The simulation model, depicted in Figure , is based on prior research showing that the layer-layer interactions have no significant impact on the electronic structure and that a single layer of LDH is a reliable model for the LDH catalysts. We simulated the LDH with full OH coverage to resemble the alkaline OER reaction conditions. Further details regarding the cell parameters are provided in the Supporting Information (Table ). The first Brillouin zone of the supercell was sampled using a 3 × 2 × 1 k point mesh for the top side model and a 3 × 1 × 2 k point mesh for the edge side model. The electronic structure convergence criteria was 10 -5 eV. The force convergence criteria and plane wave were set to 0.1 eV/ Å and 450 eV, respectively. A 15 Å vacuum region in along the non-periodic direction was included to prevent spurious interactions between periodic images.