Fe-Nx/C electrocatalysts synthesized by pyrolysis of Fe(II)-2,3,5,6-tetra(2-pyridyl)pyrazine complex for PEM fuel cell oxygen reduction reaction

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DOIResolve DOI: http://doi.org/10.1016/j.electacta.2011.03.059
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TypeArticle
Journal titleElectrochimica Acta
ISSN0013-4686
Volume56
Issue13
Pages47444752; # of pages: 9
SubjectCarbon-supported non-noble metal electrocatalysts; Iron-nitrogen complex; Methanol tolerance; Oxygen reduction reaction; PEM fuel cell; Pyrazines; Catalyst activity; Chemical analysis; Electrocatalysts; Electrochemical electrodes; Electrolytic reduction; Electron transitions; Electron transport properties; Iron compounds; Kinetic parameters; Methanol; Oxygen; Precious metals; Proton exchange membrane fuel cells (PEMFC); Pyrolysis; Rate constants; Rotating disks; X ray diffraction; Catalyst supports
Abstract2,3,5,6-Tetra(2-pyridyl)pyrazine (TPPZ) was employed as a ligand to prepare an iron(II) complex (Fe-TPPZ) that served as a precursor to synthesize carbon-supported catalysts (Fe-Nx/C) through heat-treatment at 600, 700, 800 and 900 °C under N2 atmosphere. Both the structure and composition of the synthesized Fe-Nx/C were analyzed by X-ray diffraction and energy-dispersive X-ray microanalysis, respectively. The rotating disk and ring-disk electrode measurements showed that these catalysts have strong ORR activity with an overall 4-electron transfer process through a (2 + 2)-electron transfer mechanism, which was assigned to the catalytic function of the Fe-Nx center. A study on the heat-treatment temperature on the ORR activity showed that 800 °C is the optimal temperature for the synthesized catalysts. Furthermore, the effect of both catalyst and Nafion® ionomer loadings in the catalyst layer on the corresponding ORR activity was also investigated. The kinetic parameters such as the chemical reaction rate between O2 and Fe-Nx/C (adduct formation reaction), the rate constant for the rate-determining step (RDS), and the electron numbers in the ORR, were obtained. The methanol tolerance of the catalyst was also tested. To validate the ORR activity, a membrane electrode assembly in which the cathode catalyst layer contained Fe-Nx/C was constructed and tested in a real fuel cell. The results obtained are encouraging when compared with similar non-noble catalysts. © 2011 Elsevier Ltd. All rights reserved.
Publication date
LanguageEnglish
AffiliationNational Research Council Canada (NRC-CNRC); NRC Institute for Fuel Cell Innovation (IFCI-IIPC)
Peer reviewedYes
NPARC number21271547
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Record identifier46fff3ae-2492-4c17-bc66-1aa51454522f
Record created2014-03-24
Record modified2016-05-09
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