Luminescent Fe(III) Complex Sensitizes Aerobic Photon Upconversion and Initiates Photocatalytic Radical Polymerization

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-12-10 DOI:10.1021/jacs.4c14248
Pengyue Jin, Xinhuan Xu, Yongli Yan, Heinrich Hammecke, Cui Wang
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Abstract

Light energy conversion often relies on photosensitizers with long-lived excited states, which are mostly made of precious metals such as ruthenium or iridium. Photoactive complexes based on highly abundant iron seem attractive for sustainable energy conversion, but this remains very challenging due to the short excited state lifetimes of the current iron complexes. This study shows that a luminescent Fe(III) complex sensitizes triplet–triplet annihilation upconversion with anthracene derivatives via underexplored doublet-triplet energy transfer, which is assisted by preassociation between the photosensitizer and the annihilator. In the presence of an organic mediator, the green-to-blue upconversion efficiency ΦUC with 9,10-diphenylanthracene (DPA) as the annihilator achieves a 6-fold enhancement to ∼0.2% in aerated solution at room temperature. The singlet excited state of DPA, accessed via photon upconversion in the Fe(III)/DPA pair, allows efficient photoredox catalytic radical polymerization of acrylate monomers in a spatially controlled manner, whereas this process is kinetically hindered with the prompt DPA. Our study provides a new strategy of using low-cost iron and low-energy visible light for efficient polymer synthesis, which is a significant step for both fundamental research and future applications.

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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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