Model Systems were constructed as follows. The anode was modelled using a crystal of AB-stacked graphite, with layers lying in the xz plane and the surface in the xy plane at z = 0. A unit cell with (A, B, C) dimensions lying along the (x, y, z) axes respectively was created, containing the anode crystal and a vacuum region adjacent to it, extending along the C-dimension of the cell. The vacuum region was packed with a liquid electrolyte solution to a target density of 1.32 g cm -3 using Materials Studio Amorphous Cell. The electrolyte was comprised of ethylene carbonate (EC) solvent molecules and lithium hexafluorophosphate (Li + / PF - 6 ) ion pairs to a concentration of ∼ 1.0 mol dm -3 at which Li-ion conductivity in EC-based electrolyte is close to its maximum. Geometry optimization and NVT-MD equilibration of the cell was performed using Materials Studio Forcite. Finally, the trivalent carbon atoms on the surface of the anode (at z = 0) were each assigned a charge so that the total surface charge per unit cell was -2 e, in order to create a potential difference of 2 V between anode and electrolyte. The anode acts as a steric barrier between the electrolyte and its periodic images in the Cdirection, as well as a charged surface adjacent to which a reduction zone is defined. The anode was constrained at all points in construction and MC-MD simulations. Construction of model systems was repeated to generate configurationally distinct starting cells.