First-principles study on a Li-decorated two-dimensional g-C6N6 monolayer: A promising ambient temperature reversible H2 storage material

Designing novel materials that exhibit superior reversibility and function under ambient conditions can facilitate the development of hydrogen energy applications. Two-dimensional (2D) g-C6N6 monolayers show great potential for use in hydrogen storage owing to their nanoporous structure, ultralight mass, and flexible electronic structure. However, the hydrogen storage potential of these materials is limited by the naturally weak interaction between 2D materials and hydrogen molecules caused by van de Waals forces. To address this issue, we studied the hydrogen storage performance of the complex by decorating active Li ions on a 2D g-C6N6 substrate through first-principles calculations. Our results showed that modifying the Li ions did not cause the original planar structure to deform but rather induced more active sites for hydrogen adsorption by establishing an electrostatic field between the Li ions and the g-C6N6 monolayer. Through this modification, reversible hydrogen storage was achieved under ambient conditions with an average adsorption energy of −0.197 eV/H2 and a high gravimetric capacity of 5.88 wt%. The electronic properties of the material were systematically investigated, and the results suggested that the enhanced capacity of the Li@ g-C6N6 system to store hydrogen resulted from the formation of a polarization field and the induced electrostatic effect. Our research offers a new possibility for achieving reversible hydrogen energy storage at room temperature.