Department of Clinical Laboratory Medicine, Shanghai Chest Hospital, Shanghai Jiao Tong University School of Medicine, Shanghai, 200030, P. R. China.
Shanghai Institute of Thoracic Oncology, Shanghai Chest Hospital, Shanghai Jiao Tong University School of Medicine, Shanghai, 200030, P. R. China.
J Mater Chem B. 2023 Sep 20;11(36):8639-8648. doi: 10.1039/d3tb01076g.
Biothiols participate in numerous physiological and pathological processes in an organism. Quantitative determination and reaction monitoring of biothiols have important implications for evaluating human health. Herein, we synthesized plasmonic alloys as the matrix to assist the laser desorption and ionization (LDI) process of biothiols in mass spectrometry (MS). Plasmonic alloys were constructed with mesoporous structures for LDI enhancement and trimetallic (PdPtAu) compositions for noble metal-thiol hybridization, toward enhanced detection sensitivity and selectivity, respectively. Plasmonic alloys enabled direct detection of biothiols from complex biosamples without any enrichment or separation. We introduced internal standards into the quantitative MS system, achieving accurate quantitation of methionine directly from serum samples with a recovery rate of 103.19% ± 6.52%. Moreover, we established a rapid monitoring platform for the oxidation-reduction reaction of glutathione, consuming trace samples down to 200 nL with an interval of seconds. This work contributes to the development of molecular tools based on plasmonic materials for biothiol detection toward real-case applications.
生物硫醇参与生物体中的许多生理和病理过程。定量测定和反应监测生物硫醇对评估人类健康具有重要意义。在这里，我们合成了等离子体合金作为基质，以辅助生物硫醇在质谱（MS）中的激光解吸电离（LDI）过程。等离子体合金具有介孔结构，用于 LDI 增强，以及三金属（PdPtAu）组成，用于贵金属-硫醇杂化，分别提高了检测灵敏度和选择性。等离子体合金能够直接从复杂的生物样本中检测生物硫醇，无需任何富集或分离。我们将内标引入定量 MS 系统，实现了从血清样本中直接对蛋氨酸进行准确定量，回收率为 103.19%±6.52%。此外，我们建立了一个快速监测谷胱甘肽氧化还原反应的平台，消耗的样品量低至 200nL，间隔为秒级。这项工作为基于等离子体材料的生物硫醇检测开发分子工具做出了贡献，有助于实现实际应用。
