Unveiling the potential of aluminum-decorated 3D phosphorus graphdiyne as a catalyst for N₂O reduction

Interest in single-atom catalysts (SACs) has surged due to their potential to mitigate greenhouse N₂O gas from the environment. In this study, we explore the potential of N₂O reduction using porous 3D phosphorus graphdiyne decorated with an Al atom (3D-Al/PGDYN) through density functional theory. Results confirm the energetic stability of Al decorations on 3D-PGDYN and indicate that the Al atom plays an active role in catalysis. The N₂O molecule undergoes spontaneous dissociation on the surface of the 3D-Al/PGDYN, initiating from the O-end, with a dissociation energy of -2.93 eV. In parallel, N₂O dissociation through the N-end involves chemisorption onto the 3D-Al/PGDYN surface, with an adsorption energy (E_ad) of -1.74 eV. The negative E_ad values (-2.47 and -2.64 eV) indicate that CO and O₂ species chemisorb onto the 3D-Al/PGDYN surface, but these energies are lower than that of N₂O, suggesting that CO and O₂ molecules do not hinder the N₂O reduction process. Furthermore, the reaction CO + O* → CO₂, which is vital for catalyst regeneration, proceeds swiftly on the 3D-Al/PGDYN catalyst with a low energy barrier of 0.11 eV, highlighting the catalyst's exceptional reactivity. This work holds significance in the design of catalysts and could be instrumental in developing new and efficient solutions for effectively removing harmful N₂O from the environment.