Impact of carbon N-doping and pyridinic-N content on the fuel cell performance and durability of carbon-supported Pt nanoparticle catalysts

dc.contributor.authorHornberger, Elisabeth
dc.contributor.authorMerzdorf, Thomas
dc.contributor.authorSchmies, Henrike
dc.contributor.authorHübner, Jessica
dc.contributor.authorKlingenhof, Malte
dc.contributor.authorGernert, Ulrich
dc.contributor.authorKroschel, Matthias
dc.contributor.authorAnke, Björn
dc.contributor.authorLerch, Martin
dc.contributor.authorSchmidt, Johannes
dc.contributor.authorThomas, Arne
dc.contributor.authorChattot, Raphaël
dc.contributor.authorMartens, Isaac
dc.contributor.authorDrnec, Jakub
dc.contributor.authorStrasser, Peter
dc.date.accessioned2022-09-07T14:02:30Z
dc.date.available2022-09-07T14:02:30Z
dc.date.issued2022-04-13
dc.description.abstractCathode catalyst layers of proton exchange membrane fuel cells (PEMFCs) typically consist of carbon-supported platinum catalysts with varying weight ratios of proton-conducting ionomers. N-Doping of carbon support materials is proposed to enhance the performance and durability of the cathode layer under operating conditions in a PEMFC. However, a detailed understanding of the contributing N-moieties is missing. Here, we report the successful synthesis and fuel cell implementation of Pt electrocatalysts supported on N-doped carbons, with a focus on the analysis of the N-induced effect on catalyst performance and durability. A customized fluidized bed reduction reactor was used to synthesize highly monodisperse Pt nanoparticles deposited on N-doped carbons (N–C), the catalytic oxygen reduction reaction activity and stability of which matched those of state-of-the-art PEMFC catalysts. Operando high-energy X-ray diffraction experiments were conducted using a fourth generation storage ring; the light of extreme brilliance and coherence allows investigating the impact of N-doping on the degradation behavior of the Pt/N–C catalysts. Tests in liquid electrolytes were compared with tests in membrane electrode assemblies in single-cell PEMFCs. Our analysis refines earlier views on the subject of N-doped carbon catalyst supports: it provides evidence that heteroatom doping and thus the incorporation of defects into the carbon backbone do not mitigate the carbon corrosion during high-potential cycling (1–1.5 V) and, however, can promote the cell performance under usual PEMFC operating conditions (0.6–0.9 V).en
dc.description.sponsorshipBMBF, 03XP0251, KorrZellKat - Korrosionsresistente Katalysator- und Trägermaterialien für Niedertemperatur PEM Brennstoffzellkathodenen
dc.description.sponsorshipBMBF, 03SF0531B, Verbundvorhaben HT-linked: Hochleistungsfähige und alterungsstabile HT-PEMFC Membranelektrodeneinheiten durch neue Anbindungskonzepte Katalysator/Träger/Protonenleiter. Teilvorhaben: Präparation und in-situ Chararakterisierung von katalytischen Nanopartikeln auf funktionalisierten Trägernen
dc.identifier.eissn1944-8252
dc.identifier.issn1944-8244
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/17384
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-16165
dc.language.isoenen
dc.relation.ispartof10.14279/depositonce-16177en
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subject.ddc540 Chemie und zugeordnete Wissenschaftende
dc.subject.otherfuel cellen
dc.subject.otheroxygen reduction reactionen
dc.subject.otherelectrocatalysten
dc.subject.otherN-doped carbonen
dc.subject.otheroperando HE-XRDen
dc.subject.otherMEAen
dc.titleImpact of carbon N-doping and pyridinic-N content on the fuel cell performance and durability of carbon-supported Pt nanoparticle catalystsen
dc.typeArticleen
dc.type.versionacceptedVersionen
dcterms.bibliographicCitation.doi10.1021/acsami.2c00762en
dcterms.bibliographicCitation.issue16en
dcterms.bibliographicCitation.journaltitleACS Applied Materials & Interfacesen
dcterms.bibliographicCitation.originalpublishernameAmerican Chemical Societyen
dcterms.bibliographicCitation.originalpublisherplaceWashington, DCen
dcterms.bibliographicCitation.pageend18430en
dcterms.bibliographicCitation.pagestart18420en
dcterms.bibliographicCitation.volume14en
tub.accessrights.dnbdomain*
tub.affiliationFak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Anorganische Chemie - Festkörper- und Materialchemiede
tub.affiliation.facultyFak. 2 Mathematik und Naturwissenschaftende
tub.affiliation.groupFG Anorganische Chemie - Festkörper- und Materialchemiede
tub.affiliation.instituteInst. Chemiede
tub.publisher.universityorinstitutionTechnische Universität Berlinen

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