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 meta...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 dualdoping induces charge polarization to generate Pd^(δ-)-La/Ce^(δ+)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 industrialscale fuel cell applications.This work provides transformative strategies for next-generation energy conversion systems requiring high efficiency and ultra-stability.展开更多
基金supported by the National Natural Science Foundation of China(12204253,52502102,22502229)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB430039,24KJB150026)+3 种基金the Distinguished Young Scholars Fund of Jiangsu Province(BK20220061)the Training Programs of Innovation for Undergraduates(202510304023)the Collaborative Innovation Center of Suzhou Nano Science and Technologythe Large Instruments Open Foundation of Nantong University(KFJN2526)。
文摘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 dualdoping induces charge polarization to generate Pd^(δ-)-La/Ce^(δ+)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 industrialscale fuel cell applications.This work provides transformative strategies for next-generation energy conversion systems requiring high efficiency and ultra-stability.
