Scholarlink

<p>Maximizing metal-substrate interactions by self-reconstruction of coadjutant metastable phases can be a delicate strategy to obtain robust and efficient high-density single-atom catalysts. Here, we prepare high-density iridium atoms embedded ultrathin CoCeOOH nanosheets (CoCe-O-Ir<sub>SA</sub>) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH)<sub>2</sub> substrates. The CoCe-O-Ir<sub>SA</sub> delivers an overpotential of 187 mV at 100 mA cm<sup>−2</sup> and a steady lifespan of 1000 h at 500 mA cm<sup>−2</sup> for oxygen evolution reaction. Furthermore, the CoCe-O-Ir<sub>SA</sub> is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm<sup>−2</sup> for 150 h. Operando experimental and theoretical calculation results demonstrate that the reconstructed thermodynamically stable iridium single atoms act as highly active sites by regulating charge redistribution with strongly <i>p</i>-<i>d</i>-<i>f</i> orbital couplings, enabling electron transfer facilitated, the adsorption energies of intermediates optimized, and the surface reactivity of Co/Ce sites activated, leading to high oxygen evolution performance. These results open up an approach for engineering metastable phases to realize stable single-atom systems under ambient conditions toward efficient energy-conversion applications.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Atomic-scale self-rearrangement of hetero-metastable phases into high-density single-atom catalysts for the oxygen evolution reaction

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年3月25日

查看全文
  • Quan Quan,
  • Yuxuan Zhang,
  • Haifan Li,
  • Wei Wang,
  • Pengshan Xie,
  • Dong Chen,
  • Weijun Wang,
  • You Meng,
  • Di Yin,
  • Yezhan Li,
  • Dongyuan Song,
  • Lijie Chen,
  • Shaohai Li,
  • Cheng Yang,
  • Takeshi Yanagida,
  • Chun-Yuen Wong,
  • SenPo Yip,
  • Johnny C. Ho

摘要

Maximizing metal-substrate interactions by self-reconstruction of coadjutant metastable phases can be a delicate strategy to obtain robust and efficient high-density single-atom catalysts. Here, we prepare high-density iridium atoms embedded ultrathin CoCeOOH nanosheets (CoCe-O-IrSA) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH)2 substrates. The CoCe-O-IrSA delivers an overpotential of 187 mV at 100 mA cm−2 and a steady lifespan of 1000 h at 500 mA cm−2 for oxygen evolution reaction. Furthermore, the CoCe-O-IrSA is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm−2 for 150 h. Operando experimental and theoretical calculation results demonstrate that the reconstructed thermodynamically stable iridium single atoms act as highly active sites by regulating charge redistribution with strongly p-d-f orbital couplings, enabling electron transfer facilitated, the adsorption energies of intermediates optimized, and the surface reactivity of Co/Ce sites activated, leading to high oxygen evolution performance. These results open up an approach for engineering metastable phases to realize stable single-atom systems under ambient conditions toward efficient energy-conversion applications.