2022/04/29 by Qiang Gao, Hemanth Somarajan Pillai, Yang Huang +8 · 3 citations
Chemical Engineering · Chemistry · Energy · #Ammonia Synthesis and Nitrogen Reduction #Nanomaterials for catalytic reactions #Advanced Photocatalysis Techniques
paper · pdf · doi:10.1038/s41467-022-29926-w
openalex publication_date 2022/04/29 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/26
Abstract The electrochemical nitrate reduction reaction (NO 3 RR) to ammonia is an essential step toward restoring the globally disrupted nitrogen cycle. In search of highly efficient electrocatalysts, tailoring catalytic sites with ligand and strain effects in random alloys is a common approach but remains limited due to the ubiquitous energy-scaling relations. With interpretable machine learning, we unravel a mechanism of breaking adsorption-energy scaling relations through the site-specific Pauli repulsion interactions of the metal d -states with adsorbate frontier orbitals. The non-scaling behavior can be realized on (100)-type sites of ordered B2 intermetallics, in which the orbital overlap between the hollow *N and subsurface metal atoms is significant while the bridge-bidentate *NO 3 is not directly affected. Among those intermetallics predicted, we synthesize monodisperse ordered B2 CuPd nanocubes that demonstrate high performance for NO 3 RR to ammonia with a Faradaic efficiency of 92.5% at −0.5 V RHE and a yield rate of 6.25 mol h −1 g −1 at −0.6 V RHE . This study provides machine-learned design rules besides the d -band center metrics, paving the path toward data-driven discovery of catalytic materials beyond linear scaling limitations.