Synergistic Catalysis at Zn–Mn Dual‐Atoms Sites for Efficient Electrocatalytic Oxidation of Formaldehyde

ABSTRACT Developing high‐performance electrocatalysts through rational structural design is essential for advancing integrated energy conversion technologies. The versatile coordination between organic ligands and metal centers enables precise incorporation of metallic species within carbon matrix, offering exceptional atomic dispersion control. Herein, as evidenced by HAADF‐STEM and XAS, a bimetallic‐bridged coordination architecture featuring a ZnMn‐N 8 atomic structure is rationally fabricated. In a custom‐built gas‐solid phase electrocatalytic system for formaldehyde (HCHO) degradation, it exhibits 63.8% HCHO decomposition efficiency with 92.3% CO 2 selectivity. Density functional theory (DFT) calculations reveal that the bridged metal‐nitrogen coordination modulates the d ‐band center, facilitating Zn‐to‐Mn electron transfer. This electronic redistribution creates electron‐deficient Zn active sites that enhance oxygen‐binding with HCHO through optimized orbital hybridization, thereby boosting electrocatalytic conversion efficiency. This work not only extends bimetallic‐bridged coordination catalysts from liquid‐phase to gas‐phase applications, but also provides fundamental insights into gaseous HCHO removal.