B ₃ N ₃ Li ₆ ‐ <i>n</i> H ₂ Complexes: A Computational Breakthrough in High‐Capacity and Stable Hydrogen Storage Systems

Abstract Efficient hydrogen storage is critical for enabling a sustainable energy future, demanding materials with exceptional capacity, reversibility, and stability under diverse conditions. Here, we investigate the hexalithioborazine (B 3 N 3 Li 6 ) as a promising hydrogen storage system, leveraging its unique structural and electronic properties using density functional theory. Systematic adsorption energy analysis reveals highly favorable adsorption energies ranging from −0.123 to −0.100 eV, ensuring reversible hydrogen uptake. Remarkably, the B 3 N 3 Li 6 ‐6H 2 complex achieves a hydrogen storage capacity of 9.44 wt%, surpassing DOE benchmarks, while adsorption extends up to 15H 2 molecules, attaining an unprecedented capacity of 20.69 wt%. The stabilization arises from strong ion‐induced dipole interactions between Li‐atoms and H 2 molecules, facilitated by charge transfer and polarization. Thermal stability of the B 3 N 3 Li 6 ‐6H 2 system is validated through atom density matrix propagation (ADMP) simulations across a broad temperature range (0–500 K), demonstrating stability even at elevated temperatures. These findings may suggest B 3 N 3 Li 6 as a transformative material for next‐generation hydrogen storage technologies, bridging the theoretical potential and practical application gap.