Atomically Dispersed Fe–Mo Catalytic Pairs Enable Two‐Electron Li 2 C 2 O 4 Pathway for Reversible Li–CO 2 Batteries

ABSTRACT Lithium‐carbon dioxide (Li–CO 2 ) batteries present a promising strategy for coupling high‐energy storage with CO 2 utilization, yet their development is impeded by sluggish kinetics and severe polarization associated with insulating discharge products. Achieving selective and reversible two‐electron conversion toward Li 2 C 2 O 4 remains a critical challenge for improving energy efficiency and cycling stability. Herein, we report electronically asymmetric dual‐atom Fe–N–Mo catalytic pairs anchored on a highly conjugated N‐doped carbon (NC) framework, forming Fe 1 ‐Mo 1 integrated catalytic pairs (Fe 1 ‐Mo 1 /ICPs) to promote a reversible two‐electron Li 2 C 2 O 4 conversion pathway. The πconjugated highly conjugated N‐doped carbon framework stabilizes atomically dispersed Fe and Mo sites while enhancing inter‐site electronic coupling. Within the proposed heteronuclear Fe–N–Mo configuration, intrinsic electronic asymmetry generates electrophilic Fe and nucleophilic Mo sites, enabling dynamic charge redistribution and complementary catalytic behavior. Such a donor‐acceptor bridge effectively regulates intermediate adsorption/desorption and suppresses competing reaction pathways, thereby favoring the selective and reversible formation of Li 2 C 2 O 4 . Operando spectroscopic analysis confirms the preferential reversible Li 2 C 2 O 4 evolution during cycle, while density functional theory calculations reveal substantially reduced energy barriers for key reaction intermediates. Benefiting from the unique electronic environment and synergistic effects of asymmetric dual‐atom sites, the FeMoCN catalyst delivers outstanding electrochemical performance.