An efficient, mild, and atom-economical synthesis of benzo[]fluorenols from 1,6-enynes has been developed under photocatalytic conditions. A single P/N heteroleptic Cu(I)-photosensitizer might exhibit both energy-transfer and photoredox catalytic activities in the formation of benzo[]fluorenols.
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http://dx.doi.org/10.1021/acs.orglett.1c01427 | DOI Listing |
Chem Sci
December 2024
College of Materials Science and Engineering, Fuzhou University New Campus 350108 China
Atomically precise metal nanoclusters (NCs) have recently been recognized as an emerging sector of metal nanomaterials but suffer from light-induced poor stability, giving rise to the detrimental self-transformation into metal nanocrystals (NYs), losing the photosensitization effect and ultimately retarding their widespread applications in photoredox catalysis. Are metal NCs definitely superior to metal NYs in heterogeneous photocatalysis in terms of structural merits? To unlock this mystery, herein, we conceptually demonstrate how to rationally manipulate the instability of metal NCs to construct high-efficiency artificial photosystems and examine how the metal NYs self-transformed from metal NCs influence charge transfer in photoredox selective organic transformation. To our surprise, the results indicate that the Schottky-type electron-trapping ability of Au NYs surpasses the photosensitization effect of glutathione (GSH)-protected Au clusters [Au(GSH) NCs] in mediating charge separation and enhancing photoactivities towards selective photoreduction of aromatic nitro compounds to amino derivatives and photocatalytic oxidation of aromatic alcohols to aldehydes under visible light irradiation.
View Article and Find Full Text PDFChem Biodivers
January 2025
Department of Pharmaceutical Chemistry, MM College of Pharmacy, Maharishi Markandeshwar (Deemed to be University), Ambala, India.
Quinolone antibiotics are a crucial class of synthetic antibacterial agents, widely utilized due to their broad spectrum of antibacterial activity. Due to the development of antimicrobial resistance, the potency of quinolone drugs decreased. Many conventional methods have been developed to elevate amination rate and to improve yield.
View Article and Find Full Text PDFSmall
January 2025
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
The ligands in metal-organic framework (MOF) play as light absorption center and transfer photogenerated electrons to metal node through ligand-to-metal charge transfer (LMCT) during photocatalysis, and energy utilization efficiency is strongly restricted by the light inertness of ligands. Herein, a ligand updating strategy is proposed by inserting energy centers to MOFs to activate the inherent ligands, realizing boosting hot electron generation and photocatalytic activities via the cascaded proceeding of energy transfer and charge transfer. By taking PCN-777 (a zeotype mesoporous Zr-containing MOF) as an example, this study shows that the embedded energy center of 1-pyrenecarboxylic acid (PCA) can activate the inherent ligand of PCN-777 through triplet-triplet energy transfer, where triplet excitons would dissociate into photocarriers migrating to the Zr metal cluster via LMCT process.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
School of Chemistry and Physics, Queensland University of Technology (QUT), 2 George Street, Brisbane, QLD 4000, Australia.
We demonstrate that single-chain nanoparticles (SCNPs) - compact covalently folded single polymer chains - can increase photocatalytic performance of an embedded catalytic center, compared to the comparable catalytic system in free solution. In particular, we demonstrate that the degree of compaction allows to finely tailor the catalytic activity, thus evidencing that molecular confinement is a key factor in controlling photocatalysis. Specifically, we decorate a linear parent polymer with both photoreactive chalcone moieties as well as Ru(bpy) catalytic centers.
View Article and Find Full Text PDFJACS Au
December 2024
Department of Chemistry, University of Connecticut, Storrs, Connecticut 06269-3060, United States.
Red-light absorbing photoredox catalysts offer potential advantages for large-scale reactions, expanding the range of usable substrates and facilitating bio-orthogonal applications. While many red-light absorbing/emitting fluorophores have been developed recently, functional red-light absorbing photoredox catalysts are scarce. Many photoredox catalysts rely on long-lived triplet excited states (triplets), which can efficiently engage in single electron transfer (SET) reactions with substrates.
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