Blue-to-UVB Upconversion,Solvent Sensitization and Challenging Bond Activation Enabled by a Benzene-Based Annihilator |
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Authors: | Till J. B. Zähringer Julian A. Moghtader Maria-Sophie Bertrams Dr. Bibhisan Roy Masanori Uji Prof. Dr. Nobuhiro Yanai Prof. Dr. Christoph Kerzig |
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Affiliation: | 1. Department of Chemistry, Johannes Gutenberg University Mainz, Duesbergweg 10–14, 55128 Mainz, Germany;2. Department of Applied Chemistry, Graduate School of Engineering, Center for Molecular Systems (CMS), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka, 819-0395 Japan |
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Abstract: | Several energy-demanding photoreactions require harsh UV light from inefficient light sources. The conversion of low-energy visible light to high-energy singlet states via triplet-triplet annihilation upconversion (TTA-UC) could offer a solution for driving such reactions under mild conditions. We present the first annihilator with an emission maximum in the UVB region that, combined with an organic sensitizer, is suitable for blue-to-UVB upconversion. The annihilator singlet was successfully employed as an energy donor in subsequent FRET activations of aliphatic carbonyls. This hitherto unreported UC-FRET reaction sequence was directly monitored using laser spectroscopy and applied to mechanistic irradiation experiments demonstrating the feasibility of Norrish chemistry. Our results provide clear evidence for a novel blue light-driven substrate or solvent activation strategy, which is important in the context of developing more sustainable light-to-chemical energy conversion systems. |
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Keywords: | Energy Transfer Photochemistry Sustainable Chemistry Time-Resolved Spectroscopy Upconversion |
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