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<p>A&#xa0;photosensitization-based synthesis strategy is established&#xa0;enabling the room-temperature preparation of sulfur-doped graphene quantum dots (S-GQDs). Under 365-nm UV irradiation, GQDs produce singlet oxygen (<sup>1</sup>O<sub>2</sub>), catalyzing the oxidation of dimethyl sulfoxide (DMSO) into sulfur-containing intermediates, which subsequently react with surface functional groups on GQDs to achieve precise sulfur doping. The introduced defect states significantly enhanced radiative recombination, raising the quantum yield to 29.5%. The S-GQDs showed outstanding stability, including superior photobleaching resistance (minimal fluorescence change after 3.5&#xa0;h UV exposure), high thermal stability (minimal variation from 20 to 80&#xa0;°C), excellent pH tolerance (&lt; 10% fluctuation within pH 3–12), and stable fluorescence in high-salinity and long-term storage conditions. Utilizing photoinduced electron transfer (PET) and fluorescence resonance energy transfer (FRET) mechanisms, the S-GQDs exhibited sensitivity and selectivity toward picric acid (PA), with a linear response between 1 and 60&#xa0;μM and a detection limit of 0.56&#xa0;μM. Practical tests confirmed reliable detection of PA on human finger surfaces, and the results were in&#xa0;good&#xa0; agreement with those obtained by high-performance liquid chromatography (HPLC). This photosensitization-based oxidation strategy provides a green, scalable route for preparation of high-performance S-GQDs that have broad potential applications in environmental monitoring, bioanalysis, etc.</p> Graphical Abstract <p></p>

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Facile sulfur-doping by self-photosensitization of graphene quantum dots in DMSO for improved sensing

  • 期刊论文

  • 发表日期：

    2025年9月25日

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  • Dongping Cai,
  • Kai Shi,
  • Zhengxing Gong,
  • Xinfeng Zhang

摘要

A photosensitization-based synthesis strategy is established enabling the room-temperature preparation of sulfur-doped graphene quantum dots (S-GQDs). Under 365-nm UV irradiation, GQDs produce singlet oxygen (1O2), catalyzing the oxidation of dimethyl sulfoxide (DMSO) into sulfur-containing intermediates, which subsequently react with surface functional groups on GQDs to achieve precise sulfur doping. The introduced defect states significantly enhanced radiative recombination, raising the quantum yield to 29.5%. The S-GQDs showed outstanding stability, including superior photobleaching resistance (minimal fluorescence change after 3.5 h UV exposure), high thermal stability (minimal variation from 20 to 80 °C), excellent pH tolerance (< 10% fluctuation within pH 3–12), and stable fluorescence in high-salinity and long-term storage conditions. Utilizing photoinduced electron transfer (PET) and fluorescence resonance energy transfer (FRET) mechanisms, the S-GQDs exhibited sensitivity and selectivity toward picric acid (PA), with a linear response between 1 and 60 μM and a detection limit of 0.56 μM. Practical tests confirmed reliable detection of PA on human finger surfaces, and the results were in good  agreement with those obtained by high-performance liquid chromatography (HPLC). This photosensitization-based oxidation strategy provides a green, scalable route for preparation of high-performance S-GQDs that have broad potential applications in environmental monitoring, bioanalysis, etc.

Graphical Abstract