Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.079
Publication date: 18th July 2023
A multi-scale first-principles reaction-transport model is derived for the electrochemical reduction of CO2 to fuels and chemicals on polycrystalline copper electrodes. The model utilizes a continuous stirred-tank reactor (CSTR) approximation that captures the relative timescales for mesoscale stochastic processes at the electrode/electrolyte interface
that determine product selectivity. The model is built starting from a large experimental dataset obtained under a broad range of well-defined transport regimes in a gastight rotating cylinder electrode cell. Product distributions under different conditions of transport, applied potential, bulk electrolyte concentration, temperature and catalyst porosity are rationalized by introducing dimensionless numbers that reduce complexity and capture relative time scales for mesoscopic and microscopic dynamics of electrocatalytic reactions on copper electrodes of any porosity. This work demonstrates that one CO2 reduction mechanism can explain differences in selectivity reported for copper-based electrocatalysts when mass transport, concentration polarization effects, and primary and secondary current distributions are taken into account. The reaction-transport model presented in this talk should enable the rational design of CO2 electrolyzers.
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