Single-Atom Anchored on Perovskite With Strong Metal-Oxide Interaction for Efficient High Temperature CO2 Electrolysis.

Efficient electrochemical CO2 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 Sr2Fe1.5Mo0.5O6-δ (SFM) perovskite electrocatalyst, designed for high temperature CO2 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 CO2 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 CO2 electrolysis.