Aluminium storage using nitrogen-doped graphene nanoribbons from first principles

TL;DR

This study uses first-principles DFT calculations to show that nitrogen doping, especially with edge NO groups and pyridinic N, significantly enhances aluminum adsorption on graphene nanoribbons, informing better battery electrode design.

Contribution

It demonstrates that specific N-doping configurations can nearly double Al adsorption strength on graphene nanoribbons, a novel insight for battery material development.

Findings

N-doping with edge NO groups increases Al adsorption nearly twofold.

Edge sites alone do not significantly affect Al adsorption energetics.

Different N-containing defects have varying impacts on Al interaction.

Abstract

Pristine graphene interacts relatively weakly with Al, which is a specie of importance for novel generations of metal-ion batteries. We employ DFT calculations to explore the possibility of enhancing Al interaction with graphene. We investigate non-doped and N-doped graphene nanoribbons, address the impact of the edge sites, which are always present to some extent in real samples, and N-containing defects on the material's reactivity towards Al. The results are compared to that of pristine graphene. We show that introduction of edges does not affect the energetics of Al adsorption significantly by itself. On the other hand, N-doping of graphene nanoribbons is found to affect the adsorption energy of Al to the extent that strongly depends on the type of N-containing defect. While graphitic and pyrrolic N induce minimal changes, the introduction of edge NO group and doping with in plane pyridinic N result in Al adsorption nearly twice as strong as on pristine graphene. The obtained results could guide the further design of advanced materials for Al-ion rechargeable batteries.