All the DFT calculations were performed by using the Vienna Ab-initio Simulation Package (VASP). The projector augmented wave (PAW) pseudopotential was used to describe the effect of core electrons. The exchange-correlation of valence electrons is described by using Perdue-Burke-Ernzerhof (PBE) functional , while density-dependent energy correction (dDsC) was used to describe dispersion. Interatomic distances for Cu, Pd, and Ag are 2.56, 2.78, and 2.92 Å, respectively. The Brillouin zone was sampled using 4×4×1 or 6×6×1 Γ-centered Monkhorst-Pack mesh for 4×4 (111) slabs calculations. Geometries were optimized with Γcentered 441 k-points, followed by single-point calculations with Γ-centered 661 k-points. VASPsol was used for the implicit solvation calculations. The effective surface tension is set to 0 for numerical stability. For the potential-dependent adsorption energy calculations, the electrode potential on the SHE scale was computed from the calculated work function by subtracting 4.44 eV, adding/removing electrons as required during adsorption to maintain the desired potential. Overall charge neutrality is maintained via the electrolyte distribution through the linearized Poisson-Boltzmann equation. All thermodynamic integration calculations were performed by using the FIST module in CP2K. More extended systems, 86 (111) facets with 200 water molecules with a vacuum layer of longer than 20 Å, were used for the MM calculations. Molecular dynamics were run in the NVT ensemble at 300 K, using the Nose-Hoover thermostat. Lennard-Jones parameters and atomic charge for benzaldehyde are obtained from OPLS-AA, generated using LigParGen. The TIP3P force field was used for describing water molecules. Refer to the Supporting Information for complete details.