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Peer-reviewedCC BY 4.0Chemistry (Weinheim an Der Bergstrasse, Germany)

Efficient Light‐Driven Multi‐Electron Accumulation on Viologens by Molecular Control Over Photochemical Reaction Pathways

  • Fatemeh Sousani1
  • Georgina E. Shillito2
  • Alexander K. Mengele1
  • Martin D. Hager3,4,5,6,7
  • Ulrich S. Schubert3,4,5,6,7
  • Stefanie Gräfe2,8
  • Stephan Kupfer2
  • Sven Rau1
8 affiliations
  1. 1Institute of Inorganic Chemistry Ulm University Ulm Germany
  2. 2Institute of Physical Chemistry and Abbe Center of Photonics Friedrich Schiller University Jena Jena Germany
  3. 3Laboratory of Organic and Macromolecular Chemistry (IOMC) Friedrich Schiller University Jena Jena Germany
  4. 4Jena Center for Soft Matter (JCSM) Friedrich Schiller University Jena Jena Germany
  5. 5Center For Energy and Environmental Chemistry Jena (CEEC Jena) Friedrich Schiller University Jena Jena Germany
  6. 6Helmholtz Institute for Polymers in Energy Applications Jena (HIPOLE Jena) Jena Germany
  7. 7Helmholtz Zentrum für Materialien Und Energie Berlin (HZB) Berlin Germany
  8. 8Fraunhofer Institute for Applied Optics and Precision Engineering Jena Germany
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Abstract

Achieving multiple photo‐induced charge accumulations on the same acceptor is one option to propel photochemical reactions that demand highly reducing or oxidizing conditions. By switching the initial light‐driven process from an oxidative to a reductive quenching pathway via mutual redox potential control over Ru(II) polypyridyl chromophores and sacrificial electron donors (SEDs), acceleration of complete single electron reduction of methyl viologen (MV2+) and polymer‐bound viologens by a factor of up to 2,200 as well as a rapid subsequent second reduction of MV•+ to MV0 was achieved in homogeneous solution. Ab initio molecular dynamics (AIMD) allowed the conformer space to be mapped and to shed light on the thermodynamics of the photochemical intermediates involved in the formation of the two‐electron reduced methyl viologen (MV0). These results provide a toolbox of structurally simple compounds for the modular construction of efficient artificial photosynthesis schemes.

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Cite

BibTeXRIS
BibTeX
@article{sousani2026efficient,
  title = {{Efficient Light‐Driven Multi‐Electron Accumulation on Viologens by Molecular Control Over Photochemical Reaction Pathways}},
  author = {Fatemeh Sousani and Georgina E. Shillito and Alexander K. Mengele and Martin D. Hager and Ulrich S. Schubert and Stefanie Gräfe and Stephan Kupfer and Sven Rau},
  journal = {Chemistry (Weinheim an Der Bergstrasse, Germany)},
  year = {2026},
  month = jul,
  doi = {10.1002/chem.71467},
  url = {https://doi.org/10.1002/chem.71467},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Efficient Light‐Driven Multi‐Electron Accumulation on Viologens by Molecular Control Over Photochemical Reaction Pathways
AU  - Fatemeh Sousani
AU  - Georgina E. Shillito
AU  - Alexander K. Mengele
AU  - Martin D. Hager
AU  - Ulrich S. Schubert
AU  - Stefanie Gräfe
AU  - Stephan Kupfer
AU  - Sven Rau
PY  - 2026
DA  - 2026/07/30
JO  - Chemistry (Weinheim an Der Bergstrasse, Germany)
DO  - 10.1002/chem.71467
UR  - https://doi.org/10.1002/chem.71467
AB  - Achieving multiple photo‐induced charge accumulations on the same acceptor is one option to propel photochemical reactions that demand highly reducing or oxidizing conditions. By switching the initial light‐driven process from an oxidative to a reductive quenching pathway via mutual redox potential control over Ru(II) polypyridyl chromophores and sacrificial electron donors (SEDs), acceleration of complete single electron reduction of methyl viologen (MV2+) and polymer‐bound viologens by a factor of up to 2,200 as well as a rapid subsequent second reduction of MV•+ to MV0 was achieved in homogeneous solution. Ab initio molecular dynamics (AIMD) allowed the conformer space to be mapped and to shed light on the thermodynamics of the photochemical intermediates involved in the formation of the two‐electron reduced methyl viologen (MV0). These results provide a toolbox of structurally simple compounds for the modular construction of efficient artificial photosynthesis schemes.
SN  - 0947-6539
SN  - 1521-3765
ER  -