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Integrating a Triplet-triplet Annihilation Up-conversion System to Enhance Dye-sensitized Solar Cell Response to Sub-bandgap Light
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Luminescent Fe(III) Complex Sensitizes Aerobic Photon Upconversion and Initiates Photocatalytic Radical
Pengyue Jin1, Xinhuan Xu2, Yongli Yan2
1Department of Biology and Chemistry, Osnabrück University, Barbarastraße 7, Osnabrück 49076, Germany.
Journal of the American Chemical Society
|December 10, 2024
Summary
This study demonstrates efficient green-to-blue photon upconversion using an iron photosensitizer and anthracene derivatives. This iron-based system enables controlled radical polymerization with visible light, offering a sustainable alternative to precious metals.
Area of Science:
- Inorganic Chemistry
- Photochemistry
- Polymer Science
Background:
- Precious metal-based photosensitizers are crucial for light energy conversion but are costly.
- Iron complexes offer a sustainable alternative, yet their short excited-state lifetimes limit applications.
- Developing efficient iron-based photosensitizers is vital for sustainable energy technologies.
Purpose of the Study:
- To investigate doublet-triplet energy transfer for photosensitization in iron complexes.
- To achieve efficient triplet-triplet annihilation upconversion (TTAUC) using an iron(III) photosensitizer.
- To demonstrate the application of iron-photosensitized upconversion in photoredox catalysis for polymer synthesis.
Main Methods:
- Utilized a luminescent Fe(III) complex as a photosensitizer.
- Employed anthracene derivatives, specifically 9,10-diphenylanthracene (DPA), as the annihilator.
- Investigated doublet-triplet energy transfer mechanisms and preassociation effects.
- Incorporated an organic mediator to enhance upconversion efficiency in aerated solutions.
- Applied the upconverted light for photoredox catalytic radical polymerization.
Main Results:
- Achieved a 6-fold enhancement in green-to-blue upconversion efficiency (ΦUC) to approximately 0.2% using the Fe(III)/DPA pair.
- Demonstrated efficient TTAUC via an underexplored doublet-triplet energy transfer pathway.
- Enabled spatially controlled radical polymerization of acrylate monomers using the upconverted singlet excited state of DPA.
- Showcased efficient polymerization under visible light using a low-cost iron photosensitizer.
Conclusions:
- Developed a novel strategy for efficient photon upconversion using abundant iron.
- Established a new pathway for visible-light-driven photoredox catalysis and polymer synthesis.
- Highlighted the potential of iron-based photosensitizers for sustainable energy applications and advanced material fabrication.
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