Here, n p is the number of equivalent diffusion paths, l is the jump length, and ν 0 is the attempt/jump frequency of the adsorbate that is related to their vibrational free energies. Results and Discussion The computational efficiency of the above MLP development protocol depends on the sampling strategy used to select configurations for DFT/SPE calculations. In this work, we employ a wider sampling range compared to previous studies. Specifically, we use 0.2 eV/ Å and 0.7 eV/ Å as the lower and upper ϵ t bounds for sampling, respectively. Within these bounds, configurations from the MD trajectory are randomly sampled to obtain a maximum of 100 possible configurations for each adsorbate. If fewer than 100 configurations lie within the chosen ϵ t bounds, then all available configurations are used for DFT/SPE. To minimize sampling of configurations that are already well described by the model, a tighter sampling procedure (0.3 -0.7 eV/ Å) was used for the final two iterations.