Crossing the dark forest of CO2 electrolysis with molecular electrocatalysts: Which route to take?
Kevinjeorjios Pellumbi a, Kai junge Puring a, Ulf-Peter Apfel a b
a Fraunhofer Institute for Environmelal, Safety, and Energy Technology UMSICHT, Germany
b Ruhr University Bochum, Technical Electrochemistry
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
CO2 electrocatalysis for sustainable fuels and chemicals - #CATSUS
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Carlota Bozal-Ginesta and Alessandro Senocrate
Oral, Kevinjeorjios Pellumbi, presentation 390
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.390
Publication date: 16th December 2024

The electrochemical conversion of CO2 has in recent years emerged as a promising technology towards allowing the conversion of CO2 emissions to valuable chemicals and synthons. In recent years, molecular electrocatalysts have risen to the foreground as a tunable, more mass active and selective alternative to transition metal electrocatalysts. Despite the impressive results reached in recent years for a multitude of systems, transferring molecular systems to the large-scale is not yet a smooth endeavor.
Herein, we present our recent efforts towards a holistic transfer of molecular based assemblies, based on the Ag-BIAN (BIAN: N,N′-bis(arylimino)acenaphthene) structure in industrially relevant CO2 electrolyzers operating at elevated current densities ≥ 300 mA cm-2 at 60°C. Notably, we show how the performance and long-term stability of gas diffusion electrodes coated with Ag-BIANs is not only affected by the nature of the ligand system but also the operation conditions. Together with the performance of ex-situ and operando characterization, we show how ink compositions can play a crucial role in unlocking the activity and stability of previously though inactive complexes under electrolytic conditions at 600 mA cm-2.

Furthermore, the currently running and future scale-up projects of Fraunhofer UMSICHT will be presented opening the discussion on the possible up-scaling of molecular systems.

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