First-principles simulations of catalytic systems for hydrogen production*

One way to produce hydrogen more efficiently is by using a catalyst which can increase the rate of the hydrogen evolution reaction (HER). In order to assist the design of new catalytic systems, we perform first-principles density functional theory (DFT) calculations of the electronic structure of several catalysts and attempt to predict their efficiency for HER. We focus on one class of molecular catalysts of the form M(L)₂ composed of an inexpensive transition metal atom (M=Co, Ni, Cu) and coordinated with two organic ligands L which can be bipyridine (bipy) or pyridine DAT (PyDAT). We use the abinit software and the projector-augmented-wave (PAW) methods to compute the structural parameters of the molecules, and the formation energy of each step of the four-step catalytic cycle. Our method accurately reproduces the efficiency of catalysts in the literature. We will also discuss its predictive power for different ligands and their respective hydrogen production.