CO₂ and H₂ Adsorption and Reaction at Ni_n/YSZ(111) Interfaces: A Density Functional Theory Study

To recycle CO2 into sustainable fuel and chemicals, co-electrolysis of CO2 and H2O can be achieved in solid oxide electrolysis cells, where the molecules are supplied to the Ni/YSZ electrode (YSZ = yttria-stabilized zirconia). We have investigated the interaction of a CO2 molecule with the clean YSZ(111) surface and with Nin/YSZ(111) (n =1, 4-7, 10, 20) interfaces, using spin polarized density functional theory (DFT) and long-range dispersion correction. In this work, we show that, although the electronic structure of the clusters depends on the cluster size, the interaction strength of CO2 with the interface is independent of the size of the supported nickel particle. Finally, we have considered the reverse water gas shift reaction and determined the hydrocarboxylic intermediate in the reaction mechanism over Ni5/YSZ(111). The data described here are: 1- The calculated energies and geometries of the CO2 molecule adsorbed on YSZ(111) and Nin/YSZ(111) (n =1, 4-7, 10, 20) interfaces. 2- The calculated elongations and angles of the CO2 molecule adsorbed on YSZ(111) and Nin/YSZ(111) (n =1, 4-7, 10, 20) interfaces. 3- The IR spectra of the CO2 molecule adsorbed on YSZ(111) and Nin/YSZ(111) (n =1, 4-7, 10, 20) interfaces. 4- The Density of States of the CO2 molecule adsorbed on YSZ(111) and Nin/YSZ(111) (n =1, 4-7, 10, 20) interfaces. 5- The energy profile of the reverse water gas shift reaction