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journal article·2026-01Open access

Rational Design of Asymmetric FeN 3 S Single‐Atom Sites for e g Orbital Engineering Toward Efficient ORR in PEMFCs

Chengjie Chen, Xin Lai, Yongqi Jian, Dengke Zhang, Wenyu Huang, Jian Chen, Fangyan Xie, Yanshuo Jin, Ming‐Hsien Lee, Guixiang Li, Nan Wang, Hui Meng, Mohammad Khaja Nazeeruddin

Small· Volume 22· Issue 2
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Source abstract

Abstract

Abstract Iron and nitrogen co‐doped FeNC catalysts with symmetric Fe‐N 4 as the active site are the most promising alternative to noble metal catalysts for proton exchange membrane fuel cells (PEMFCs). However, the symmetric structure in the Fe–N 4 site endows oxygen intermediates with strong binding energy, which hinders the activity optimization of the active center. In this work, an asymmetric configuration (Fe‐N 3 SC) is constructed to alleviate the electron localization caused by the d – π conjugation of Fe‐N 4 . The asymmetric configuration can effectively reduce the splitting energy of the Fe‐3d orbital, leading to a decrease in the energy barrier for the electrons to fill in the e g orbitals. Increased electron occupancy in the e g orbitals reduces the bond order/adsorption of the oxygen‐containing intermediates on the active site, which leads to increased oxygen reduction (ORR) activity. The results of this work highlight the possibility of asymmetric configurations in manipulating and optimizing electron transfer and spin regulation of single‐atom catalysts.
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Research context

Catalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · Metal-Catalyzed Oxygenation Mechanisms · Fuel Cells and Related Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Siyuan laboratory Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy Materials Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials Guangdong Provincial Key Laboratory of Nanophotonic Manipulation Department of Physics Jinan University Guangzhou 510632 P. R. China

State Key Laboratory of Organic‐Inorganic Composites Beijing University of Chemical Technology Beijing 100029 P. R. China

Instrumental Analysis & Research Center Sun Yat‐sen University Guangzhou Guangdong 510275 P. R. China

Department of Physics Tamkang University New Taipei 25137 Taiwan

School of Materials Science and Engineering Southeast University Nanjing Jiangsu 211189 P. R. China

Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne (EPFL) Lausanne CH‐1015 Switzerland

Funding

National Natural Science Foundation of China · Basic and Applied Basic Research Foundation of Guangdong Province

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