| Summary: | Hydrogen, as an important clean energy source, is difficult to store and transport, which hinders its applications in real practice. Developing robust yet affordable storage media remains to be a challenge for scientists. In this study, Ab Initio Molecular Dynamics (AIMD) simulations were employed to evaluate the performance of aluminum (Al) decorated carbon nitride (g-C<sub>3</sub>N<sub>4</sub>, heptazine structure) in hydrogen storage; and a benchmarking study with Mg-doped g-C<sub>3</sub>N<sub>4</sub> was also performed to provide theoretical insights for future study. We found that each 2 × 2 supercell can accommodate four Al atoms, and that partial charge from single Al sites can be transferred to adjacent nitrogen atoms of g-C<sub>3</sub>N<sub>4</sub>. These isolated Al sites tend to be electronically positive charged, serving as active sites for H<sub>2</sub> adsorption, predominately by triggering enhanced electrostatic interactions. The H<sub>2</sub> molecules are adsorbed by both Al and N atoms, and are easily polarized, giving rise to electrostatic interactions between the gas molecules and the surface. Effective adsorption sites were determined by electronic potential distribution maps of the optimized configurations. Each 2 × 2 supercell can adsorb up to 36 H<sub>2</sub> molecules, and the corresponding adsorption energies are within the range of −0.10 to −0.26 eV. The H<sub>2</sub> storage capacity of the Al-decorated g-C<sub>3</sub>N<sub>4</sub> is 7.86 wt%, which surpasses the goal of 5.5 wt%, set by the US department of energy. This proposed Al-decorated g-C<sub>3</sub>N<sub>4</sub> material is therefore predicted to be efficient for hydrogen storage. This work may offer some fundamental understandings from the aspect of electronic sharing paradigm of the origin of the excellent hydrogen storage performance by metal decorated 2D materials, acting as an demonstration for guiding single metal atom site-based materials’ designing and synthesis.
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