Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy
In the past, platinum–copper catalysts have proven to be highly active for the oxygen reduction reaction (ORR), but transferring the high activities measured in thin-film rotating disk electrodes (TF-RDEs) to high-performing membrane electrode assemblies (MEAs) has proven difficult due to stability...
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MDPI AG
2023-05-01
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| Online Access: | https://www.mdpi.com/1996-1944/16/9/3544 |
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| author | Maximilian Grandi Matija Gatalo Ana Rebeka Kamšek Gregor Kapun Kurt Mayer Francisco Ruiz-Zepeda Martin Šala Bernhard Marius Marjan Bele Nejc Hodnik Merit Bodner Miran Gaberšček Viktor Hacker |
| author_facet | Maximilian Grandi Matija Gatalo Ana Rebeka Kamšek Gregor Kapun Kurt Mayer Francisco Ruiz-Zepeda Martin Šala Bernhard Marius Marjan Bele Nejc Hodnik Merit Bodner Miran Gaberšček Viktor Hacker |
| author_sort | Maximilian Grandi |
| collection | DOAJ |
| description | In the past, platinum–copper catalysts have proven to be highly active for the oxygen reduction reaction (ORR), but transferring the high activities measured in thin-film rotating disk electrodes (TF-RDEs) to high-performing membrane electrode assemblies (MEAs) has proven difficult due to stability issues during operation. High initial performance can be achieved. However, fast performance decay on a timescale of 24 h is induced by repeated voltage load steps with H<sub>2</sub>/air supplied. This performance decay is accelerated if high relative humidity (>60% RH) is set for a prolonged time and low voltages are applied during polarization. The reasons and possible solutions for this issue have been investigated by means of electrochemical impedance spectroscopy and distribution of relaxation time analysis (EIS–DRT). The affected electrochemical sub-processes have been identified by comparing the PtCu electrocatalyst with commercial Pt/C benchmark materials in homemade catalyst-coated membranes (CCMs). The proton transport resistance (<i>R</i><sub>pt</sub>) increased by a factor of ~2 compared to the benchmark materials. These results provide important insight into the challenges encountered with the de-alloyed PtCu/KB electrocatalyst during cell break-in and operation. This provides a basis for improvements in the catalysts’ design and break-in procedures for the highly attractive PtCu/KB catalyst system. |
| first_indexed | 2024-03-11T04:13:38Z |
| format | Article |
| id | doaj.art-dfe97e33e29e4ca2a8154498b4a03b66 |
| institution | Directory Open Access Journal |
| issn | 1996-1944 |
| language | English |
| last_indexed | 2024-03-11T04:13:38Z |
| publishDate | 2023-05-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Materials |
| spelling | doaj.art-dfe97e33e29e4ca2a8154498b4a03b662023-11-17T23:17:31ZengMDPI AGMaterials1996-19442023-05-01169354410.3390/ma16093544Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance SpectroscopyMaximilian Grandi0Matija Gatalo1Ana Rebeka Kamšek2Gregor Kapun3Kurt Mayer4Francisco Ruiz-Zepeda5Martin Šala6Bernhard Marius7Marjan Bele8Nejc Hodnik9Merit Bodner10Miran Gaberšček11Viktor Hacker12Institute of Chemical Engineering and Environmental Technology, Graz University of Technology, Inffeldgasse 25/C, 8010 Graz, AustriaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaInstitute of Chemical Engineering and Environmental Technology, Graz University of Technology, Inffeldgasse 25/C, 8010 Graz, AustriaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaDepartment of Analytical Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaInstitute of Chemical Engineering and Environmental Technology, Graz University of Technology, Inffeldgasse 25/C, 8010 Graz, AustriaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaInstitute of Chemical Engineering and Environmental Technology, Graz University of Technology, Inffeldgasse 25/C, 8010 Graz, AustriaDepartment of Materials Chemistry, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, SloveniaInstitute of Chemical Engineering and Environmental Technology, Graz University of Technology, Inffeldgasse 25/C, 8010 Graz, AustriaIn the past, platinum–copper catalysts have proven to be highly active for the oxygen reduction reaction (ORR), but transferring the high activities measured in thin-film rotating disk electrodes (TF-RDEs) to high-performing membrane electrode assemblies (MEAs) has proven difficult due to stability issues during operation. High initial performance can be achieved. However, fast performance decay on a timescale of 24 h is induced by repeated voltage load steps with H<sub>2</sub>/air supplied. This performance decay is accelerated if high relative humidity (>60% RH) is set for a prolonged time and low voltages are applied during polarization. The reasons and possible solutions for this issue have been investigated by means of electrochemical impedance spectroscopy and distribution of relaxation time analysis (EIS–DRT). The affected electrochemical sub-processes have been identified by comparing the PtCu electrocatalyst with commercial Pt/C benchmark materials in homemade catalyst-coated membranes (CCMs). The proton transport resistance (<i>R</i><sub>pt</sub>) increased by a factor of ~2 compared to the benchmark materials. These results provide important insight into the challenges encountered with the de-alloyed PtCu/KB electrocatalyst during cell break-in and operation. This provides a basis for improvements in the catalysts’ design and break-in procedures for the highly attractive PtCu/KB catalyst system.https://www.mdpi.com/1996-1944/16/9/3544PEFCcatalyst layerplatinum–copperdegradationionomerelectrochemical impedance spectroscopy |
| spellingShingle | Maximilian Grandi Matija Gatalo Ana Rebeka Kamšek Gregor Kapun Kurt Mayer Francisco Ruiz-Zepeda Martin Šala Bernhard Marius Marjan Bele Nejc Hodnik Merit Bodner Miran Gaberšček Viktor Hacker Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy Materials PEFC catalyst layer platinum–copper degradation ionomer electrochemical impedance spectroscopy |
| title | Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy |
| title_full | Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy |
| title_fullStr | Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy |
| title_full_unstemmed | Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy |
| title_short | Mechanistic Study of Fast Performance Decay of PtCu Alloy-based Catalyst Layers for Polymer Electrolyte Fuel Cells through Electrochemical Impedance Spectroscopy |
| title_sort | mechanistic study of fast performance decay of ptcu alloy based catalyst layers for polymer electrolyte fuel cells through electrochemical impedance spectroscopy |
| topic | PEFC catalyst layer platinum–copper degradation ionomer electrochemical impedance spectroscopy |
| url | https://www.mdpi.com/1996-1944/16/9/3544 |
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