High‐Spin Pt Sites of Intermetallic Compound via Pinning Effect Boost Oxygen Reduction Performance
Abstract
ABSTRACT The commercialization of proton exchange membrane fuel cells (PEMFCs) is hindered by sluggish oxygen reduction reaction (ORR) kinetics at the cathode, demanding high‐performance Pt‐based catalysts. The ORR efficiency is critically governed by the spin configuration of Pt sites, yet regulating Pt spin states remains challenging due to their inherently paramagnetic nature. Here, we report core–shell L1 0 ‐Pt 2 CoFe/Pt 2 FeNi intermetallic compounds that achieve stable high‐spin Pt sites via a spin‐pinning effect. The remanent magnetization of the ferromagnetic core induces a persistent high‐spin configuration in the Pt shell after external magnetic field removal. This spin‐engineering strategy optimizes Pt 5d orbital splitting, lowering the activation barrier for electron transfer to O 2 and facilitating its activation. Magnetized L1 0 ‐Pt 2 CoFe exhibits 8‐fold higher mass activity and 31‐fold higher specific activity than its nonmagnetized counterpart, outperforming commercial Pt/C. The catalyst also retains 90% of its initial activity after 50 000 cycles and maintains performance after 6 months of storage, demonstrating excellent stability. This field‐free spin‐pinning strategy offers a practical, generalizable route to designing advanced Pt‐based ORR catalysts.
Article Details
Authors (26)
Renjie Gui
State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science
Yifan Yin
Han Cheng
State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science
Junxiang Wang
Yi Tan
State Key Laboratory of Bioactive Molecules and Druggability Assessment, and School of Pharmacy, Jinan University, 601 Huangpu Avenue West, Guangzhou 510632, China
Min Ge
The Instruments Center for Physical Science
Huijuan Wang
Zhou Pan
Molecular Synthesis Center & Key Laboratory of Marine Drugs, Chinese Ministry of Education, School of Medicine and Pharmacy Ocean University of China Qingdao China
Zuyuan Zhang
Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science University of Science and Technology of China Hefei Anhui P. R. China
Minghao Wang
State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science
Huijuan Zhang
Department of Oncology The Affiliated Yantai Yuhuangding Hospital of Qingdao University Medical College Yantai China
Xuemin Cao
Caijie Su
Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science University of Science and Technology of China Hefei Anhui P. R. China
Chen Chen
Yumeng Bian
Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science University of Science and Technology of China Hefei Anhui P. R. China
Yangjun Lou
Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science University of Science and Technology of China Hefei Anhui P. R. China
Xuguang Liu
Instruments Center for Physical Science University of Science and Technology of China Hefei China
Jing Peng
Min Zhou
Gongming Wang
State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science
Wangsheng Chu
National Synchrotron Radiation Laboratory
Haifeng Lv
Yue Lin
Xiaojun Wu
Yi Xie
Changzheng Wu
State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science