Aromatic M12B60 (M = Y, Lu) metallo-borospherenes for reversible hydrogen storage

Abstract

Metallo-borospherenes, a rapidly evolving class of boron-based nanostructures, exhibit intriguing diversity in both geometric architectures and electronic properties. Recently, the experimental identification of the D_3h-symmetric Ln₃B₁₈⁻ (Ln = La, Tb) clusters marked a significant milestone in this emerging field. In this study, a new family of metallo-borospherenes M₁₂B₆₀ (M = Y, Lu) was predicted using first-principles calculations. Ab initio molecular dynamics simulations and vibrational frequency analyses confirm their thermodynamic and kinetic stability. Detailed bonding analysis reveals the presence of 108 delocalized multi-center two-electron bonds within the cage, accompanied by pronounced aromatic character, which collectively account for their exceptional stability. Notably, the Y₁₂B₆₀ cage exhibits potential as a promising hydrogen storage material. Its curved surface provides multiple favorable adsorption sites, enabling H₂ molecules to form layered distributions. The Y₁₂B₆₀ cage can adsorb up to 89 H₂ molecules with an average adsorption energy of −0.201 eV per H₂, corresponding to a gravimetric density of 9.44 wt%, meeting practical adsorption requirements. Ab initio molecular dynamics simulations further validate the structural robustness and adsorption capacity of Y₁₂B₆₀ under near-ambient conditions, underscoring its promise for reversible hydrogen storage applications.