Single‐Atom Anchored on Perovskite With Strong Metal‐Oxide Interaction for Efficient High Temperature CO 2 Electrolysis

Abstract Efficient electrochemical CO 2 reduction remains a grand challenge in advancing carbon‐neutral energy technologies. Here, an efficient solid‐state approach for the fabrication of a novel single‐atom Ir anchored Sr 2 Fe 1.5 Mo 0.5 O 6‐δ (SFM) perovskite electrocatalyst, designed for high temperature CO 2 electrolysis in solid oxide electrolysis cells (SOECs) is reported. The resulting four‐coordinated Ir‐O‐Fe/Mo configuration induces pronounced interfacial electronic reconstruction and strong metal‐oxide interaction, substantially lowering the energy barrier for CO 2 electrolysis, as indicated by extended X‐ray absorption fine structure (EXAFS) analysis and density functional theory (DFT) calculations. When employed as a cathode in SOECs, the 2Ir/SFM (2 wt.% Ir) electrocatalyst achieves a high current density of 1.63 A cm −2 at 1.5 V and 800 °C, along with excellent Faradaic efficiency and long‐term operational stability. These findings offer atomistic insights into the structure‐performance relationship of single‐atom/perovskite heterostructures, underscoring the commercial potential of SOECs for CO 2 electrolysis.