Bottom-up modelling of COF/electrode systems for CO2 reduction in confinement

PN 3 A-9

Project description

This project aims to understand, model and control confinement effects on the electrocatalytic CO2 reduction reaction (CO2RR) in the atomically precise pores of covalent organic frameworks (COFs). We combine COF design, advanced electrochemistry and theoretical modelling in a tight feedback loop to arrive at a fundamental understanding of CO2RR reactivity under confinement. Confinement effects to be studied include (i) CO2 capture and oversolubility in mesopores, (ii) increase of CO2RR vs. hydrogen evolution reaction selectivity via control of the local pH, mass transport and electrochemical double layer, and (iii) selectivity enhancement for multicarbon (C2+) products by tandem catalysis. To this end we employ a data-integrated, bottom-up, modeling approach starting with quantum-chemical calculations on the density functional theory level of the electrode/electrolyte interface. This information will be embedded into semi-classical atomistic simulations that allow to study the electric potential-dependent compositional changes and transport coefficients that ultimately are linked to reaction rates and selectivity. Within the CRC 1333 “Molecular Heterogeneous Catalysis in Confined Geometries” we envision a strong feedback loop with experimental results like differential capacitance and electrochemical impedance spectroscopy for COFs supported on electrode interfaces. Our study of the electrical double layer properties therefore will help choosing backbone design and pore wall functionalization for our project partners involved in synthesis of oriented thin COF films.

Project information

Project title Bottom-up modelling of COF/electrode systems for CO2 reduction in confinement
Project leader Alexander Schlaich
Project staff Henrik Jäger, doctoral researcher
Project website https://www.crc1333.de/research/projects/covalent-organic-frameworks-as-tailored-substrates-with-molecularly-defined-pores-for-molecular-heterogeneous-catalysis/ 
Project duration July 2022 - June 2026
Project number PN 3 A-9

Publications PN 3 A-9

  1. 2023

    1. H. Jäger, A. Schlaich, J. Yang, C. Lian, S. Kondrat, and C. Holm, “A screening of results on the decay length in concentrated electrolytes,” Faraday Discussions, Feb. 2023, doi: 10.1039/d3fd00043e.
    2. M. Hammer, G. Bauer, R. Stierle, J. Groß, and Ø. Wilhelmsen, “Classical density functional theory for interfacial properties of hydrogen, helium, deuterium, neon, and their mixtures,” The Journal of Chemical Physics, vol. 158, no. 10, Art. no. 10, 2023, doi: 10.1063/5.0137226.
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