Stabilizing High‐Activity FeN <sub>5</sub> Sites via an Adaptive N‐linked Carbon Bilayer for Stable Fuel Cells
Abstract
ABSTRACT The practical application of Fe‐N‐C catalysts in proton exchange membrane fuel cells is fundamentally constrained by the inherent activity‐stability trade‐off. Here, we propose a “repair‐and‐upgrade” engineering strategy that not only repairs pyrolysis‐induced defects through carbon and nitrogen supplementation but also evolves conventional FeN 4 moieties into stabilized FeN 5 configurations via an in situ constructed carbon bilayer. The axial nitrogen modulates the electronic structure of Fe center to enhance catalytic activity, while the adaptive interlayer spacing of the N‐linked carbon bilayer compensates for fluctuations in the axial Fe─N bond length during catalysis, therefore anchoring the Fe active sites. When integrated into membrane electrode assemblies, the catalyst delivers a high peak power density of 1221 mW cm −2 and exhibits exceptional durability, retaining over 85% of its initial power density after 10,000 cycles in H 2 ‐O 2 and showing negligible decay over 45 h at 0.6 V in H 2 ‐air tests. This work presents a novel design strategy for stable single‐atom catalysts, centered on creating an adaptive local environment that ensures exceptional electrocatalytic stability.
Article Details
Authors (14)
Long‐Ji Yuan
Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advanced Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen China
Zhen‐Yu Miao
State Key Laboratory of Space Power‐Sources MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage MOE Engineering Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang China
Qi Li
Yu‐Zhe Liu
Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advanced Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen China
Tao Gong
Zhao‐Yang Han
Guangdong Hebei Key Laboratory of Applied Chemistry School of Environmental and Chemical Engineering Yanshan University Qinhuangdao China
Wei Gong
Li‐Xiao Shen
Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advanced Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen China
Wen‐Liang Feng
Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advanced Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen China
Bin Wu
Shu‐Rong Yuan
Intelligent Power Station Technology Research&Development Department Xian XD Switchgear Electric Co., Ltd Shaanxi China
Guo‐Xu Zhang
State Key Laboratory of Space Power‐Sources MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage MOE Engineering Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang China
Xu‐Lei Sui
Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advanced Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen China
Zhen‐Bo Wang
State Key Laboratory of Space Power‐Sources MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage MOE Engineering Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin China