Importance of d-electron coupling in dual-atom catalysts for electrocatalytic CO2 reduction reaction

• • Mn/Cu-NC dual-atom catalyst achieves a limiting potential of -0.15 V for CO2RR to HCOOH, significantly lower than most single-atom catalysts (typically > -0.5 V), enabling reduced overpotential and higher energy efficiency in industrial electrolyzers. • • The d-band center of Mn shifts upward by approximately 0.3 eV due to d-electron coupling with Cu, enhancing *OCHO adsorption and reducing the limiting potential; this descriptor can guide rational design of DACs with tailored activity. • • Heteronuclear DACs outperform homonuclear counterparts: Mn/Cu-NC shows a selectivity for HCOOH over CO and H2, with a calculated Faradaic efficiency exceeding 90% at -0.15 V, addressing the low selectivity bottleneck in CO2RR. • • The study establishes a direct correlation between d-band center position and catalytic activity, providing a predictive metric for screening DACs; this can accelerate experimental development by reducing trial-and-error synthesis costs.