The transport behavior of CO2 in the ionic liquids (ILs)-electrode interface is revealed via the joint molecular dynamics simulation and thermodynamic analysis method. Combining the hopping mechanism within the interfacial region and the self-diffusive behavior in bulk, a hopping-diffusion model is developed to evaluate the transport performance of CO2. The effective transport efficiency of CO2 transporting across interfacial ILs could be predicted based on the hopping-diffusion model, showing the faster transport feature of CO2 in [Emim][BF4]. Meanwhile, the enhanced antisymmetric stretching mode and entropy decrease of CO2 in various ILs interface are identified, demonstrating [Emm245im][BF4] possesses the biggest thermodynamic advantage in terms of reducing the entropy cost. As both fast mass transport and small entropy cost can enhance the performance of ILs, the detailed correlation between the transport process and thermodynamic information would help to clarify the molecular mechanism of ILs/CO2-electrode interface in the specific electrochemical applications.

Molecular insight into the mass transport mechanism of CO2 in the interfacial ionic liquids

ACS Spring Meeting 2021

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