Details
Originalsprache | Englisch |
---|---|
Aufsatznummer | e202400303 |
Fachzeitschrift | CHEMSUSCHEM |
Jahrgang | 17 |
Ausgabenummer | 17 |
Frühes Online-Datum | 20 März 2024 |
Publikationsstatus | Veröffentlicht - 9 Sept. 2024 |
Extern publiziert | Ja |
Abstract
Advanced in situ analyses are indispensable for comprehending the catalyst aging mechanisms of Pt-based PEM fuel cell cathode materials, particularly during accelerated stress tests (ASTs). In this study, a combination of in situ small-angle and wide-angle X-ray scattering (SAXS & WAXS) techniques were employed to establish correlations between structural parameters (crystal phase, quantity, and size) of a highly active skeleton-PtCo (sk-PtCo) catalyst and their degradation cycles within the potential range of the start-up/shut-down (SUSD) conditions. Despite the complex case of the sk-PtCo catalyst comprising two distinct fcc alloy phases, our complementary techniques enabled in situ monitoring of structural changes in each crystal phase in detail. Remarkably, the in situ WAXS measurements uncover two primary catalyst aging processes, namely the cobalt depletion (regime I) followed by the crystallite growth via Ostwald ripening and/or particle coalescence (regime II). Additionally, in situ SAXS data reveal a continuous size growth over the AST. The Pt-enriched shell thickening based on the Co depletion within the first 100 SUSD cycles and particle growth induced by additional potential cycles were also collaborated by ex situ STEM-EELS. Overall, our work shows a comprehensive aging model for the sk-PtCo catalyst probed by complementary in situ WAXS and SAXS techniques.
ASJC Scopus Sachgebiete
- Umweltwissenschaften (insg.)
- Umweltchemie
- Chemische Verfahrenstechnik (insg.)
- Werkstoffwissenschaften (insg.)
- Energie (insg.)
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in: CHEMSUSCHEM, Jahrgang 17, Nr. 17, e202400303, 09.09.2024.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review
}
TY - JOUR
T1 - Monitoring the Morphological Changes of Skeleton-PtCo Electrocatalyst during PEMFC Start-Up/Shut-Downprobed by in situ WAXS and SAXS
AU - Janssen, Marek
AU - Drnec, Jakub
AU - Martens, Isaac
AU - Quinson, Jonathan
AU - Pittkowski, Rebecca
AU - Park, Daesung
AU - Weber, Philipp
AU - Arenz, Matthias
AU - Oezaslan, Mehtap
N1 - Publisher Copyright: © 2024 The Authors. ChemSusChem published by Wiley-VCH GmbH.
PY - 2024/9/9
Y1 - 2024/9/9
N2 - Advanced in situ analyses are indispensable for comprehending the catalyst aging mechanisms of Pt-based PEM fuel cell cathode materials, particularly during accelerated stress tests (ASTs). In this study, a combination of in situ small-angle and wide-angle X-ray scattering (SAXS & WAXS) techniques were employed to establish correlations between structural parameters (crystal phase, quantity, and size) of a highly active skeleton-PtCo (sk-PtCo) catalyst and their degradation cycles within the potential range of the start-up/shut-down (SUSD) conditions. Despite the complex case of the sk-PtCo catalyst comprising two distinct fcc alloy phases, our complementary techniques enabled in situ monitoring of structural changes in each crystal phase in detail. Remarkably, the in situ WAXS measurements uncover two primary catalyst aging processes, namely the cobalt depletion (regime I) followed by the crystallite growth via Ostwald ripening and/or particle coalescence (regime II). Additionally, in situ SAXS data reveal a continuous size growth over the AST. The Pt-enriched shell thickening based on the Co depletion within the first 100 SUSD cycles and particle growth induced by additional potential cycles were also collaborated by ex situ STEM-EELS. Overall, our work shows a comprehensive aging model for the sk-PtCo catalyst probed by complementary in situ WAXS and SAXS techniques.
AB - Advanced in situ analyses are indispensable for comprehending the catalyst aging mechanisms of Pt-based PEM fuel cell cathode materials, particularly during accelerated stress tests (ASTs). In this study, a combination of in situ small-angle and wide-angle X-ray scattering (SAXS & WAXS) techniques were employed to establish correlations between structural parameters (crystal phase, quantity, and size) of a highly active skeleton-PtCo (sk-PtCo) catalyst and their degradation cycles within the potential range of the start-up/shut-down (SUSD) conditions. Despite the complex case of the sk-PtCo catalyst comprising two distinct fcc alloy phases, our complementary techniques enabled in situ monitoring of structural changes in each crystal phase in detail. Remarkably, the in situ WAXS measurements uncover two primary catalyst aging processes, namely the cobalt depletion (regime I) followed by the crystallite growth via Ostwald ripening and/or particle coalescence (regime II). Additionally, in situ SAXS data reveal a continuous size growth over the AST. The Pt-enriched shell thickening based on the Co depletion within the first 100 SUSD cycles and particle growth induced by additional potential cycles were also collaborated by ex situ STEM-EELS. Overall, our work shows a comprehensive aging model for the sk-PtCo catalyst probed by complementary in situ WAXS and SAXS techniques.
KW - accelerated stress test (AST)
KW - oxygen reduction reaction (ORR)
KW - skeleton-PtCo nanoparticles (NPs)
KW - small-angle X-ray scattering (SAXS)
KW - start-up/shut-down (SUSD)
KW - wide-angle X-ray scattering (WAXS)
UR - http://www.scopus.com/inward/record.url?scp=85190597680&partnerID=8YFLogxK
U2 - 10.1002/cssc.202400303
DO - 10.1002/cssc.202400303
M3 - Article
AN - SCOPUS:85190597680
VL - 17
JO - CHEMSUSCHEM
JF - CHEMSUSCHEM
SN - 1864-5631
IS - 17
M1 - e202400303
ER -