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Construction of PEGylated boronate-affinity-oriented imprinting magnetic nanoparticles for ultrasensitive detection of ellagic acid from beverages

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Abstract

Molecularly imprinted polymers (MIPs) can exhibit antibody-level affinity for target molecules. However, the nonspecific adsorption of non-imprinted regions for non-target molecules limits the application range of MIPs. Herein, we fabricated PEGylated boronate-affinity-oriented ellagic acid-imprinting magnetic nanoparticles (PBEMN), which first integrated boronate-affinity-oriented surface imprinting and sequential PEGylation for small molecule-imprinted MIPs. The resultant PBEMN possess higher adsorption capacity and faster adsorption rate for template ellagic acid (EA) molecules than the non-PEGylated control. To prove the excellent performance, the PBEMN were linked with hydrophilic boronic acid-modified/fluorescein isothiocyanate-loaded graphene oxide (BFGO), because BFGO could selectively label cis-diol-containing substances by boronate-affinity and output ultrasensitive fluorescent signals. Based on a dual boronate-affinity synergy, the PBEMN first selectively captured EA molecules by boronate-affinity-oriented molecular imprinted recognition, and then the EA molecules were further labeled with BFGO through boronate-affinity. The PBEMN linked BFGO (PBPF) strategy provided ultrahigh sensitivity for EA molecules with a limit of detection of 39.1 fg mL−1, resulting from the low nonspecific adsorption of PBEMN and the ultrasensitive fluorescence signal of BFGO. Lastly, the PBPF strategy was successfully employed in the determination of EA concentration in a spiked beverage sample with recovery and relative standard deviation in the range of 96.5 to 104.2% and 3.8 to 5.1%, respectively. This work demonstrates that the integration of boronate-affinity-oriented surface imprinting and sequential PEGylation may be a universal tool for improving the performance of MIPs.

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Funding

This work was financially supported by the National Natural Science Foundation of China (Grant No. 21605114) and Tianjin Natural Science Foundation (Grant No. 17JCQNJC13300).

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  1. Meng-Ying Chen and Jin-Ye Lang contributed equally to this work.

Authors and Affiliations

  1. Tianjin Key Laboratory on Technologies Enabling Development of Clinical Therapeutics and Diagnostics, School of Pharmacy, Tianjin Medical University, Building B, 22 Qixiangtai Road, Heping District, Tianjin, 300072, China

    Meng-Ying Chen, Jin-Ye Lang, Chen-Chen Bai, Shi-Song Yu, Lin-Yi Dong & Xian-Hua Wang

  2. School of Chemistry and Chemical Engineering, Shandong Provincial Key Laboratory/Collaborative Innovation Center of Chemical Energy Storage & Novel Cell Technology, Liaocheng University, Liaocheng, 252000, China

    Xiang-Jin Kong

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  1. Meng-Ying Chen
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Chen, MY., Lang, JY., Bai, CC. et al. Construction of PEGylated boronate-affinity-oriented imprinting magnetic nanoparticles for ultrasensitive detection of ellagic acid from beverages. Anal Bioanal Chem 414, 6557–6570 (2022). https://doi.org/10.1007/s00216-022-04213-1

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