Mechanisms of Hydrogen-Assisted CO2 Reduction on Nickel

High Resolution Image Download MS PowerPoint Slide Mechanistic details of catalytic reactions are critical to the development of improved catalysts. Here, we perform high quality Born–Oppenheimer molecular dynamics simulations of the reaction mechanisms associated with hydrogen-assisted CO 2 reduction on Ni(110). The simulation results show direct theoretical evidence for both associative and redox mechanisms in the reaction of atomic hydrogen with CO 2 . Because H 2 is dissociatively chemisorbed on Ni(110) with nearly unit probability, the mechanisms we find are also relevant to the reverse water-gas shift reaction (H 2 with adsorbed CO 2 ). Furthermore, we provide the first real-time demonstration of both Eley–Rideal (ER) and hot atom (HA) mechanisms when H impinges on adsorbed CO 2, and we show that both occur even for low kinetic energies. The trade-off between ER or HA mechanisms is found to be strongly dependent on CO 2 coverage. The results are compared with recent gas/surface measurements.