Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction
Abstract While Fe–N–C materials have shown promising initial oxygen reduction reaction (ORR) activity, they lack durability in acidic medium. Key degradation mechanisms include FeN4 site demetallation and deactivation by reactive oxygen species. Here we show for mainstream Fe–N–Cs that adding 1 wt.%...
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Nature Portfolio
2025-07-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-61806-x |
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| author | Nicolas A. Ishiki Keyla Teixeira Santos Nicolas Bibent Kavita Kumar Ina Reichmann Yu-Ping Ku Tristan Asset Laetitia Dubau Michel Mermoux Hongxin Ge Sandrine Berthon-Fabry Viktoriia A. Saveleva Vinod K. Paidi Pieter Glatzel Andrea Zitolo Tzonka Mineva Hazar Guesmi Serhiy Cherevko Edson A. Ticianelli Frédéric Maillard Frédéric Jaouen |
| author_facet | Nicolas A. Ishiki Keyla Teixeira Santos Nicolas Bibent Kavita Kumar Ina Reichmann Yu-Ping Ku Tristan Asset Laetitia Dubau Michel Mermoux Hongxin Ge Sandrine Berthon-Fabry Viktoriia A. Saveleva Vinod K. Paidi Pieter Glatzel Andrea Zitolo Tzonka Mineva Hazar Guesmi Serhiy Cherevko Edson A. Ticianelli Frédéric Maillard Frédéric Jaouen |
| author_sort | Nicolas A. Ishiki |
| collection | DOAJ |
| description | Abstract While Fe–N–C materials have shown promising initial oxygen reduction reaction (ORR) activity, they lack durability in acidic medium. Key degradation mechanisms include FeN4 site demetallation and deactivation by reactive oxygen species. Here we show for mainstream Fe–N–Cs that adding 1 wt.% Pt nanoparticles via a soft polyol method results in well-defined and stable Pt/Fe–N–C hybrids. The Pt addition strongly reduces the H2O2 production and Fe leaching rate during ORR, while post mortem Mössbauer spectroscopy reveals that the highly active but unstable Fe(III)N4 site is partially stabilized. The similar H2O2 electroreduction activity of Pt/Fe–N–C and Fe–N–C and other analyses point toward a long-distance electronic effect of Pt nanoparticles in stabilizing FeN4 sites. Computational chemistry reveals that spin polarization of distant Pt atoms mitigates the structural changes of FeN4 sites upon adsorption of oxygenated species atop Fe, especially in high-spin state. |
| format | Article |
| id | doaj-art-2a8e99edc4954a918c8202709fb04b60 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-2a8e99edc4954a918c8202709fb04b602025-08-20T04:02:57ZengNature PortfolioNature Communications2041-17232025-07-0116111510.1038/s41467-025-61806-xEvidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reductionNicolas A. Ishiki0Keyla Teixeira Santos1Nicolas Bibent2Kavita Kumar3Ina Reichmann4Yu-Ping Ku5Tristan Asset6Laetitia Dubau7Michel Mermoux8Hongxin Ge9Sandrine Berthon-Fabry10Viktoriia A. Saveleva11Vinod K. Paidi12Pieter Glatzel13Andrea Zitolo14Tzonka Mineva15Hazar Guesmi16Serhiy Cherevko17Edson A. Ticianelli18Frédéric Maillard19Frédéric Jaouen20Univ. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMIUniv. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMIICGM, Univ. Montpellier, CNRS, ENSCM, 1919 route de MendeUniv. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMIForschungszentrum Jülich GmbH, Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IET-2), Cauerstraße 1Forschungszentrum Jülich GmbH, Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IET-2), Cauerstraße 1ICGM, Univ. Montpellier, CNRS, ENSCM, 1919 route de MendeUniv. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMIUniv. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMIMINES Paris, PSL University PERSEE - Centre procédés, énergies renouvelables et systèmes énergétiques, CS 10207 rue Claude DaunesseMINES Paris, PSL University PERSEE - Centre procédés, énergies renouvelables et systèmes énergétiques, CS 10207 rue Claude DaunesseESRF, The European Synchrotron, 71 Avenue des MartyrsESRF, The European Synchrotron, 71 Avenue des MartyrsESRF, The European Synchrotron, 71 Avenue des MartyrsSynchrotron SOLEIL, L’Orme des Merisiers, BP 48 Saint AubinICGM, Univ. Montpellier, CNRS, ENSCM, 1919 route de MendeICGM, Univ. Montpellier, CNRS, ENSCM, 1919 route de MendeForschungszentrum Jülich GmbH, Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IET-2), Cauerstraße 1Instituto de Química de São Carlos (IQSC), Universidade de São Paulo, Av. Trabalhador São-Carlense, 400, CP 780Univ. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMIICGM, Univ. Montpellier, CNRS, ENSCM, 1919 route de MendeAbstract While Fe–N–C materials have shown promising initial oxygen reduction reaction (ORR) activity, they lack durability in acidic medium. Key degradation mechanisms include FeN4 site demetallation and deactivation by reactive oxygen species. Here we show for mainstream Fe–N–Cs that adding 1 wt.% Pt nanoparticles via a soft polyol method results in well-defined and stable Pt/Fe–N–C hybrids. The Pt addition strongly reduces the H2O2 production and Fe leaching rate during ORR, while post mortem Mössbauer spectroscopy reveals that the highly active but unstable Fe(III)N4 site is partially stabilized. The similar H2O2 electroreduction activity of Pt/Fe–N–C and Fe–N–C and other analyses point toward a long-distance electronic effect of Pt nanoparticles in stabilizing FeN4 sites. Computational chemistry reveals that spin polarization of distant Pt atoms mitigates the structural changes of FeN4 sites upon adsorption of oxygenated species atop Fe, especially in high-spin state.https://doi.org/10.1038/s41467-025-61806-x |
| spellingShingle | Nicolas A. Ishiki Keyla Teixeira Santos Nicolas Bibent Kavita Kumar Ina Reichmann Yu-Ping Ku Tristan Asset Laetitia Dubau Michel Mermoux Hongxin Ge Sandrine Berthon-Fabry Viktoriia A. Saveleva Vinod K. Paidi Pieter Glatzel Andrea Zitolo Tzonka Mineva Hazar Guesmi Serhiy Cherevko Edson A. Ticianelli Frédéric Maillard Frédéric Jaouen Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction Nature Communications |
| title | Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction |
| title_full | Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction |
| title_fullStr | Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction |
| title_full_unstemmed | Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction |
| title_short | Evidence for the stabilization of FeN4 sites by Pt particles during acidic oxygen reduction |
| title_sort | evidence for the stabilization of fen4 sites by pt particles during acidic oxygen reduction |
| url | https://doi.org/10.1038/s41467-025-61806-x |
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