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Laser ablative TiO2 and tremella-like CuInS2 nanocomposites for robust and ultrasensitive photoelectrochemical sensing of let-7a

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Abstract

A photoelectrochemical (PEC) biosensor based on a multiple signal amplification strategy was established for highly sensitive detection of microRNA (miRNA). TiO2 was prepared on the surface of titanium sheet by laser etching to improve its stability and photoelectrical properties, and CuInS2-sensitized TiO2 was used to form a superior photoelectrical layer, which realized the initial signal amplification. The electron donor dopamine (DA) was modified to H2 as a signal regulator, which effectively increased the photocurrent signal. To further amplify the signal, an enzyme-free hybridization reaction was implemented. When target let-7a and fuel-DNA (F-DNA) were present, the base of H1 specifically recognized let-7a and forced dopamine@AuNPs-H2 away from the electrode surface. Subsequently, the end base of H1 specifically recognized F-DNA, and let-7a was replaced and recycled to participate in the next cycle. Enzyme-free circulation, as a multifunctional amplification method, ensured the recycling of target molecules. This PEC sensor for let-7a detection showed an excellent linear response from 0.5 to 1000 pM with a detection limit of 0.12 pM. The intra-batch RSD was 3.8% and the recovery was 87.74–108.1%. The sensor was further used for clinical biomolecular monitoring of miRNA, showing excellent quantitative detection capability.

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Funding

This work was supported by the National Natural Science Foundation of China (22074053, 21775055, 21874055); A project of Shandong Province Higher Educational Youth Innovation Science and Technology Program (2020GXRC047, 2019KJC016); The Project of “20 items of University” of Jinan (2018GXRC001); the Taishan Scholars program and Case-by-Case Project for Top Outstanding Talents of Jinan.

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Author notes

  1. Cuiping Fu and Xuefeng Wang contributed equally to this work.

Authors and Affiliations

  1. Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, Institute for Advanced Interdisciplinary Research, University of Jinan, Jinan, 250022, People’s Republic of China

    Cuiping Fu, Xuefeng Wang, Weijia Zhou & Shenguang Ge

  2. Shandong Analysis and Test Center, Qilu University of Technology (Shandong Academy of Sciences), Jinan, 250014, People’s Republic of China

    Fumin Xue

  3. School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, People’s Republic of China

    Peihua Zhu & Jinghua Yu

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  1. Cuiping Fu
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  2. Xuefeng Wang
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Correspondence to Peihua Zhu, Weijia Zhou or Shenguang Ge.

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Fu, C., Wang, X., Xue, F. et al. Laser ablative TiO2 and tremella-like CuInS2 nanocomposites for robust and ultrasensitive photoelectrochemical sensing of let-7a. Microchim Acta 189, 145 (2022). https://doi.org/10.1007/s00604-022-05178-9

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