journal article·2024-10Open access

Electron Transfer from Encapsulated Fe3C to the Outermost N‐Doped Carbon Layer for Superior ORR

Javier Quílez‐Bermejo, Ayoub Daouli, Sergio García Dalí, Yingdan Cui, Andrea Zitolo, Jimena Castro‐Gutiérrez, Mélanie Emo, Maria T. Izquierdo, William Mustain, Michael Badawi, Alain Celzard, Vanessa Fierro

Advanced Functional Materials· Volume 34· Issue 40

Abstract

Abstract Encapsulating Fe3C in carbon layers has emerged as an innovative strategy for protecting Fe3C while preserving its high oxygen reduction activity. However, fundamental questions persist regarding the active sites of encapsulated Fe3C due to the restricted accessibility of oxygen molecules to the metal sites. Herein, the intrinsic electron transfer mechanisms of Fe3C nanoparticles encapsulated in N‐doped carbon materials are unveiled for oxygen reduction electrocatalysis. The precision‐structured C1N1 material is used to synthesize N‐doped carbons with encapsulated Fe3C, significantly enhancing catalytic activity (EONSET = 0.98 V) and achieving near‐100% operational stability. In anion‐exchange membrane fuel cells, an excellent peak power density of 830 mW cm−2 is reached at 60 °C. The experimental and computational results revealed that the presence of Fe3C cores dynamically triggers electron transfer to the outermost carbon layer. This phenomenon amplifies the oxygen reduction reaction performance at N sites, contributing significantly to the observed catalytic enhancement.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Fuel Cells and Related Materials · Semiconductor materials and devices

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

Affiliations

Université de Lorraine Centre National de la Recherche Scientifique (CNRS) Institut Jean Lamour (IJL) Épinal F‐88000 France

Université de Lorraine Centre National de la Recherche Scientifique (CNRS) Laboratoire de Physique et Chimie Théoriques (LPCT) Nancy F‐54000 France

Departamento de Ciencia de los Materiales e Ingeniería Metalúrgica Universidad de Oviedo Oviedo 33004 Spain

Department of Chemical Engineering University of South Carolina Columbia SC 29208 USA

Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology Kowloon Hong Kong 999077 China

Synchrotron SOLEIL Départementale 128 Saint Aubin F‐91190 France

Université de Lorraine Centre National de la Recherche Scientifique (CNRS) Institut Jean Lamour (IJL) Nancy F‐54011 France

Instituto de Carboquímica (ICB‐CSIC) Miguel Luesma Castán 4 Zaragoza E‐50018 Spain

Université de Lorraine Centre National de la Recherche Scientifique (CNRS) Laboratoire Lorrain de Chimie Moléculaire (L2CM) Metz F‐57000 France

Institut Universitaire de France (IUF) Paris F‐75231 France

Funding

Ministerio de Universidades · Conseil régional du Grand Est · European Regional Development Fund · Agence Nationale de la Recherche

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