The computation of pK a (and redox potentials) in aqueous solution within the context of density functional theory-based molecular dynamics (DFTMD) has been worked out previously by Cheng, Sprik, and co-workers using the proton insertion method. It involves the calculations of the deprotonation free energy of hydrated hydronium ions (proton) ∆ dp A H 3 O + and that of hydrated water molecule ∆ dp A H 2 O calculated from the free energy perturbation theory. For the computational details, including system setup and free energy calculation method, the reader is referred to the Supporting Information. These DFTMD simulations with the BLYP functional were carried out with CP2K code in LiCl solutions of concentrations from 0.0 to 9.3 m (molality).