The first step is exchange of surface Li with H, and the second step is removing an H, O, and metal (M ) from the (001) surface. We assume that the removal of any M -OH species results in a delocalization of electrons, since operation of Li-ion batteries relies upon the oxidation/reduction response of redox active M in the cathode. To compute the change in free energy associated with metal release, ∆G tot , a DFT + solvent ion method based on Hess's Law is employed. In the DFT + solvent ion method, ∆G tot is partitioned between the computed energies of the reactants and products (used in ∆G 1 ) and experimental data (used in ∆G 2 ). Zero-point energy (ZPE) correction terms are added to the DFT total energies of NMC slabs to obtain ∆G 1 = E products -E reactants + ZPE, as described in Ref. and in the style on Ref. Based on the previous work, we assume that the minimum energy pathway of release involves removal of an M -OH unit. The total energies of M , O, and H released from the surface are for the atoms in their standard state, which implies that ∆G 1 can be used as a term that gauges relative lattice stability for the removal of an isolated M -OH unit per surface slab.