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<p>The performance of solid oxide electrolysis cells (SOECs) for CO<sub>2</sub> electrolysis is significantly impeded by the limited electrochemical activity and insufficient durability of the cathode. This study introduces a novel (LaSrPrBaCaGd)<sub>2</sub>Fe<sub>1.5</sub>Mo<sub>0.5</sub>O<sub>6-<i>δ</i></sub> (LSPBCGFM) perovskite via A-site entropy engineering, to improve both activity and durability. Experimental results reveal that LSPBCGFM cathode-based SOEC achieves a current density of 1.34&#xa0;A·cm<sup>−2</sup> at 1.5&#xa0;V and 800&#xa0;°C, maintaining stable operation for more than 400&#xa0;h at 1.2&#xa0;V with negligible degradation. Theoretical calculations suggest that the high-entropy strategy shifts the transition metal d-band center and O-2p-band center closer to the Fermi energy level simultaneously, thereby initiating more favorable CO<sub>2</sub> adsorption and activation. In addition, a higher O-2p-band center promotes the formation and diffusion of oxygen vacancies. The findings of this study provide crucial insights into the role of conformational entropy strategies in CO<sub>2</sub> electrolysis and offer potential pathways for the development of highly efficient and stable catalysts.</p> Graphical abstract <p></p>

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Enhanced stability of perovskite cathode via entropy engineering for CO2 electrolysis

  • 期刊论文

  • 发表日期：

    2025年1月20日

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  • Nan Zhang,
  • Wen-Yu Zhang,
  • Yan-Sheng Gong,
  • Rui Wang,
  • Huan-Wen Wang,
  • Jun Jin,
  • Ling Zhao,
  • Bei-Bei He

摘要

The performance of solid oxide electrolysis cells (SOECs) for CO2 electrolysis is significantly impeded by the limited electrochemical activity and insufficient durability of the cathode. This study introduces a novel (LaSrPrBaCaGd)2Fe1.5Mo0.5O6-δ (LSPBCGFM) perovskite via A-site entropy engineering, to improve both activity and durability. Experimental results reveal that LSPBCGFM cathode-based SOEC achieves a current density of 1.34 A·cm−2 at 1.5 V and 800 °C, maintaining stable operation for more than 400 h at 1.2 V with negligible degradation. Theoretical calculations suggest that the high-entropy strategy shifts the transition metal d-band center and O-2p-band center closer to the Fermi energy level simultaneously, thereby initiating more favorable CO2 adsorption and activation. In addition, a higher O-2p-band center promotes the formation and diffusion of oxygen vacancies. The findings of this study provide crucial insights into the role of conformational entropy strategies in CO2 electrolysis and offer potential pathways for the development of highly efficient and stable catalysts.

Graphical abstract