Fe-doped carbon nanotubes: towards the molecular design of new catalysts for the oxygen reduction reaction.

Using DFT computational methods, single-walled carbon nanotubes (CNT) are explored in different geometric configurations (armchair, chiral and zigzag) doped with Fe. Geometry, electronic structure and magnetic properties are investigated for all systems, in order to evaluate a potential application of these structures as electrocatalysts in efficient and low-cost fuel cells. In search for a better electrode material, we turn our attention on nature for help. Oxygen molecules are well-known to reveal a remarkable affinity to the heme group. Therefore, we model the adsorption/dissociative behavior of oxygen molecules on carbon nanotubes doped with Fe atoms. We analyze in detail the effect of the chiral nature of carbon nanotubes that governs their electric, magnetic and chemical behavior. Our results indicate that the dissociation phenomenon involving the armchair (5,5) Fe@CNT is more favored than other chiralities and other doped CNT systems, leading to the lowest activation barrier.