Charge-Polarized Lanthanide Coordination Strategy Enables Activity-Stability Synergy in Rare Earth-Tailored Metallene Electrocatalysts
The development of durable electrocatalysts that overcome activity-stability compromises remains pivotal for advancing anion-exchange membrane fuel cells (AEMFCs). Herein, a rare earth-incorporated Pd-based metallene (PdLaCe) is engineered 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.