Ternary Sn‐Ti‐O Electrocatalyst Boosts the Stability and Energy Efficiency of CO2 Reduction

Abstract Simultaneously improving energy efficiency (EE) and material stability in electrochemical CO 2 conversion remains an unsolved challenge. Among a series of ternary Sn‐Ti‐O electrocatalysts, 3D ordered mesoporous (3DOM) Sn 0.3 Ti 0.7 O 2 achieves a trade‐off between active‐site exposure and structural stability, demonstrating up to 71.5 % half‐cell EE over 200 hours, and a 94.5 % Faradaic efficiency for CO at an overpotential as low as 430 mV. DFT and X‐ray absorption fine structure analyses reveal an electron density reconfiguration in the Sn‐Ti‐O system. A downshift of the orbital band center of Sn and a charge depletion of Ti collectively facilitate the dissociative adsorption of the desired intermediate COOH* for CO formation. It is also beneficial in maintaining a local alkaline environment to suppress H 2 and formate formation, and in stabilizing oxygen atoms to prolong durability. These findings provide a new strategy in materials design for efficient CO 2 conversion and beyond.