Bimodal multiphoton catalysis via structural regeneration

Abstract Most of the current photocatalytic methodologies for the generation of reactive radical intermediates have limited redox windows and can operate within a single redox manifold. Here, to overcome these constraints, we report a purely organic photocatalyst that operates via a two-photon excitation mechanism, enabling both oxidative and reductive transformations within a unified platform. Upon visible-light irradiation, the molecule undergoes reversible fragmentation into three reactive subunits spanning a 5.7 V redox window. These fragments orchestrate an unusual consecutive light-induced electron-transfer mechanism that enables the orthogonal activation of thermodynamically challenging substrates. The mechanistic scenario is revealed through a combination of spectroscopic and optical techniques, supported by quantum calculations. Selectivity is mainly governed by the activity of a transiently generated catalytic species, whose presence prevents the need for external radical-sorting agents. Finally, the generality of this light-driven radical-coupling reactivity is demonstrated across a broad range of structurally diverse substrates.

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Publication Details

Journal
Nature Catalysis
Published
2026-08-14
DOI
https://doi.org/10.1038/s41929-026-01593-w
Primary Topic
Radical Photochemical Reactions
Type
article
Field-Weighted Citation Impact
0.00

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article

Bimodal multiphoton catalysis via structural regeneration

Giorgio Pelosi, Luca Dell’Amico, Giovanni Bistoni, Federico Droghetti et al.
Nature Catalysis
Radical Photochemical Reactions
article

Bimodal multiphoton catalysis via structural regeneration

Giorgio Pelosi, Luca Dell’Amico, Giovanni Bistoni, Federico Droghetti, Cristian Rosso, Giorgia Barison, Marco Bortolus, Mirco Natali, Elisabetta Collini, Paolo Costa, Andrea Sartorel, Stefano Visentini, Nicola Michelazzo, Alessia Marrese, Sofia Lerda, Vittoria Burigana, Sara Bonacchi
article en

Abstract

Abstract Most of the current photocatalytic methodologies for the generation of reactive radical intermediates have limited redox windows and can operate within a single redox manifold. Here, to overcome these constraints, we report a purely organic photocatalyst that operates via a two-photon excitation mechanism, enabling both oxidative and reductive transformations within a unified platform. Upon visible-light irradiation, the molecule undergoes reversible fragmentation into three reactive subunits spanning a 5.7 V redox window. These fragments orchestrate an unusual consecutive light-induced electron-transfer mechanism that enables the orthogonal activation of thermodynamically challenging substrates. The mechanistic scenario is revealed through a combination of spectroscopic and optical techniques, supported by quantum calculations. Selectivity is mainly governed by the activity of a transiently generated catalytic species, whose presence prevents the need for external radical-sorting agents. Finally, the generality of this light-driven radical-coupling reactivity is demonstrated across a broad range of structurally diverse substrates.

Nature Catalysis
University of Parma (IT), University of Padua (IT), University of Ferrara (IT), University of Perugia (IT)
Università degli Studi di Padova, Horizon 2020 Framework Programme
Life in Land
Openalex Percentile: Top 18%
Radical Photochemical Reactions
DOIOpen Access PDFOpenAlex
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