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<p>A largely unexplored approach for optimizing surface strains on terrace-type catalysts is the break of atomic symmetry to release surface stress. The key challenge lies in how to implement this approach into practical nanocatalysts, in particular the promising high-entropy alloys (HEAs). Herein, we design and synthesize a series of HEA nanorings (NRs) with abundant terrace-type defects for oxygen reduction reaction (ORR) electrocatalysis. The asymmetry-triggered release of surface stress enables the modulation of compressive strain for optimizing the electronic structure. On the optimally-tuned PtPdFeCoNi HEA NRs, we achieve mass and specific activities of 0.99 A mg<sup>-1</sup><sub>platinum group metal (PGM)</sub> and 1.32 mA cm<sup>-2</sup><sub>PGM</sub> at 0.95 V versus reversible hydrogen electrode (vs. RHE), demonstrating a competitive performance. Experimental and theoretical investigations unveil that the stress-released compressive strain lowers the <i>d</i>-band center of Pt sites in HEA NRs, resulting in favorable desorption of oxygenated intermediates and thus accelerated ORR kinetics.</p>

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Breaking the symmetry of high-entropy alloy surfaces for compressively strain-tuned oxygen reduction reaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月2日

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  • Lin He,
  • Menggang Li,
  • Longyu Qiu,
  • Xue Ren,
  • Fenyang Tian,
  • Jie Sheng,
  • Yequn Liu,
  • Mingchuan Luo,
  • Xin Zhou,
  • Yongsheng Yu,
  • Weiwei Yang,
  • Shaojun Guo

摘要

A largely unexplored approach for optimizing surface strains on terrace-type catalysts is the break of atomic symmetry to release surface stress. The key challenge lies in how to implement this approach into practical nanocatalysts, in particular the promising high-entropy alloys (HEAs). Herein, we design and synthesize a series of HEA nanorings (NRs) with abundant terrace-type defects for oxygen reduction reaction (ORR) electrocatalysis. The asymmetry-triggered release of surface stress enables the modulation of compressive strain for optimizing the electronic structure. On the optimally-tuned PtPdFeCoNi HEA NRs, we achieve mass and specific activities of 0.99 A mg-1platinum group metal (PGM) and 1.32 mA cm-2PGM at 0.95 V versus reversible hydrogen electrode (vs. RHE), demonstrating a competitive performance. Experimental and theoretical investigations unveil that the stress-released compressive strain lowers the d-band center of Pt sites in HEA NRs, resulting in favorable desorption of oxygenated intermediates and thus accelerated ORR kinetics.