Rational Design of Transition-Metal Dual-Atom Catalysts: Exploiting Neighboring Effects for Efficient CO₂ Reduction

Abstract

Harnessing the synergistic interactions between adjacent bimetallic atoms, dual-atom catalysts (DACs) emerge as promising candidates for the CO₂ reduction reaction (CO₂RR). However, precise regulation of neighboring effects at dual-atom sites to optimize and enhance CO₂RR performance remains highly challenging. This review focuses on Fe-, Co-, Ni-, and Cu-based DACs, systematically elucidating how proximity effects modulate reaction intermediates and product selectivity in both homonuclear and heteronuclear systems. The distinct electronic configurations of homonuclear and heteronuclear DACs lead to diversified CO₂RR pathways and product distributions. When the two metal atoms are spatially separated, the weakened electronic coupling primarily lowers the energy barrier for C₁ intermediates, thereby improving the selectivity toward C₁ products. In contrast, a reduced metal–metal distance strengthens interatomic electronic interactions through the formation of N/O-coordinated or direct metal–metal structures, facilitating C─C coupling and thus enhancing C₂ product formation. A mechanistic understanding of C─C coupling serves as a fundamental basis for directing CO₂RR toward multi-carbon products with higher energy density and practical relevance. Additionally, theoretical investigations provide valuable insights into structure–activity relationships, offering guidelines for the rational design of efficient DACs for CO₂RR.

Keywords

C─C coupling / CO₂RR / dual-atom catalysts / neighboring effect / transition metal

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