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<p>Developing highly active, low-cost, and durable catalysts for efficient oxygen reduction reactions remain a challenge, hindering the commercial viability of proton exchange membrane fuel cells (PEMFCs). In this study, an ordered PtZnFeCoNiCr high-entropy intermetallic electrocatalyst with Pt antisite point defects (PD-PZFCNC-HEI) is synthesized. The electrocatalyst shows high mass activity of 4.12 A mg<sub>Pt</sub><sup>-1</sup> toward the oxygen reduction reaction (ORR), which is 33 times that of the commercial Pt/C. PEMFC, assembled with PD-PZFCNC-HEI as the cathode (0.05 mg<sub>Pt</sub> cm<sup>-2</sup>), exhibits a peak power density of 1.9 W cm<sup>-2</sup> and a high mass activity of 3.0 A mg<sub>Pt</sub><sup>-1</sup> at 0.9 V. Theoretical calculations combined with in situ X-ray absorption fine structure results reveal that defect engineering optimizes Pt’s electronic structure and activates non-noble metal site active centers, achieving exceptionally high ORR catalytic activity. This study provides guidance for the development of nanostructured ordered high-entropy intermetallic catalysts.</p>

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Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月7日

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  • Tao Chen,
  • Xinkai Zhang,
  • Hangchao Wang,
  • Chonglin Yuan,
  • Yuxuan Zuo,
  • Chuan Gao,
  • Wukun Xiao,
  • Yue Yu,
  • Junfei Cai,
  • Tie Luo,
  • Yan Xiang,
  • Dingguo Xia

摘要

Developing highly active, low-cost, and durable catalysts for efficient oxygen reduction reactions remain a challenge, hindering the commercial viability of proton exchange membrane fuel cells (PEMFCs). In this study, an ordered PtZnFeCoNiCr high-entropy intermetallic electrocatalyst with Pt antisite point defects (PD-PZFCNC-HEI) is synthesized. The electrocatalyst shows high mass activity of 4.12 A mgPt-1 toward the oxygen reduction reaction (ORR), which is 33 times that of the commercial Pt/C. PEMFC, assembled with PD-PZFCNC-HEI as the cathode (0.05 mgPt cm-2), exhibits a peak power density of 1.9 W cm-2 and a high mass activity of 3.0 A mgPt-1 at 0.9 V. Theoretical calculations combined with in situ X-ray absorption fine structure results reveal that defect engineering optimizes Pt’s electronic structure and activates non-noble metal site active centers, achieving exceptionally high ORR catalytic activity. This study provides guidance for the development of nanostructured ordered high-entropy intermetallic catalysts.