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<p>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.</p>

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Stable high-valent iridium single atoms for high-temperature CO2 electrolysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月18日

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  • Shaowei Zhang,
  • Shuo Wang,
  • Hewei Liu,
  • Geng Zou,
  • Yige Guo,
  • Wenwen Zhang,
  • Lina Yu,
  • Haolin Liu,
  • Xiaomin Zhang,
  • Mingrun Li,
  • Peng Zhang,
  • Runsheng Yu,
  • Xusheng Zheng,
  • Yuefeng Song,
  • Guoxiong Wang,
  • Xinhe Bao

摘要

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 CO2 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 La0.6Sr0.4FeO3−δ (LSF) cathode by weakening the Fe−O hybridization, finally promoting oxygen vacancy formation and enhancing CO2 adsorption and activation. This approach boosts the CO2-to-CO electrolysis current density by 80.8% relative to the pristine LSF cathode, achieving 3.02 A cm−2 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.