Ab Initio Study on Doped Cu 138 X 2 Nanoparticles With Dispersed Surface‐Active Sites for Enhanced Electrocatalytic Nitrate Reduction to Ammonia
Year: 2025
Type: article
Abstract: Copper nanoparticles (NPs) exhibit significant potential in electrocatalysis owing to their tunable electronic structure and abundant surface‐active sites. However, the multifaceted complexity of Cu‐based nanoparticles induced by heteroatom dopants fundamentally limits our ability to decipher the electrochemical nitrate reduction reaction (NO 3 RR) mechanism, creating a critical knowledge gap that obstructs the targeted engineering of advanced catalysts with atomic precision. In this study, we employed first‐principles calculations to design a series of highly surface‐dispersed transition metal‐doped Cu 138 X 2 (X = Ag, Au, Pd, Zn, Ni, Pt) bimetallic electrocatalysts for nitrate reduction to ammonia (NH 3 ), based on the structure of Cu 140 NPs. Theoretical analysis revealed that Cu 138 Au 2 exhibits significant advantages in NO 3 RR, with a remarkably low limiting potential of −0.20 eV. In addition, significant energy barriers were observed for the formation of by‐products NO and NO 2 on Cu 138 Au 2 , ensuring high selectivity towards ammonia. For Cu‐based catalysts, we propose that the *NO 2 → *HNO 2 step is critical and can serve as a descriptor for rapid screening of these catalysts. This study not only provides important insights into the research of Cu NPs as NO 3 RR electrocatalysts but also establishes a theoretical foundation for enhancing their catalytic performance through surface modification or compositional tuning.
Source: Chemistry - A European Journal
Authors: Hao‐nan Xu, Tao Wu, An‐hui Lu
Language: English
Subfield: Catalysis
Field: Chemical Engineering
Domain: Physical Sciences
Open Access status: bronze
Awards: G1852470804, G3133593441
OpenAlex ID: W4409216392