Engineering atomic-scale synergy of Ni and Mn dual-atom catalysts for highly efficient CO2 electroreduction

Abstract

The electrochemical CO₂ reduction into value-added products is a promising way to reduce CO₂ emissions. However, the design of efficient dual-atom catalysts to improve electrochemical CO₂ reduction performance remains a challenge. Herein, a novel Ni₁Mn₁–NC dual-atom catalyst with neighboring Ni and Mn atomic interactions is developed for CO₂ reduction. The Ni₁Mn₁–NC catalyst with Ni and Mn atomic pairs exhibits excellent performance with a faradaic efficiency of CO (FE_CO) of up to 97% at −0.7 V vs. RHE, far outperforming the Ni₁–NC and Mn₁–NC single-atom catalysts. In addition, the CO partial current density achieves 9.0 mA cm⁻² at −1.1 V vs. RHE, which is 2.3 and 45.0 times higher than that of Ni₁–NC and Mn₁–NC. Moreover, Ni₁Mn₁–NC demonstrated long-term stability with FE_CO above 90% for over 60 h. Structural characterization and kinetic analysis reveal that Mn atoms donate partial electrons to Ni via N-bridged interaction and facilitate the adsorption of CO₂ and the formation of *COOH, thus boosting CO₂ electroreduction. This work elucidates the importance of the cooperative effect between adjacent dual atoms and provides a new strategy for designing highly efficient metal–N–C catalysts for boosted catalysis.