It should be noted that around 40 billion HAT reaction SMILES can in principle be constructed by making combinations between bond dissociation reactions in the BDE-db dataset. Most of these reactions are very similar, involving HAT among two carbon atoms. We aimed to select a tiny sample (2,000 reactions) from this huge search space, covering maximal structural diversity, to compute explicitly. To this end, we iteratively sampled enumerated reactions in such a way that the differential reaction fingerprint (radius = 3; nbits = 2048) distances with all previously sampled reactions exceeded 0.85 (see Section S1 for more details). As the level of theory for the DFT calculations, we selected M06-2X/def2-SVP for optimizations and frequency calculations, i.e., thermal corrections. Single-point energy refinements were performed at M06-2X/def2-TZVP level of theory. The choice for the functional and basis set was inspired by the benchmarking results from Paton et al. One technical aspect where we decided to deviate in our workflow from the previous work on cycloaddition reactions is the conformer selection. Previously, the default number of conformers in autodE (300) would be generated for every species along the profile, a root mean squared deviation (RMSD) threshold of 0.3 Å would then be applied to remove very similar conformer geometries, after which the lowest energy conformer, computed at GFN2-xTB level of theory, would be selected. Remarkably, for HAT reactions, this methodology leads to poor reproducibility of the activation energies (mean absolute errors between successive runs on 30 randomly sampled reactions amounting to more than 2.1 kcal/mol for the activation energy, and ∼ 0.5 kcal/mol for the reaction energy; cf. Section S1). After some benchmarking, we adapted these conformer selection settings, selecting 1000 conformers for every species, using an RMSD cut-off of 0.1 Å, and ranking conformers based on single-point M06-2X/def2-SVP energies. In this manner, two successive runs of the workflow on the same set of reaction SMILES result in an acceptable mean absolute error (MAE) of ∼1 kcal/mol for the activation energies and ∼0.6 kcal/mol for the reaction energies.