Nowadays, scientists are increasingly focused on finding new efficient 2D materials for hydrogen storage due to their large specific surface area, exceptional physisorption properties, and high gravimetric capacity. In this respect, we have analyzed the potential of new 2D orthorhombic (o)-B₂CN and o-B₂C₂ materials as lightweight solid mediums for hydrogen storage, employing lithium decoration through density functional theory (DFT) calculations. Both materials were found to be conductive and demonstrated excellent mechanical, dynamical and thermal stability. The binding energies of lithium adatoms to the monolayers during the decoration process were found to be −3.38 and −3.72 eV for o-B₂CN and o-B₂C₂, respectively. These values indicate strong interactions with both substrates and the lack of lithium clustering given that they are higher than its cohesive energy (−1.63 eV). The lithium decoration technique significantly improves the adsorption of H₂ molecules on both materials, where each system adsorbs 32 molecules with an average adsorption energy of 0.25 and 0.23 eV for 32H₂@8Li-B₂CN and 32H₂@8Li-B₂C₂, respectively, along with excellent gravimetric capacities of 12.87 and 13.29 wt% and desorption temperatures of 186 and 171 K. To assess dynamical stability, AIMD calculations were conducted on fully loaded H₂ systems at temperatures of 100, 200, 400 and 500 K, demonstrating complete H₂ desorption and confirming the reversibility of both systems. A radial distribution function (RDF) analysis was conducted to examine the thermal effects on Li–H atomic correlations and assess the stability of hydrogen adsorption at different temperatures. Based on these results, it can be concluded that Li-decorated o-B₂CN and o-B₂C₂ show considerable potential for hydrogen storage applications.

Finding an appropriate new anode material with high electrochemical performance for lithium-ion batteries (LIBs) is considered one of the significant challenges for both the academic and industrial research communities. Herein, we propose to explore the efficiency of a newly designed two-dimensional (2D) material, named orthorhombic dialuminium dinitride (o-Al2N2), as an alternative anode material for LIB systems through first-principles calculations and ab initio molecular dynamics (AIMD) simulations. The obtained results show that orthorhombic-Al2N2 exhibits a high specific capacity of 1144.2913 mAhg−1, an operating voltage around 0.575 V, and a low kinetic diffusion barrier of 0.26 eV. These results prove the suitability of the o-Al2N2 monolayer as a promising anode material for LIBs with high structural stability, strong binding energy towards lithium adsorbent, fast lithium diffusion, and a high theoretical capacity. These features rank the 2D o-Al2N2 monolayer among the best choices for the anode part of the next-generation rechargeable LIBs.