<p>The rational design of low-Pd catalysts for the oxygen reduction reaction (ORR) remains a central challenge toward cost-effective fuel cell technologies. Here, we report a multiwalled carbon nanotubes supported binary CoPd catalyst with an ultralow Pd loading of only 5 wt% and abundant oxygen vacancies in CoO domains (denoted as CoPd-O<sup>V</sup>). As prepared CoPd-O<sup>V</sup> catalyst delivers an impressive half-wave potential (E<sub>1/2</sub>) of 0.883&#xa0;V versus RHE and a kinetic current density (J<sub>K</sub>) of 12.35&#xa0;mA cm<sup>−2</sup> in alkaline ORR (0.1&#xa0;M KOH), significantly surpassing the benchmark J.M.-Pt/C catalyst wit 20 wt% Pt loading (E<sub>1/2</sub> = 0.844&#xa0;V vs. RHE, J<sub>k</sub> = 4.37&#xa0;mA cm<sup>−2</sup>). In situ X-ray absorption spectroscopy (XAS) at the Co K-edge reveals that oxygen vacancies in CoO promote O<sub>2</sub> bond activation and splitting, while the neighboring Pd domains facilitate the subsequent hydration step through a strong electron relocation effect from Co-to-Pd. A control CoPd catalyst with similar Pd content but lacking oxygen vacancies shows markedly suppressed ORR activity, confirming the synergistic role of O<sup>V</sup>s and Pd. These findings establish a powerful strategy for engineering vacancy–metal interfaces, enabling high-performance ORR electrocatalysis at minimal noble metal cost.</p>

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Heterogeneous CoO–Pd interface along with oxygen vacancies boosts the oxygen reduction reaction performance of Pd nanoparticles

  • Amisha Beniwal,
  • Sajana Pooniya,
  • V. R. Libin,
  • Hariom Gurjar,
  • Khushabu Shekhawat,
  • Ashima Bagaria,
  • Dinesh Bhalothia

摘要

The rational design of low-Pd catalysts for the oxygen reduction reaction (ORR) remains a central challenge toward cost-effective fuel cell technologies. Here, we report a multiwalled carbon nanotubes supported binary CoPd catalyst with an ultralow Pd loading of only 5 wt% and abundant oxygen vacancies in CoO domains (denoted as CoPd-OV). As prepared CoPd-OV catalyst delivers an impressive half-wave potential (E1/2) of 0.883 V versus RHE and a kinetic current density (JK) of 12.35 mA cm−2 in alkaline ORR (0.1 M KOH), significantly surpassing the benchmark J.M.-Pt/C catalyst wit 20 wt% Pt loading (E1/2 = 0.844 V vs. RHE, Jk = 4.37 mA cm−2). In situ X-ray absorption spectroscopy (XAS) at the Co K-edge reveals that oxygen vacancies in CoO promote O2 bond activation and splitting, while the neighboring Pd domains facilitate the subsequent hydration step through a strong electron relocation effect from Co-to-Pd. A control CoPd catalyst with similar Pd content but lacking oxygen vacancies shows markedly suppressed ORR activity, confirming the synergistic role of OVs and Pd. These findings establish a powerful strategy for engineering vacancy–metal interfaces, enabling high-performance ORR electrocatalysis at minimal noble metal cost.