Multiplexed derivatization strategy-based dummy molecularly imprinted polymers as sorbents for magnetic dispersive solid phase extraction of globotriaosylsphingosine prior to UHPLC-MS/MS quantitation

• Published in: Mikrochimica acta (1966) Vol. 187; no. 7; p. 373
• Main Authors: Hu, Jingwen, Zhu, Shuyun, Chen, Shi-En, Liu, Ruisheng, Sun, Jing, Zhao, Xian-En, Liu, Huwei
• Format: Journal Article
• Language: English
• Published: Vienna Springer Vienna 01.07.2020; Springer; Springer Nature B.V
• Subjects: Analytical Chemistry; Biomarkers; Characterization and Evaluation of Materials; Chemical tests and reagents; Chemistry; Chemistry and Materials Science; Derivatives; Dispersion; Fourier transforms; High performance liquid chromatography; Hydrogen bonding; Hydrophobicity; Imprinted polymers; Ions; Labelling; Mass spectrometry; Microengineering; Nanochemistry; Nanotechnology; Original Paper; Photoelectrons; Photomicrographs; Polymer industry; Reagents; Recognition; Selectivity; Solid phases; Sorbents; Transmission electron microscopes; Transmission electron microscopy; X-ray spectroscopy; Dummy molecular imprinting technology; Globotriaosylsphingosine; Magnetic material; Multiplexed labeling; Fabry disease biomarker; Triple quadrupole mass spectrometry
• ISSN: 0026-3672; 1436-5073
• DOI: 10.1007/s00604-020-04341-4

A new series of 9-plex chemical isotope-labeling reagents, levofloxacin-based mass tags (LMTs) named as LMT359, 360, 361, 362, 363, 373, 375, 376, and 378, was firstly designed and synthesized for the high-throughput labeling of globotriaosylsphingosine (lyso-Gb3), a disease biomarker of Fabry disease. Creatively based on derivatization strategy—dummy template technique, dummy magnetic molecularly imprinted polymers (DMMIPs) were designed and prepared using LMT387-labeled lyso-Gb3 as a dummy template. The novel DMMIP material was used as sorbents for magnetic dispersive solid-phase extraction of 9-plexed LMT derivatives of lyso-Gb3 from equally mixed derivatization solutions. The enriched 8-plexed lyso-Gb3 derivatives from 8 real samples were quantified by ultra-high-performance liquid chromatography tandem mass spectrometry in a single run using simultaneously extracted LMT359-labeled standard lyso-Gb3 as internal standards. DMMIPs were characterized by using the transmission electron microscope (TEM), Fourier transform infrared, X-ray photoelectron spectroscopy, and some other characterization techniques. TEM micrograph showed that the prepared DMMIPs had an apparent imprinting layer. Triple-recognition abilities of DMMIPs towards LMT-lyso-Gb3 mainly rely on the hydrogen bonding, electrostatic attraction, hydrophobic interaction, and boronate affinity. The imprinting factor of DMMIPs towards LMT-lyso-Gb3 was 5.1. This method shows the advantages of high selectivity (triple recognition), high sensitivity, high accuracy (recovery 93.5–108.8%), and high throughput (8 samples in a single run). The proposed method was successfully applied to the determination of lyso-Gb3 in plasma samples with spiked recoveries in the range of 95.0–102.4%. This indicates that the method is promising in bioanalysis and medical testing of lyso-Gb3 in the future. Graphical abstract Synthesis of multiplexed derivatization reagents and its correlative molecularly imprinted polymers for magnetic extraction of globotriaosylsphingosine