A Multiscale Model of Electrochemical Double Layers in Energy Conversion and Storage Devices

In this paper we report a statistical-mechanics-based continuum theory allowing tackling the simulation of electrochemical double layers under non-equilibrium conditions at electrolyte/electrode interfaces relevant to electrochemical cells for energy conversion and storage. The present theory is designed to capture the impact onto the overall electrode behavior of the electrolyte composition in terms of solvent, charged polymers and ions concentration, for a large diversity of cases, from diluted solutions to ionic liquids. From its continuum character, the theory is particularly useful for the simulation of interfacial electrochemical mechanisms within multiscale frameworks scaling up atomistic and molecular level properties onto overall performance cell models. Results obtained with our home-made MS LIBER-T simulation package are presented and discussed within the context of fuel cells and lithium ion batteries.