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Room temperature ionic liquids are attractive to numerous applications andparticularly, to renewable energy devices. As solvent free electrolytes, theydemonstrate a paramount connection between the material morphology andCoulombic interactions: unlike dilute electrolytes, the electrode/RTILinterface is a product of both electrode polarization and spatiotemporal bulkproperties. Yet, theoretical studies have dealt almost exclusively withindependent models of morphology and electrokinetics. In this work, we developa novel Cahn-Hilliard-Poisson type mean-field framework that couplesmorphological evolution with electrokinetic phenomena. Linear analysis of themodel shows that spatially periodic patterns form via a finite wavenumberinstability, a property that cannot arise in the currently usedFermi-Poisson-Nernst-Planck equations. Numerical simulations in above one-spacedimension, demonstrate that while labyrinthine type patterns develop in thebulk, stripe patterns emerge near charged surfaces. The results qualitativelyagree with empirical observations and thus, provide a physically consistentmethodology to incorporate phase separation properties into an electrochemicalframework.

Theory of phase separation and polarization for dissociated ionic liquids