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Sensitive colorimetric assay of hydrogen peroxide and glucose in humoral samples based on the enhanced peroxidase-mimetic activity of NH2-MIL-88-derived FeS2@CN nanocomposites compared to its precursors

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Abstract

By employing NH2-MIL-88 as a template, we synthesized the intermediate Fe@CN under high-temperature calcination and further fabricated the FeS2@CN nanocomposites in the presence of sulfur powder. Under varying temperatures (300–600 °C) and Fe@CN-to-S ratios (1:3–6), FeS2@CN500-5 nanocomposites had the highest peroxidase-mimetic activity. Under optimized conditions (incubation temperature 40 °C; solution pH 4.0 and nanocomposite concentration 10 μg/mL; 652-nm absorption), the Michaelis-Menten constant (Km) of FeS2@CN was much lower than that of horseradish peroxidase (HRP), therefore demonstrating that it had a higher affinity for both chromogenic substrates than conventional HRP. The limits of detection for H2O2 and glucose were 0.15 and 0.30 μmol/L, respectively, and the recoveries for glucose were 91.8–103% with RSDs <5.2%. The novelty of this study lies in (1) the FeS2@CN was confirmed to possess stronger enzyme-mimetic activity than its precursors (NH2-MIL-88 and Fe@CN); (2) the enhanced activity resulted from the unsaturated sites of N and S doping and the plentiful defects on the porous carbon surface; and (3) free radical trapping experiments evidenced that •OH played a major role in the catalytic reaction, while h+ and •O2− simultaneously participated in the catalytic process. These convincing performance metrics lead us to postulate that the FeS2@CN-based colorimetric biosensor provides a promising approach for several real-world applications, such as point-of-care diagnosis and workplace health evaluations.

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Funding

This work was jointly supported by the National Science Foundation of China (22076134 and 21876125), Zhejiang Provincial Public Benefit Project (LGC22B070002), Jiangsu Provincial Natural Science Foundation (BK20211338), Key Science & Technology Project of Suzhou City (SS202028), Zhejiang Provincial University Student Sci&Tech Innovation Activity Plan and New Seedling Talent Plan (No. 2021R413061), and National Training Program of Innovation and Entrepreneurship for Undergraduates (202110343068S).

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Authors and Affiliations

  1. Zhejiang Provincial Key Laboratory of Watershed Science and Health, College of Public Health and Management, Wenzhou Medical University, Wenzhou, 325035, China

    Ru Fan, Jinrong Tian & Peipei Zhou

  2. School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou, 215009, China

    Huili Wang & Xuedong Wang

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  1. Ru Fan
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Fan, R., Tian, J., Wang, H. et al. Sensitive colorimetric assay of hydrogen peroxide and glucose in humoral samples based on the enhanced peroxidase-mimetic activity of NH2-MIL-88-derived FeS2@CN nanocomposites compared to its precursors. Microchim Acta 189, 427 (2022). https://doi.org/10.1007/s00604-022-05525-w

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