A research team led by Prof. Nuria Lopez from ICIQ and Prof. Sophia Haussener from EPFL has developed a novel ab-initio multiscale methodology for electrochemical CO2 reduction (e-CO2R). By combining the atomic-scale kinetics with the transport effects, the team has identified optimal electrolyte conditions that enhance the selectivities of e-CO2R products.
e-CO2R is a promising technology to convert harmful greenhouse gases into valuable chemicals and fuels using renewable electricity. While catalyst materials have been widely studied, the surrounding electrolyte environment also strongly influences the reactivity and faradaic efficiencies. Despite advances in the computational catalyst design through scaling relations and volcano plots, the rational design of electrolyte microenvironments remained scarcely investigated.
The team filled this gap by coupling ab-initio microkinetic modeling with continuum-scale transport simulations, explicitly considering electrolyte effects across all relevant length scales. For liquid electrolytes, the results revealed an inverse relationship between cation concentration and CO2 availability at the catalyst interface. This led to a “volcano” type relation between current densities and the number of microenvironments at the electrode/electrolyte interface. Extending the methodology to realistic membrane/electrode configurations, the researchers showed that while ionomers can overcome this limitation through fixed background charge concentrations, water management becomes critical to achieve high current densities.
These findings were recently published in the journal Nature Catalysis, marking an important step towards rational design of electrolytes.
Prof. Lopez said “This is a long-term and fantastic collaboration between two computational groups to model the electrochemical interfaces. All the information usually hard to obtain through experimental characterization is now unlocked through the ab-initio multiscale model.”
Prof. Haussener said “Multiscale modelling is essential to capture the complex interactions at the electrode/electrolyte interfaces and guide the design of efficient eCO2R systems. Our innovative approach stems from combining expertise across fields in interdisciplinary teams.”
Looking ahead, the researchers plan to extend their methodologies to model gas-diffusion electrolyzers and zero-gap membrane electrode assembly configurations, which are essential for optimizing industrial-scale electrolyzers. This work has broad implications for the development of predictive digital twin technologies, not only for e-CO2R but also for other electrochemical processes such as electrosynthesis of organic compounds.
Reference publication
Microenvironment effects in electrochemical CO2 reduction from first-principles multiscale modelling
Lorenzutti, F.; Seemakurthi, R. R.; Johnson, E. F.; Morandi, S.; Nikačević, P.; López, N.; Haussener, S.
Nat. Catal. 2025
DOI: 10.1038/s41929-025-01399-2
La entrada Modelling electrolyte effects in CO₂ reduction se publicó primero en ICIQ.