In Situ Self-Assembled Active and Stable Ir@MnO_x/La_0.7Sr_0.3Cr_0.9Ir_0.1O_3-δ Interfaces for CO₂ Electrolysis

Solid oxide electrolysis cells are prospective approaches for CO₂ utilization but face significant challenges due to the sluggish reaction kinetics and poor stability of the fuel electrodes. Herein, we strategically addressed the long-standing trade-off phenomenon between enhanced exsolution and improved structural stability via topotactic ion exchange. The surface dynamic reconstruction of the MnO_x/La_0.7Sr_0.3Cr_0.9Ir_0.1O_3-δ (LSCIr) catalyst was visualized at the atomic scale. Compared with the Ir@LSCIr interface, the in situ self-assembled Ir@MnO_x/LSCIr interface exhibited greater CO₂ activation and easily removable carbonate intermediates, thus reached a 42 % improvement in CO₂ electrolysis performance at 1.6 V. Furthermore, an improved CO₂ electrolysis stability was achieved due to the uniformly wrapped MnO_x shell of the Ir@MnO_x/LSCIr cathode. Our approach enables a detailed understanding of the dynamic microstructure evolution at active interfaces and provides a roadmap for the rational design and evaluation of efficient metal/oxide catalysts for CO₂ electrolysis.