A Covalent Organic Framework for Cooperative Water Oxidation
Zitieren Sie bitte immer diese URN: urn:nbn:de:bvb:20-opus-287591
- The future of water-derived hydrogen as the “sustainable energy source” straightaway bets on the success of the sluggish oxygen-generating half-reaction. The endeavor to emulate the natural photosystem II for efficient water oxidation has been extended across the spectrum of organic and inorganic combinations. However, the achievement has so far been restricted to homogeneous catalysts rather than their pristine heterogeneous forms. The poor structural understanding and control over the mechanistic pathway often impede the overall development.The future of water-derived hydrogen as the “sustainable energy source” straightaway bets on the success of the sluggish oxygen-generating half-reaction. The endeavor to emulate the natural photosystem II for efficient water oxidation has been extended across the spectrum of organic and inorganic combinations. However, the achievement has so far been restricted to homogeneous catalysts rather than their pristine heterogeneous forms. The poor structural understanding and control over the mechanistic pathway often impede the overall development. Herein, we have synthesized a highly crystalline covalent organic framework (COF) for chemical and photochemical water oxidation. The interpenetrated structure assures the catalyst stability, as the catalyst’s performance remains unaltered after several cycles. This COF exhibits the highest ever accomplished catalytic activity for such an organometallic crystalline solid-state material where the rate of oxygen evolution is as high as ∼26,000 μmol L\(^{–1}\) s\(^{–1}\) (second-order rate constant k ≈ 1650 μmol L s\(^{–1}\) g\(^{–2}\)). The catalyst also proves its exceptional activity (k ≈ 1600 μmol L s\(^{–1}\) g\(^{–2}\)) during light-driven water oxidation under very dilute conditions. The cooperative interaction between metal centers in the crystalline network offers 20–30-fold superior activity during chemical as well as photocatalytic water oxidation as compared to its amorphous polymeric counterpart.…
Autor(en): | Suvendu Karak, Vladimir Stepanenko, Matthew A. AddicoatORCiD, Philipp Keßler, Simon Moser, Florian Beuerle, Frank WürthnerORCiDGND |
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URN: | urn:nbn:de:bvb:20-opus-287591 |
Dokumentart: | Artikel / Aufsatz in einer Zeitschrift |
Institute der Universität: | Fakultät für Physik und Astronomie / Physikalisches Institut |
Fakultät für Chemie und Pharmazie / Institut für Organische Chemie | |
Sprache der Veröffentlichung: | Englisch |
Titel des übergeordneten Werkes / der Zeitschrift (Englisch): | Journal of the American Chemical Society |
ISSN: | 0002-7863 |
Erscheinungsjahr: | 2022 |
Band / Jahrgang: | 144 |
Heft / Ausgabe: | 38 |
Seitenangabe: | 17661–17670 |
URL der Erstveröffentlichung: | https://pubs.acs.org/doi/10.1021/jacs.2c07282 |
DOI: | https://doi.org/10.1021/jacs.2c07282 |
Allgemeine fachliche Zuordnung (DDC-Klassifikation): | 5 Naturwissenschaften und Mathematik / 54 Chemie / 547 Organische Chemie |
Freie Schlagwort(e): | catalysis; catalyst; covalent organic framework; crystalline; nanoparticles; sustainable energy source; water oxidation |
Datum der Freischaltung: | 29.09.2022 |
EU-Projektnummer / Contract (GA) number: | 787937 |
OpenAIRE: | OpenAIRE |
Lizenz (Deutsch): | CC BY-NC-ND: Creative-Commons-Lizenz: Namensnennung, Nicht kommerziell, Keine Bearbeitungen 4.0 International |