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<p>The development of durable electrocatalysts overcoming activity-stability compromises remains pivotal for advancing anion-exchange membrane fuel cells (AEMFCs). Herein, we engineer a rare earth-incorporated Pd-based metallene (PdLaCe) through lanthanide-based bimetallic coordination, resolving critical limitations in oxygen reduction reaction (ORR) catalysis. Combined experimental characterization and theoretical simulations reveal that La/Ce dual-doping induces charge polarization to generate Pd<sup><i>δ</i>−</sup>-La/Ce<sup><i>δ</i>+</sup> active sites, synergistically optimizing the electronic structure via d-band center downshifting. This configuration weakens oxygen intermediate adsorption while enhancing structural integrity across thermal cycles. The optimized PdLaCe metallene delivers exceptional ORR performance, achieving a record half-wave potential of 0.903 V (vs. RHE) with negligible degradation (&lt;6%) after 20,000 cycles, far surpassing commercial Pt/C benchmarks. Integrated into AEMFCs, it demonstrates a peak power density of 82.8 mW cm<sup>−2</sup> alongside unprecedented stability (0.8 V for 22 h). Fundamental insights into lanthanide-induced charge redistribution establish a universal paradigm for designing robust multimetallic electrocatalysts via rare earth coordination engineering, bridging critical gaps between functional optimization and industrial-scale fuel cell applications. This work provides transformative strategies for next-generation energy conversion systems requiring high efficiency and ultra-stability.</p>

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Charge-polarized lanthanide coordination strategy enables activity-stability synergy in rare earth-tailored metallene electrocatalysts

  • 期刊论文

  • 发表日期：

    2025年9月16日

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  • Tianheng Du,
  • Sijie Chen,
  • Xianzhe Zhao,
  • Xueheng Liu,
  • Lifang Zhang,
  • Xi Zhou,
  • Linbo Li,
  • Tongfei Li,
  • Tao Qian

摘要

The development of durable electrocatalysts overcoming activity-stability compromises remains pivotal for advancing anion-exchange membrane fuel cells (AEMFCs). Herein, we engineer a rare earth-incorporated Pd-based metallene (PdLaCe) through lanthanide-based bimetallic coordination, resolving critical limitations in oxygen reduction reaction (ORR) catalysis. Combined experimental characterization and theoretical simulations reveal that La/Ce dual-doping induces charge polarization to generate Pdδ−-La/Ceδ+ active sites, synergistically optimizing the electronic structure via d-band center downshifting. This configuration weakens oxygen intermediate adsorption while enhancing structural integrity across thermal cycles. The optimized PdLaCe metallene delivers exceptional ORR performance, achieving a record half-wave potential of 0.903 V (vs. RHE) with negligible degradation (<6%) after 20,000 cycles, far surpassing commercial Pt/C benchmarks. Integrated into AEMFCs, it demonstrates a peak power density of 82.8 mW cm−2 alongside unprecedented stability (0.8 V for 22 h). Fundamental insights into lanthanide-induced charge redistribution establish a universal paradigm for designing robust multimetallic electrocatalysts via rare earth coordination engineering, bridging critical gaps between functional optimization and industrial-scale fuel cell applications. This work provides transformative strategies for next-generation energy conversion systems requiring high efficiency and ultra-stability.