Layer-by-layer assembly strategy for fabrication of polydopamine-polyethyleneimine hybrid modified fibers and their application to solid-phase microextraction of bioactive molecules from medicinal plant samples followed by surface plasmon resonance biosensor validation
Graphical abstract
Introduction
Traditional phytochemical pattern of identifying bioactive compounds, which consists of tedious separation and purification steps, consumes several months of time and yields a lot of organic wastewater, cannot meet the green and environmentally-friendly requirements of pharmaceutical industry in the new stage [1]. Thus, solid-phase microextraction (SPME) is introduced due to the reduced operation times and low reagent consumptions. SPME has been applied in various analytical fields such as environmental [[2], [3], [4]] and food analysis [5], bioanalysis [6], etc. Among them, affinity SPME is more interesting to us [7,8]. For affinity SPME, the receptor or antibody are immobilized onto the surface of a modified fiber or capillaries. Reactive groups of receptor or antibody form linkages with the solid support. The receptor–ligand or antibody-antigen interaction is specific, which leads to the extraction of the desired compounds from the sample.
In the current, a plethora of modifications to the SPME technique were developed to adapt the SPME procedure to receptors. For instance, polydopamine (PDA) has received more and more attention as it exhibits a strong adhesive property to many materials through spontaneous oxidative self-polymerization [9]. PDA layer could be utilized for secondary immobilization reactions since it contains functional groups which can be fabricated with various biomolecules, such as proteins, and enzymes etc. via Michael addition or Schiff base formation. Thus, PDA was widely used for the biomimetic surface modification. Polyethylenimine (PEI) is a cationic polymer, which contains the amine group and two carbon aliphatic CH2CH2 spacers [10]. The negatively charged receptors will be easily bound to fibers coated with PEI.
Herein, as a showcase, we proposed the layer-by-layer assembly strategy for preparing PVDF fibers@PDA@PEI@receptors for efficient SPME of xanthine oxidase (XOD) binding ligands from medicinal plant samples. The schematic of fabrication of the functionalized PVDF fibers for SPME of XOD inhibitors (XOIs) from herbal mixtures is present in Fig. 1. XOIs are typically used for treating nephropathy and renal stone diseases linked to hyperuricemia. In addition, in order to cross-validate the results, surface plasmon resonance biosensor (SPR) [11,12] are utilized for probing the interaction between XOD and ligands. Avidity value (pD2) of these ligands are calculated and plotted against their IC50 values.
Section snippets
Reagents
XOD (from bovine milk, EC:1.1.3.22), dopamine hydrochloride (DA), polyethyleneimine (PEI, 25 kDa), EDC, NHS and ethanolamine hydrochloride (ETA) were obtained from Sigma Co. Allopurinol was supplied by Aladdin Bio- Chem Technology Co. Anti-xanthine oxidase antibody (rabbit polyclonal) was purchased from Bioss Bio-technology Co. Polyvinylidene fluoride fibers (PVDF) were purchased from H-Filtration Membrance Technology & Engineering Co. The rhizome of Plantago depressa was obtained from Qingyang
Characterization of PVDF@PDA@PEI@XOD fibers by using SEM
The morphology of the PVDF fibers, PVDF@PDA fibers, PVDF@PDA@PEI fibers, PVDF@PDA@PEI@XOD fibers were characterized by using SEM. The front and vertical picture of PVDF fibers are present in Fig. 2a–b. The inner diameter and outer diameter of PVDF fibers were measured as 0.9 mm and 1.2 mm, respectively. As is shown in Fig. 2c–f, different surface structures were observed for the fabricated PVDF fibers at different stages, which were different from the smooth surface of PVDF fibers. SEM image in
Conclusion
In this work, the XOD functionalized PVDF fibers was fabricated by using layer-by-layer assembly strategy. Under the optimized conditions, PVDF @PDA@PEI@XOD fibers with high extraction efficiency for isoaceoside was obtained, which was then applied to extract XOD binding ligands from crude extract of Plantago depressa samples prior to UHPLC-Q-TOF-MS analysis. The developed SPME method showed good performance. It should be noticed that seven new XOD inhibitors were identified by using the SPME
CRediT authorship contribution statement
Yi Tao: Conceptualization, Methodology, Supervision, Writing - review & editing. Lin Chen: Data curation, Visualization, Investigation, Writing - original draft. Enci Jiang: Software, Validation.
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This study was supported by the National Natural Science Foundation of China (No.81703701) and Natural Science Foundation of Zhejiang Province (No.LY21H280008). The authors would like to thank the anonymous reviewers for their invaluable suggestions that helped improve the manuscript.
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