Modulation of charge in C9N4 monolayer for a high-capacity hydrogen storage as a switchable strategy

Developing advanced hydrogen storage materials with high capacity and efficient reversibility is a crucial aspect for utilizing hydrogen source as a promising alternate to fossil fuels. In this paper, we have systematically investigated the hydrogen storage properties of neutral and negatively charged C₉N₄ monolayer based on density functional theory (DFT). Our foundings indicate that injecting additional electrons into the adsorbent significantly boosts the adsorption capacity of C₉N₄ monolayer to H₂ molecules. The gravimetric density of negatively charged C₉N₄ monolayer can reach up to 10.80 wt% when fully covered with hydrogen. Unlike other hydrogen storage methods, the storage and release processes happen automatically upon introducing or removing extra electrons. Moreover, these operations can be easily adjusted through activating or deactivating the charging voltage. As a result, the method is easily reversible and has tunable kinetics without requiring particular activators. Significantly, C₉N₄ is proved to be a suitable candidate for efficient electron injection/release due to its well electrical conductivity. Our work can serve as a valuable guide in the quest for a novel category of materials for hydrogen storage with high capacity.