where G[X (aq)] represents the potential-dependent grand potential energy including vibrational corrections as described in the Supplementary Material. All energies were calculated using implicit solvation with potential control using the VASPsol code, with additional details included in the Supplementary Material. We note that the absolute values of chemical potential of the complex μCu and E f [VCu] are modulated by details of the DFT calculations (e.g., the exchange correlation functional) and the degree of solvation in the models (for instance, secondary solvation shell inclusion, etc.), and therefore the computational results primarily serve to provide quantitative insight and qualitative trends. The present study focuses on thermodynamic trends in comparison with experimental observations, but does not account for possible kinetic effects.