Plasmonic alloys for quantitative determination and reaction monitoring of biothiols

Abstract

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.