Dynamic calculations for HER and CO2RR. Ab initio molecular dynamics (AIMD) simulations were conducted using the Nose-Hoover thermostat in the canonical (NVT) ensemble at 300 K with a time step of 1 fs. Thermodynamic integrations and the "slow-growth" method were employed to derive the free energy profiles for the ratedetermining steps in HER and CO2RR. The collective variable (CV) increment was set to 0.0008 Å, and the simulation time was 3 ps. Reaction barriers and reaction energies were determined by integrating the free-energy gradients to generate the free energy profiles.