Ab-initio calculations of the double layer suffer from several limitations that lead to unfeasible computational costs which can be circumvented in the continuum treatment of the double layer . In addition, the results derived using a continuum ap-proach such as the GMPNP can provide valuable inputs to atomistic quantum mechanical models by defining the steady-state environment under which reaction energetics need to be studied . However, the continuum treatment of the electrolyte system does not capture effects pertaining to ion specificity which can potentially play a role at molecular length scales and concentrations relevant in the EDL for highly charged surfaces such as in the case of CO 2 ER . The Bjerrum length (l B = e 2 /4πε r ε 0 k B T , 0.7 nm at room temperature) defines the length scale at which the electrostatic interaction between two charged species is comparable to the thermal energy k B T . The relative permittivity of the electrolyte can decrease drastically in the EDL where the electric field strength is high (Figure ) . This will lead to an increase in the Bjerrum length indicating a prevalence of ionspecific effects. There is therefore a need to develop computational frameworks applicable to practical electrocatalytic systems with high surface charge densities that correct the mean-field continuum dynamics of the double-layer for electrostatic correlations.