Comparative study and screening of Single-Atom and homonuclear Dual-Atom catalysts for NO reduction via electrocatalysis

Abstract

Electrocatalytic technology offers a promising solution to address environmental pollution and resource scarcity. The development of high-stability and selective catalysts is crucial in this regard. This paper focuses on single-atom catalysts (SACs) and homonuclear dual-metal catalysts (DACs) constructed using transition metal atoms as active centers. Catalytic activity and selectivity of these catalysts in the nitric oxide reduction reaction (NORR) process are systematically investigated through first-principles calculations, while exploring the influence of adjacent metal atoms on their characteristics. Using a four-step screening approach, we identify Ti2-N6 as a standout candidate catalyst with a low applied voltage (-0.24 V) for selective NO catalysis and significant inhibition of competitive responses. Homonuclear DACs inherit the advantages of SACs while disrupting the inherent linear relationship, resulting in reduced applied voltage requirements and enhanced catalytic performance. This work presents an efficient catalyst screening method and highlights the unique characteristics and advantages of homonuclear DACs over SACs.