Luo, Fang ; Wagner, Stephan ; Ju, Wen ; Primbs, Mathias ; Li, Shuang ; Wang, Huan ; Kramm, Ulrike I. ; Strasser, Peter (2022)
Kinetic diagnostics and synthetic design of platinum group metal-free electrocatalysts for the oxygen reduction reaction using reactivity maps and site utilization descriptors.
In: Journal of the American Society, 144 (30)
doi: 10.1021/jacs.2c01594
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The experimental development of catalytically ever-more active platinum group metal (PGM)-free materials for the oxygen reduction reaction (ORR) at fuel cell cathodes has been until recently a rather empirical iteration of synthesis and testing. Here, we present how kinetic reactivity maps based on kinetic descriptors of PGM-free single-metal-site ORR electrocatalysts can help to better understand the origin of catalytic reactivity and help to derive rational synthetic guidelines toward improved catalysts. Key in our analysis are the catalytic surface site density (SD) and the catalytic turnover frequency (TOF) in their role as controlling kinetic parameters for the ORR reactivity of PGM-free nitrogen-coordinated single-metal M-site carbon (MNC) catalysts. SD-TOF plots establish two-dimensional reactivity maps. We also consider the ratio between SD and the total number of single-metal sites in the bulk, referred to as the site utilization factor, which we propose as another guiding parameter for optimizing the synthesis of MNC catalysts. Exemplified by two sets of FeNC, CoNC, and SnNC catalysts prepared using two distinctly different N- and C-precursor material classes (Zn-based zeolitic imidazolate frameworks and covalent polyaniline), we comparatively diagnose the intrinsic kinetic ORR parameters as well as structural, morphological, and chemical properties. From there, we derive and discuss possible synthetic guidelines for further improvements. Our approach can be extended to other families of catalysts and may involve kinetic performance data of idealized liquid-electrolyte cells as well as gas diffusion layer-type flow cells.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2022 |
| Autor(en): | Luo, Fang ; Wagner, Stephan ; Ju, Wen ; Primbs, Mathias ; Li, Shuang ; Wang, Huan ; Kramm, Ulrike I. ; Strasser, Peter |
| Art des Eintrags: | Bibliographie |
| Titel: | Kinetic diagnostics and synthetic design of platinum group metal-free electrocatalysts for the oxygen reduction reaction using reactivity maps and site utilization descriptors |
| Sprache: | Englisch |
| Publikationsjahr: | Juli 2022 |
| Verlag: | ACS Publications |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Journal of the American Society |
| Jahrgang/Volume einer Zeitschrift: | 144 |
| (Heft-)Nummer: | 30 |
| DOI: | 10.1021/jacs.2c01594 |
| Kurzbeschreibung (Abstract): | The experimental development of catalytically ever-more active platinum group metal (PGM)-free materials for the oxygen reduction reaction (ORR) at fuel cell cathodes has been until recently a rather empirical iteration of synthesis and testing. Here, we present how kinetic reactivity maps based on kinetic descriptors of PGM-free single-metal-site ORR electrocatalysts can help to better understand the origin of catalytic reactivity and help to derive rational synthetic guidelines toward improved catalysts. Key in our analysis are the catalytic surface site density (SD) and the catalytic turnover frequency (TOF) in their role as controlling kinetic parameters for the ORR reactivity of PGM-free nitrogen-coordinated single-metal M-site carbon (MNC) catalysts. SD-TOF plots establish two-dimensional reactivity maps. We also consider the ratio between SD and the total number of single-metal sites in the bulk, referred to as the site utilization factor, which we propose as another guiding parameter for optimizing the synthesis of MNC catalysts. Exemplified by two sets of FeNC, CoNC, and SnNC catalysts prepared using two distinctly different N- and C-precursor material classes (Zn-based zeolitic imidazolate frameworks and covalent polyaniline), we comparatively diagnose the intrinsic kinetic ORR parameters as well as structural, morphological, and chemical properties. From there, we derive and discuss possible synthetic guidelines for further improvements. Our approach can be extended to other families of catalysts and may involve kinetic performance data of idealized liquid-electrolyte cells as well as gas diffusion layer-type flow cells. |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Anorganische Chemie > Fachgruppe Katalysatoren und Elektrokatalysatoren 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Anorganische Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut |
| Hinterlegungsdatum: | 07 Mai 2024 06:02 |
| Letzte Änderung: | 07 Mai 2024 08:52 |
| PPN: | 51791493X |
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