Precisely Designed Morphology and Surface Chemical Structure of Fe-N-C Electrocatalysts for Enhanced Oxygen Reaction Reduction Activity

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Abstract
Fe-N-C materials have been regarded as one of the potential candidates to replace traditional noble-metal-based electrocatalysts for the oxygen reduction reaction (ORR). It is believed that the structure of carbon support in Fe-N-C materials plays an essential role in highly efficient ORR. However, precisely designing the morphology and surface chemical structure of carbon support remains a challenge. Herein, we present a novel synthetic strategy for the preparation of porous carbon spheres (PCSs) with high specific surface area, well-defined pore structure, tunable morphology and controllable heteroatom doping. The synthesis involves Schiff-based polymerization utilizing octaaminophenyl polyhedral oligomeric silsesquioxane (POSS-NH2) and heteroatom-containing aldehydes, followed by pyrolysis and HF etching. The well-defined pore structure of PCS can provide the confinement field for ferroin and transform into Fe-N-C sites after carbonization. The tunable morphology of PCS can be easily achieved by changing the solvents. The surface chemical structure of PCS can be tailored by utilizing different heteroatom-containing aldehydes. After optimizing the structure of PCS, Fe-N-C loading on N,S-codoped porous carbon sphere (NSPCS-Fe) displays outstanding ORR activity in alkaline solution. This work paves a new path for fabrication of Fe-N-C materials with the desired morphology and well-designed surface chemical structure, demonstrating significant potential for energy-related applications.
Funding Information
  • Guangxi Science and Technology Base and Talent Special Project (AD22035007, 2024GXNSFBA010237, 2022KY0424, 20243202, 2021KYQD04)
  • Guangxi Natural Science Foundation of China (AD22035007, 2024GXNSFBA010237, 2022KY0424, 20243202, 2021KYQD04)
  • Guangxi Enhancing Young and Middle-aged Teacher’s Research Basis Ability (AD22035007, 2024GXNSFBA010237, 2022KY0424, 20243202, 2021KYQD04)
  • Marine Science Program for Guangxi First-Class Discipline, Beibu Gulf University (AD22035007, 2024GXNSFBA010237, 2022KY0424, 20243202, 2021KYQD04)
  • high-level talent start up project of Beibu Gulf University (AD22035007, 2024GXNSFBA010237, 2022KY0424, 20243202, 2021KYQD04)

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