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Capacitive deionization (CDI) is a fast-emerging technology most commonlyapplied to brackish water desalination. In CDI, salt ions are removed from thefeedwater and stored in electric double layers (EDLs) within micropores ofelectrically charged porous carbon electrodes. Recent experiments havedemonstrated that CDI electrodes exhibit selective ion removal based on ionsize, with the smaller ion being preferentially removed in the case ofequal-valence ions. However, state-of-the-art CDI theory does not capture thisobserved selectivity, as it assumes volume-less point ions in the microporeEDLs. We here present a theory which includes multiple couterionic species, andrelaxes the point ion assumption by incorporating ion volume exclusioninteractions into a description of the micropore EDLs. The developed model is acoupled set of nonlinear algebraic equations which can be solved for microporeion concentrations and electrode Donnan potential at cell equilibrium. Wedemonstrate that this model captures key features of the experimentallyobserved size-based ion selectivity of CDI electrodes.

Size-based ion selectivity of micropore electric double layers in capacitive deionization electrodes