cu-based electrocatalysts with high conversion to syngas and multicarbon products, respectively. These materials are synthesized via a single pyrolysis using a benzoxazine monomer (BO) as a precursor,[4] which leads to more active and stable catalyst materials than those produced with just the metal precursor. Besides the catalyst synthesis, we will discuss how the gas diffusion layer, and the hydrophobic/ion conductivity properties of the catalyst layer, strongly influence the GDEs’ stability and suppress the parasitic hydrogen evolution reaction. We show that, upon optimization, the Ni-BO-based GDE exhibits syngas production at -200 mA/cm2 with a minimum stability of 2 h while the Cu-BO-based GDE is able to reach current densities up to -600 mA/cm2 with high selectivity for ethanol and ethylene. The present work provides insight into important parameters that must be considered to fabricate stable GDEs for the conversion of CO2 into valuable products at industrially-relevant current densities.
All the authors acknowledge funding by the BMBF in the framework of the NanomatFutur project “MatGasDif” (03XP0263). V.C. is grateful to IMPRS-SURMAT for a Ph.D. fellowship.
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