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

Abstract

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 (Ead) of -1.74 eV. The negative Ead 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.