Altering the reactivity of pristine, N- and P-doped graphene by strain engineering: a DFT view on energy related aspects

TL;DR

This study uses DFT calculations to explore how strain affects the structure, electronic properties, and reactivity of pristine, N-doped, and P-doped graphene, revealing tunable surface topology and adsorption behaviors relevant for energy applications.

Contribution

It demonstrates how strain and dopant choice can modulate graphene's reactivity and surface topology, providing insights for optimizing energy-related applications.

Findings

Strain can both enhance and weaken H and Na adsorption on graphene.

Na adsorption energy correlates linearly with phosphorus charge in P-doped graphene.

Potential candidates for hydrogen storage and sodium-ion batteries are identified.

Abstract

For carbon-based materials, in contrast to metal surfaces, the relationship between strain and reactivity is not yet established, even though there are literature reports on strained graphene. Knowledge of such relationships would be extremely beneficial for understanding the reactivity of graphene-based surfaces and finding optimisation strategies which would make these materials more suitable for targeted applications. Here we investigate the effects of compressive and tensile strain (up to +/-5%) on the structure, electronic properties and the reactivity of pure, N-doped and P-doped graphene, using DFT calculations. We demonstrate the possibility of tuning the topology of the graphene surface by strain, as well as by the choice of the dopant atom. The reactivity of (doped) strained graphene is probed using H and Na as simple adsorbates of great practical importance. Strain can both enhance and weaken H and Na adsorption on (doped) graphene. In case of Na adsorption, a linear relationship is observed between the Na adsorption energy on P-doped graphene and the phosphorus charge. A linear relationship between the Na adsorption energy on flat graphene surfaces and strain is found. Based on the adsorption energies and electrical conductivity, potentially good candidates for hydrogen storage and sodium-ion battery electrodes are discussed.