Decomposition of activated CO2 species on Ni(110): Role of surface diffusion in the reaction mechanism

• Adsorption and decomposition of CO2 on Ni(110) was studied.
• Possible reaction pathways were investigated.
• Mechanism of CO2 decomposition on Ni(110) was clarified.

Chemisorption and decomposition of CO2 on Ni(110) surface have been studied by means of spin-polarized density functional theory calculations. Several possible CO2/Ni(110) conformations with similar adsorption energies were found. The bonding nature of the adsorbed CO2 was further analyzed on the basis of partial density of states (PDOS) and effective bond order (EBO) results, indicating the enhanced charge transfer and significant activation of the CO bond. Climbing image nudged elastic bound calculations provide an insight into CO2/Ni(110) → CO/Ni(110) + O/Ni(110) reaction mechanism. All computed reaction pathways can be separated into two stages: 1) surface diffusion of CO2 to the one energetically favored conformation; 2) breakage of the coordinated C–O bond. The total reaction barrier (relative to the energy of CO2/Ni(110)) was found about 0.44 eV.

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