Electronic Activation via Targeted Interface Engineering: Unlocking High‐Performance CO 2 Electrolysis in Commercial Electrodes

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High‐temperature CO 2 electrolysis is a promising route for sustainable fuel production and carbon utilization, yet its efficiency is limited by the scarcity of highly active electrode materials. This study demonstrates heterointerface engineering as a key strategy to dramatically enhance the performance of the commercial electrode La 0.7 Sr 0.3 CoO 3− δ (LSC) for high‐temperature CO 2 electrolysis. Advanced spectroscopic techniques identify carbonate species (CO 3 2− ) as critical reaction intermediates, whose formation is effectively promoted at the PrO 2 –LSC heterointerface. It is confirmed that charge transfer from the LSC matrix to the PrO 2 layer induces a local electric field and alters oxygen defect chemistry. The synergistic effects of stronger CO 2 adsorption, enhanced electron transfer, and strengthened bonding between surface metal sites and oxygen‐containing intermediates near the heterointerface collectively drive the superior CO 2 reduction activity of the PrO 2 –LSC electrode. These findings provide crucial insights into the role of heterostructure interfaces in boosting electrode catalytic activity for CO 2 electrolysis, guiding the rational design of highly active electrocatalysts for high‐temperature electrochemical devices for energy and environmental remediation applications.