Hydrogen storage in scandium decorated triazine based g-C3N4: Insights from DFT simulations

Abstract

Hydrogen is being considered a ‘fuel of the future,’ a viable alternative to fossil fuels in fuel cell vehicles. Using Density Functional Theory simulations, reversible, onboard hydrogen storage in Sc-decorated triazine-based graphitic carbon nitride (g-C3N4) has been explored. Sc atom binds strongly on the g-C3N4 structure with a binding energy of −7.13 eV. Each Sc atom can reversibly bind 7 molecules of hydrogen, giving a net gravimetric storage capacity of 8.55 wt%, an average binding energy of −0.394 eV per H2, and a corresponding desorption temperature of 458.28 K, fulfilling the criteria prescribed by the US Department of Energy. The issue of transition metal clustering has been investigated by computing the diffusion energy barrier (2.79 eV), which may be large enough to hinder the clustering tendencies. The structural integrity of Sc-g-C3N4 has been verified through ab-initio Molecular Dynamics simulations. The interaction mechanism of Sc over g-C3N4 and H2 over Sc-g-C3N4 has been explored using density of states and charge transfer analysis. A flow of charge from valence 3d orbitals of Sc towards vacant orbitals of g-C3N4 during the binding of Sc over g-C3N4 is observed. The binding of H2 on Sc-g-C3N4 may be via Kubas type of interactions which is stronger than physisorption due to net charge gain by H 1s orbital from Sc 3d orbital. Our systematic investigations indicate that Sc-decorated g-C3N4 may be a high-performance material for reversible hydrogen storage applications.