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

IF 5.3 2区化学 Q1 CHEMISTRY, ANALYTICAL

Microchimica Acta Pub Date : 2025-09-25 DOI:10.1007/s00604-025-07512-3

Dongping Cai, Kai Shi, Zhengxing Gong, Xinfeng Zhang

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Abstract

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

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利用自光敏石墨烯量子点在DMSO中掺杂硫以改善传感性能。

建立了一种基于光敏的合成策略，可以在室温下制备硫掺杂石墨烯量子点（S-GQDs）。在365nm紫外光照射下，GQDs产生单线态氧（1O2），催化二甲基亚砜（DMSO）氧化生成含硫中间体，这些中间体随后与GQDs上的表面官能团反应以实现精确的硫掺杂。引入的缺陷态显著增强了辐射复合，将量子产率提高到29.5%。S-GQDs表现出优异的稳定性，包括优异的光漂白抗性（在紫外线照射3.5 h后荧光变化最小），高热稳定性（在20至80°C之间变化最小），优异的pH耐受性(

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来源期刊

Microchimica Acta 化学-分析化学

CiteScore

9.80

自引率

5.30%

发文量

410

审稿时长

2.7 months

期刊介绍： As a peer-reviewed journal for analytical sciences and technologies on the micro- and nanoscale, Microchimica Acta has established itself as a premier forum for truly novel approaches in chemical and biochemical analysis. Coverage includes methods and devices that provide expedient solutions to the most contemporary demands in this area. Examples are point-of-care technologies, wearable (bio)sensors, in-vivo-monitoring, micro/nanomotors and materials based on synthetic biology as well as biomedical imaging and targeting.