摘要
The establishment of reactive oxygen species(ROS) elimination sites in iron-nitrogen-carbon(Fe-N-C) electrocatalysts to achieve durable proton-exchange membrane fuel cells(PEMFCs) performance has attracted broad interest. However, realizing ROS removal efficiency and oxygen reduction reaction(ORR) activity within a single system represents a significant challenge to date. Herein, we demonstrate uniform ROS elimination sites and ORR centers through an electrochemical reconstruction method on the parallel sites of Fe@Ce NC electrocatalyst for durable PEMFC. During the reconstruction process, the Fe sites can retain their original configuration. Meanwhile, the pristine Ce clusters will evolve into more efficient, highly dispersed sites.Furthermore, the reconstructed Fe and Ce sites exhibit favorable energy barriers for the ORR and ROS elimination pathways,respectively, thereby maintaining ORR activity and achieving high ROS tolerance. Consequently, the PEMFC assembled with our catalyst shows only a 2% decay in power density after the accelerated durability test. We anticipate that this parallel structure design will provide new insight into the development of more durable electrocatalysts for PEMFCs.
基金
supported by the National Key R&D Program of China (2022YFA1502903)
the National Natural Science Foundation of China (21925110, 22201274, 21890750, 52130202, 12175234)
the University Synergy Innovation Program of Anhui Province (GXXT-2022-007)
the support from the Major/Innovative Program of Development Foundation of the Hefei Center for Physical Science and Technology
the support from the beamline 1W1B at the Beijing Synchrotron Radiation Facility (BSRF, Beijing, China)
the BL14W1 and BL11B beamlines at the Shanghai Synchrotron Radiation Facility (SSRF, Shanghai China)
the beamlines BL11U, BL10B, and BL12B of National Synchrotron Radiation Laboratory (NSRL, Hefei, China)。