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Mechanism Switch between Radical-Polar Crossover and Radical Buffering.
Angew Chem Int Ed Engl
March 2025
Wuhan University, College of Chemistry and Molecular Sciences, No. 299 Bayi Road, Wuchang, 430072, Wuhan, CHINA.
Radical-polar crossover is a classic concept that bridges one- and two-electron chemistry. It has been widely used in Cr-catalyzed carbonyl addition reactions to clarify the formation of alkyl chromium(III) intermediate and subsequent carbonyl insertion. Herein, we proposed an orthogonal bonding model, the radical buffering scenario, for Cr-catalyzed carbonyl alkylation.
View Article and Find Full Text PDFTheoretical Exploration of the Effects of Conjugated Side Chains on the Photoelectric Properties of Y6-Based Nonfullerene Acceptors.
J Phys Chem A
March 2025
School of Materials and Energy Southwest University, 2nd Tiansheng Road, Beibei District, Chongqing 400715, China.
With the application of nonfullerene acceptors (NFAs) Y6 and its derivatives, the power conversion efficiencies (PCEs) of single-junction organic solar cells (OSCs) have exceeded 20%. Side-chain engineering has proven to be an important strategy for optimizing Y6-based NFAs. However, studies on the incorporation of conjugated side chains into Y6-based NFAs are still rare, and the corresponding underlying mechanisms are still not well understood.
View Article and Find Full Text PDFEnantioselective Total Synthesis of Fortimicin B.
Angew Chem Int Ed Engl
March 2025
Fudan University, Department of Chemistry, 220 Handan Rd., 200433, Shanghai, CHINA.
Fortimicins, featuring with a pseudodisaccharide scaffold, are an unusual class of aminoglycosides with potent efficacy against several aminoglycoside-resistant bacterial strains. Notably, these molecules also exhibit lower inherent ototoxicity and nephrotoxicity than common aminoglycosides. Consequently, fortimicins are a promising type of protypical molecules for the development of the next-generation of aminoglycoside antibiotics.
View Article and Find Full Text PDFSilylation of Aryl and Alkyl Chlorides by a Seven-Membered Dialkoxysilyl Group Si(pan)Me via an in situ Generated Silylpotassium.
Angew Chem Int Ed Engl
March 2025
Kyoto University: Kyoto Daigaku, Department of Chemistry, JAPAN.
Silicon-containing compounds are increasingly vital in pharmaceutical and agrochemical applications, yet existing silylation methods face critical limitations: poor reactivity of unactivated silanes and instability of activated silylation reagents and their products. Here, we present a seven-membered dialkoxysilyl unit, dioxasilepane, abbreviated as Si(pan), that combines exceptional stability with controllable reactivity. We demonstrate a versatile method for Si(pan)Me incorporation into organic molecules through reactions with diverse aryl, alkenyl, and alkyl chlorides.
View Article and Find Full Text PDFPhotocatalytic Regioselective Alkoxycarbonylation/Cyclization of 3-Aza-1,5-dienes: Access to Ester-Containing Pyrrolin-2-ones.
Org Lett
March 2025
School of Pharmaceutical and Chemical Engineering & Institute for Advanced Studies, Taizhou University, Taizhou 318000, China.
A direct alkoxycarbonyl radical-induced cascade reaction of 3-aza-1,5-dienes with alkyl chlorooxoacetates is reported. With this approach, an extensive range of ester-containing pyrrolin-2-ones are synthesized through photocatalyzed alkoxycarbonylation/cyclization with 3-aza-1,5-dienes under mild conditions. Moreover, dehydrogenative aromatization can proceed with the same photocatalytic system.
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