Boronated aromatic ring-fused structure: An efficient electrocatalyst for sustainable ammonia synthesis from nitric oxide pollutant

Nitric oxide (NO), a toxic and reactive member of the nitrogen oxides (NO_X) family, poses severe threats to human health and environmental ecosystems, necessitating the development of effective mitigation strategies. A promising approach involves converting NO into valuable chemical products, simultaneously reducing pollution and promoting sustainable energy utilization. To this end, this study explores the electrocatalytic potential of the recently synthesized boronated aromatic-ring fused structure (B-ARFS) for ammonia (NH₃) synthesis using NO as a feedstock. Computational analyses reveal that NO binds strongly to the B-ARFS nanostructure in an N end-on configuration, outperforming other adsorption modes such as NO side-on and O end-on. The N end-on configuration facilitates the efficient transfer of electrons, effectively weakening the N=O bond and creating an optimal environment for the electrocatalytic NO reduction reactions (NORR). The free energy profiles for various NORR mechanisms in the gas phase demonstrate that the NORR on the B-ARFS is thermodynamically a favorable process with an appreciably low limiting potential (U_L) of −0.23 V. Remarkably, introducing a solvent medium renders the NORR a spontaneous process. Furthermore, the high energy barriers associated with byproduct formation, including H₂ (HER), and N₂ show the exceptional selectivity of the B-ARFS catalyst for the NH₃ synthesis. Overall, this study highlights the transformative potential of B-ARFS nanostructure in enabling environmentally sustainable NH₃ production from NO pollutants.