Reconstructed parallel sites enhance the reactive oxygen tolerance of non-noble metal catalyst for durable proton exchange membrane fuel cells  

作　　者：Wenjie Wang Hui Ding Minghao Wang Han Cheng Xiang Shi Lin Wang Chun Wang Wangsheng Chu Yi Xie Changzheng Wu 

机构地区：[1]School of Chemistry and Materials Science,CAS Center for Excellence in Nanoscience,University of Science&Technology of China,Hefei 230026,China [2]National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China [3]Institute of Energy,Hefei Comprehensive National Science Center,Hefei 230029,China [4]Zhejiang Institute of Photoelectronics,Jinhua 321004,China

出　　处：《Science China Chemistry》2024年第11期3739-3748,共10页中国科学（化学英文版）

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)。

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.

关 键 词：parallel reaction pathways sites reconstruction oxygen reduction reaction radical elimination fuel cells 

分 类 号：TM911.4[电气工程—电力电子与电力传动] O643.36[理学—物理化学]