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Self-Assembled Supramolecular Sensor for Hydrogen Sulfate via Multipoint Hydrogen Bonding: Real-Sample Analysis and Field-Deployable Paper-Based Detection
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DOI：10.1039/D6AY00430J.png)
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Abstract
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Herein; a self-assembled rhodamine–indole based supramolecular probe (compound 1) has been reported for the selective and sensitive detection of hydrogen sulfate (HSO₄⁻) ions in aqueous medium. The probe exhibited aggregation-assisted photophysical modulation; forming nanoscale assemblies as confirmed by DLS and FESEM analyses. In the absence of the analyte; compound 1 displayed dominant indole-centered emission at 465 nm; whereas interaction with HSO₄⁻ induced hydrogen-bond-assisted spirolactam ring opening; generating a conjugated xanthene framework. This structural transformation produced a distinct ratiometric fluorescence response; characterized by suppression of indole emission and enhancement of xanthene emission at 554 nm. The probe demonstrated high sensitivity with a detection limit of 0.03 µM and a clear linear ratiometric response (R² > 0.99) in the micromolar concentration range. Excellent selectivity (~19-fold enhancement) toward HSO₄⁻ over competing anions and reversible sensing behavior (>85% recovery over five cycles) were observed. Mechanistic investigations revealed multipoint hydrogen-bonding interactions between the indole –NH unit and HSO₄⁻. The practical applicability of the system was validated through analysis of commercial shampoo samples and portable paper-strip sensors; enabling smartphone-assisted detection of HSO₄⁻ ions. These results highlight a self-assembly-driven supramolecular strategy for developing portable and sustainable sensors for anionic species.
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