Synthesis of Benzo[b]thiophene 1,1-Dioxides via Pd-Catalyzed Sulfinylation of Aryl Triflates and Their Use as Large Stokes Shift Fluorophores for Multicolor Live-Cell Imaging with Self-Labeling Tags

通过钯催化芳基三氟甲磺酸酯的亚磺酰化反应合成苯并[b]噻吩-1,1-二氧化物,并将其用作具有大斯托克斯位移的荧光团,用于多色活细胞成像及自标记标签

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Abstract

Benzo-[b]-thiophene 1,1-dioxide is a relatively underrepresented sulfone-embedded heterocycle with niche uses in material science (OLED emitters), pharmaceutical research (an electrophilic warhead in targeted covalent inhibitors), and as a structural unit in reversibly switchable diarylethene fluorophores. Benzo-[b]-thiophene 1,1-dioxides are most commonly prepared by the oxidation of the corresponding benzothiophenes. Here, we propose an alternative approach based on Pd-catalyzed sulfinylation of ortho-carbonyl-substituted aryl triflates followed by S-alkylation and Knoevenagel condensation. This methodology allows for an expedient access to diversely substituted benzo-[b]-thiophene 1,1-dioxides, including 6-dialkylamino "push-pull" type fluorophores possessing large (>140 nm) Stokes shifts. Fluorescent labels derived from this core structure are compatible with live-cell imaging using self-labeling protein tags (HaloTag, SNAP-tag, and CLIP-tag). Together with the established live-cell fluorescent labels and orthogonal self-labeling tags, they allow for simultaneous observation of up to three intracellular targets below the diffraction limit using fluorescence microscopy with three excitation lasers (485, 561, and 640 nm) and stimulated emission depletion (STED) at 775 nm.

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