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<p>High-entropy oxides have emerged as a promising group of candidates for various catalytic fields, including seawater electrolysis. However, without rational understanding and guidance, designing multielement compositions for high-entropy systems and elucidating the synergistic effect of diverse elements in catalysis remain significant challenges. Herein, we report spin-state regulation of a high-entropy Ruddlesden–Popper perovskite oxide for efficient seawater electrolysis. The Cu<sup>2+</sup> and Mn<sup>3+</sup> with Jahn-Teller effect induced a transition of Fe<sup>3+</sup>/Co<sup>3+</sup> spin state from low spin to high spin configuration. The high spin Fe<sup>3+</sup>/Co<sup>3+</sup> favor OH<sup>−</sup> adsorption and deprotonation during seawater oxidation. Besides, the oxygen intermediates adsorbed on high spin active sites repel the Cl<sup>−</sup> ions. Consequently, (La<sub>0.76</sub>Sr<sub>0.24</sub>)<sub>3</sub>(Fe<sub>0.22</sub>Co<sub>0.21</sub>Ni<sub>0.18</sub>Cu<sub>0.17</sub>Mn<sub>0.22</sub>)<sub>2</sub>O<sub>7</sub> achieved robust seawater oxidation for over 1200 h at 200 mA cm<sup>−2</sup>, showing competitive performance. The anion exchange membrane electrolyzer coupling with (La<sub>0.76</sub>Sr<sub>0.24</sub>)<sub>3</sub>(Fe<sub>0.22</sub>Co<sub>0.21</sub>Ni<sub>0.18</sub>Cu<sub>0.17</sub>Mn<sub>0.22</sub>)<sub>2</sub>O<sub>7</sub> anode and Pt/C cathode could maintain the seawater splitting performance of 1 A cm<sup>−2</sup> at 1.76 V and incessantly operate for 800 h. This spin-engineered strategy is universal to other high-entropy perovskite oxides and spinel oxides, offering promising way for designing efficient high-entropy catalysts.</p>

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Spin-state regulation of high-entropy Ruddlesden-Popper perovskite oxides for efficient seawater electrolysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月9日

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  • Yifan Liu,
  • Libin Hao,
  • Caichao Ye,
  • Yin Huang,
  • Jing Jin,
  • Mingming Gong,
  • Long Chen,
  • Jingwen Sun,
  • Li Shi,
  • Jingnan Wang,
  • Wei Xu,
  • Wenqing Zhang,
  • Xin Wang,
  • Pan Xiong,
  • Junwu Zhu

摘要

High-entropy oxides have emerged as a promising group of candidates for various catalytic fields, including seawater electrolysis. However, without rational understanding and guidance, designing multielement compositions for high-entropy systems and elucidating the synergistic effect of diverse elements in catalysis remain significant challenges. Herein, we report spin-state regulation of a high-entropy Ruddlesden–Popper perovskite oxide for efficient seawater electrolysis. The Cu2+ and Mn3+ with Jahn-Teller effect induced a transition of Fe3+/Co3+ spin state from low spin to high spin configuration. The high spin Fe3+/Co3+ favor OH− adsorption and deprotonation during seawater oxidation. Besides, the oxygen intermediates adsorbed on high spin active sites repel the Cl− ions. Consequently, (La0.76Sr0.24)3(Fe0.22Co0.21Ni0.18Cu0.17Mn0.22)2O7 achieved robust seawater oxidation for over 1200 h at 200 mA cm−2, showing competitive performance. The anion exchange membrane electrolyzer coupling with (La0.76Sr0.24)3(Fe0.22Co0.21Ni0.18Cu0.17Mn0.22)2O7 anode and Pt/C cathode could maintain the seawater splitting performance of 1 A cm−2 at 1.76 V and incessantly operate for 800 h. This spin-engineered strategy is universal to other high-entropy perovskite oxides and spinel oxides, offering promising way for designing efficient high-entropy catalysts.