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 (FECO) 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 FECO above 90% for over 60 h. Structural characterizations 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 communitive effect between adjacent dual atoms and provides a new strategy for designing highly efficient metal-N-C catalysts for boosted catalysis.