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Falling, Lorenz J. ; Jang, Woosun ; Laha, Sourav ; Götsch, Thomas ; Terban, Maxwell W. ; Bette, Sebastian ; Mom, Rik ; Velasco-Vélez, Juan-Jesús ; Girgsdies, Frank ; Teschner, Detre ; Tarasov, Andrey ; Chuang, Cheng-Hao ; Lunkenbein, Thomas ; Knop-Gericke, Axel ; Weber, Daniel ; Dinnebier, Robert ; Lotsch, Bettina V. ; Schlögl, Robert ; Jones, Travis E.:
Atomic Insights into the Competitive Edge of Nanosheets Splitting Water.
In: Journal of the American Chemical Society.
Bd. 146
(2024)
Heft 40
.
- S. 27886-27902.
ISSN 1520-5126
DOI: https://doi.org/10.1021/jacs.4c10312
Abstract
The oxygen evolution reaction (OER) provides the protons for many electrocatalytic power-to-X processes, such as the production of green hydrogen from water or methanol from CO2. Iridium oxohydroxides (IOHs) are outstanding catalysts for this reaction because they strike a unique balance between activity and stability in acidic electrolytes. Within IOHs, this balance varies with the atomic structure. While amorphous IOHs perform best, they are least stable. The opposite is true for their crystalline counterparts. These rules-of-thumb are used to reduce the loading of scarce IOH catalysts and retain the performance. However, it is not fully understood how activity and stability are related at the atomic level, hampering rational design. Herein, we provide simple design rules (Figure 12) derived from the literature and various IOHs within this study. We chose crystalline IrOOH nanosheets as our lead material because they provide excellent catalyst utilization and a predictable structure. We found that IrOOH signals the chemical stability of crystalline IOHs while surpassing the activity of amorphous IOHs. Their dense bonding network of pyramidal trivalent oxygens (mu(3 Delta)-O) provides structural integrity, while allowing reversible reduction to an electronically gapped state that diminishes the destructive effect of reductive potentials. The reactivity originates from coordinative unsaturated edge sites with radical character, i.e., mu 1-O oxyls. By comparing to other IOHs and literature, we generalized our findings and synthesized a set of simple rules that allow prediction of stability and reactivity of IOHs from atomistic models. We hope that these rules will inspire atomic design strategies for future OER catalysts.
Weitere Angaben
| Publikationsform: | Artikel in einer Zeitschrift |
|---|---|
| Begutachteter Beitrag: | Ja |
| Zusätzliche Informationen: | WOS:001320396200001 |
| Institutionen der Universität: | Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie |
| Titel an der UBT entstanden: | Nein |
| Themengebiete aus DDC: | 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Eingestellt am: | 12 Jun 2025 08:07 |
| Letzte Änderung: | 12 Jun 2025 08:07 |
| URI: | https://eref.uni-bayreuth.de/id/eprint/93657 |