(521an) High Throughput Workflow for Electrocatalysis in Single Atom 2D Materials

Two dimensional materials such as graphene and MXenes have garnered significant popularity for a variety of electrocatalytic reactions owed to their unique structural and electronic properties. Dimensional confinement provides a large surface area-to-volume ratio allowing for more actives sites while also providing unique electronic properties due to quantum confinement, whereby the electronic band structure deviates from its 3D counterpart. The introduction of transition metal (TM) dopants and non-metal ligands (B, C, N, O, Si, P, S) can further modulate the electronic properties (ergo catalytic properties) of 2D materials. A large-scale computational assessment of surface intermediates on these pristine and doped 2D structures will give invaluable insight into the catalytic nature of this relatively new class of materials. However, a full assessment of the catalytic properties of just one combination of dopant and 2D material requires numerous DFT calculations performed in serial to obtain: lattice parameters, stability of doped sites, and surface intermediates. Keeping track of and curating these calculations for one, let alone thousands, of combinations can become overwhelmingly unwieldy. We addressed this issue by constructing a high-throughput workflow that automates this entire process. In addition to performing DFT relaxations to assess the thermodynamic quantities, the workflow will also assessed the electronic properties after each calculation by obtaining the density of states and integrated crystal orbital Hamiltonian population. The initial dataset covers oxygen evolution reaction (OER) on TM and ligand doped graphene and MXenes (TM₄X₃, TM₃X₂, TM₂X, with X= C or N and TM=3d, 4d, and 5d TMs). We specifically calculated the interaction of the three surface intermediates (O*, OH*, OOH*) of OER interacting with the TM dopant on the 2D plane. The dataset provided is carefully curated and archived in a public database that can be accessible through our API which will assist in data analytics.