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Anchoring luminol based on Ti3C2-mediated in situ formation of Au NPs for construction of an efficient probe for miRNA electrogenerated chemiluminescence detection

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Abstract

An efficient electrogenerated chemiluminescence (ECL) nanoprobe (luminol-Au NPs-Ti3C2) was constructed based on Ti3C2Tx MXene (Ti3C2)-mediated in situ formation of Au NPs and anchoring luminol to fabricate a sensitive ECL biosensor for miRNA-155 detection. Herein, Ti3C2 with rich Ti vacancy defects was used as reducing agent, and Au NPs were generated in situ and anchored on the Ti3C2 (Au NPs-Ti3C2). Moreover, the Au NPs-Ti3C2 composites were used as a carrier and provided a large number of sites for the efficient linking of luminol through Au–N bonds to form stable luminol-Au NPs-Ti3C2. The immobilization of ECL emitters is a versatile strategy which not only shortens the electron transmission distance between luminol and electrode, but also provides naked catalytic predominated (111) facets of Au NPs with high electrocatalytic activity, significantly improving the ECL signal of luminol. Furthermore, a catalytic hairpin assembly (CHA) reaction was used, resulting in further amplification of the signal. As a result, the as-prepared ECL biosensor exhibited a linear range from 0.3 fM to 1 nM with a detection limit of 0.15 fM, and demonstrated high reliability of miRNA-155 detection even in human serum samples. The construction of a multifunctional ECL probe with excellent ECL emission opens a new chapter for the application of Ti3C2 in the field of bioanalysis.

Graphical abstract

Herein, Au NPs were generated in situ and anchored on the Ti3C2 (Au NPs-Ti3C2). Moreover, the Au NPs-Ti3C2 was used as a carrier and linked luminol through Au–N bonds to form a stable luminol-Au NPs-Ti3C2 nanoprobe. The strategy displayed versatility which not only shortened the electron transmission distance between luminol and the electrode, but also provided a catalytic surface with high electrocatalytic activity of Au NPs that significantly improved the ECL signal of luminol.

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Acknowledgements

This work was financially supported by the Taishan Scholar Program of Shandong Province (ts201511027) and the Natural Science Foundation of Shandong Province (ZR2020MB063), China.

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  1. Tingting Zhuang and Huixin Zhang contributed equally to this work.

Authors and Affiliations

  1. College of Chemistry and Chemical Engineering, College of Materials Science and Engineering, Shandong Sino-Japanese Centre for Collaborative Research of Carbon Nanomaterials, Instrumental Analysis Centre of Qingdao University, Institute of Biomedical Engineering, Qingdao University, Qingdao, 266071, Shandong, China

    Tingting Zhuang, Huixin Zhang, Lun Wang, Linhan Yu & Zonghua Wang

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  1. Tingting Zhuang
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  2. Huixin Zhang
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Contributions

Tingting Zhuang: Data curation, Writing – original draft, Investigation, Drafted and revised the manuscript. Huixin Zhang: Methodology, Writing – review & editing, Investigation, Design. Lun Wang: Characterization, Writing – review & editing. Linhan Yu: Routine analysis. Zonghua Wang: Methodology, Writing – review & editing, Supervision, Funding acquisition. All authors discussed the results and contributed to the writing of this manuscript. All authors have given approval to the final version of the manuscript. Tingting Zhuang and Huixin Zhang contributed equally to this work.

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Correspondence to Zonghua Wang.

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The authors declare that there is no conflict of interest.

The human serum samples used in this work were obtained from the hospital (The Affiliated Hospital of Qingdao University, Qingdao, China), and the ethics committee of the hospital approved the study.

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Zhuang, T., Zhang, H., Wang, L. et al. Anchoring luminol based on Ti3C2-mediated in situ formation of Au NPs for construction of an efficient probe for miRNA electrogenerated chemiluminescence detection. Anal Bioanal Chem 413, 6963–6971 (2021). https://doi.org/10.1007/s00216-021-03651-7

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