[FeFe]-hydrogenase mimic with organic photosensitizers for long-lived excited states and efficient photocatalytic H2 production
Year: 2025
Type: article
Abstract: We report a [FeFe]-hydrogenase mimic complex bearing two organic photosensitizers ( PS-CAT , C 70 H 44 Fe 2 N 2 O 6 S 6 ) aimed at achieving superior light-absorbing properties. PS-CAT is a dyad with two light-harvesting moieties ( PS ) and one catalytic center ( CAT ). The present study investigates the electro- and photo-reduction properties of PS-CAT , combining experimental and theoretical approaches to achieve a comprehensive understanding of the (photo)reduction mechanism of the dyad. To this aim, PS-CAT was studied by means of cyclic voltammetry, IR-spectroelectrochemistry, nanosecond-transient absorption, and scalar relativistic-time-dependent-density functional theory. The results reveal that the dyad can access the photo-excited state with a large absorption coefficient due to multiple PSs. Moreover, the PS-CAT produced long-lived excited species with a ligand-centered or charge-separated character by photon absorption. The subsequent quenching can produce the catalytically active reduced species. Furthermore, the photocatalytic activities of PS-CAT under visible light irradiation were examined, and the PS-CAT exhibited high efficiency (turnover frequency 33 h −1 ) of H 2 generation as a PS -bearing [FeFe]-H 2 ase mimic.
Source: Cell Reports Physical Science
Authors: Chizuru Kasahara, Micheal K. Farh, Katharina Rediger, Philipp Buday, Stefanie Gräfe, Mathias Micheel, Stephan Kupfer, Maria Wächtler, Wolfgang Weigand
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $5,620
OpenAlex ID: W7106501124