Stable high-valent iridium single atoms for high-temperature CO<sub>2</sub> electrolysis.

Zhang, Shaowei; Wang, Shuo; Liu, Hewei; Zou, Geng; Guo, Yige; Zhang, Wenwen; Yu, Lina; Liu, Haolin et al. · Nat Commun · 2026

basic_science · Level V

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Abstract

Single-atom catalysts (SACs) offer high atomic efficiency and catalytic activity but are prone to aggregation and degradation under high-temperature conditions. Here, we propose a thermally and electrochemically stable high-valent iridium single atom synthesis strategy based on strong metal-support interactions (SMSI) to enhance high-temperature CO<sub>2</sub> electrolysis performance in solid oxide electrolysis cells (SOECs). The SMSI effect, in situ induced during high-temperature cell fabrication and operation, stabilizes the high-valent iridium single atom and simultaneously modulates the surface electronic structure of the La<sub>0.6</sub>Sr<sub>0.4</sub>FeO<sub>3-δ</sub> (LSF) cathode by weakening the Fe-O hybridization, finally promoting oxygen vacancy formation and enhancing CO<sub>2</sub> adsorption and activation. This approach boosts the CO<sub>2</sub>-to-CO electrolysis current density by 80.8% relative to the pristine LSF cathode, achieving 3.02 A cm<sup>-2</sup> at 800°C and 1.5 V with nearly 100% Faradaic efficiency and excellent stability over 600 h. These findings provide a viable strategy for designing thermally and electrochemically robust SACs for high-temperature catalytic reactions.