Surface Energy as a Descriptor of Catalytic Activity

Computational searches for catalysts of the hydrogen evolution reaction commonly use the hydrogen binding energy (HBE) as a predictor of catalytic activity. Accurate evaluation of the HBE, however, can involve large periodic supercell slab models that render high-throughput screening relatively expensive. In contrast, calculations of other relevant surface properties, such as the surface energy, work function, and potential of zero charge (PZC), require only small surface unit cells and are hence less expensive to compute. Correlations between catalytic activity and these surface properties warrant exploration because of this reduced computational cost. Here, we use density functional theory in conjunction with three different exchange-correlation functionals—the local density approximation (LDA), the Perdew–Burke–Ernzerhof (PBE) generalized gradient approximation, and the PBEsol functional (a reparameterization of the PBE functional)—to calculate the lattice constants, surface energy, cohesive energy, an...