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DNAzyme-Triggered Visual and Ratiometric Electrochemiluminescence Dual-Readout Assay for Pb(II) Based on an Assembled Paper Device

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    DNAzyme-Triggered Visual and Ratiometric Electrochemiluminescence Dual-Readout Assay for Pb(II) Based on an Assembled Paper Device
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    • Yan Zhang
      Yan Zhang
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      More by Yan Zhang
      Orcidhttp://orcid.org/0000-0002-1936-4619
    • Jinmeng Xu
      Jinmeng Xu
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      More by Jinmeng Xu
    • Shuang Zhou
      Shuang Zhou
      College of Chemistry and Material Science, Shandong Agricultural University, Taian 271018, P.R. China
      More by Shuang Zhou
    • Lin Zhu
      Lin Zhu
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      More by Lin Zhu
    • Xue Lv
      Xue Lv
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      More by Xue Lv
    • Jing Zhang
      Jing Zhang
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      More by Jing Zhang
    • Lina Zhang
      Lina Zhang
      Shandong Provincial Key Laboratory of Preparation and Measurement of Building Materials, University of Jinan, Jinan 250022, P. R. China
      More by Lina Zhang
    • Peihua Zhu*
      Peihua Zhu
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      *E-mail: [email protected]
      More by Peihua Zhu
      Orcidhttp://orcid.org/0000-0002-6874-9013
    • Jinghua Yu*
      Jinghua Yu
      School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China
      *E-mail: [email protected]
      More by Jinghua Yu
      Orcidhttp://orcid.org/0000-0001-5043-0322
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    Analytical Chemistry

    Cite this: Anal. Chem. 2020, 92, 5, 3874–3881
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    https://doi.org/10.1021/acs.analchem.9b05343
    Published January 29, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Currently, portable, low-cost, and easy to operate on-chip analytical units are urgently demanded to meet the requirement for point-of-care testing in resource-limited regions. Herein, a dual-mode lab-on-paper platform is presented, which integrates distance-based visualized readout with ratiometric electrochemiluminescence (ECL) assay in one device. The distance-based measurement is based on a brown visualized strip generated from the oxidation reaction of 3,3′-diaminobenzidine in the presence of H2O2 initiated by horseradish peroxidase (HRP). Notably, visualized semiquantitative results are displayed as the length of a brown bar chart directly on the device—without the need for any data processing or plotting steps, thus avoiding the error caused by the naked eye for distinguishing the color depth. On the contrary, a ratiometric ECL technique was employed for accurate analysis based on the specific biorecognition between Pb2+-dependent DNAzymes and targets. Concretely, upon addition of Pb2+ into the fabricated device, cleaved oligonucleotide fragments connected with HRP functionalized Au nanocubes could permeate through the cellulose on account of their size that is smaller than paper pores, quench the ECL signal of the CdS quantum dots because of resonance energy transfer, and synchronously boost the ECL intensity generated from luminol by catalyzing H2O2. As a consequence, satisfied prediction and accurate monitoring performance was obtained in the range 0.1–2000 nM and 0.01–2000 nM by measuring the length of colored product and the ratio of ECL intensity, respectively. The beneficial advantages of low cost, high efficiency, and the capacity to perform dual-mode assay qualify this innovative device for use with diverse applications.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.9b05343.

    • Chemicals and materials, apparatus used, comments on growing dendritic Au layer, syntheses, preparations, condition optimizations, and EIS characterizations, figures of photographs of wax patterns, photographs of screen-printed electrodes, schematic fabrication procedures of the lab-on-paper device, assay procedures of assembled paper device, folding forms of paper device, representative SEM images, UV–vis absorption spectra, PL spectra, EDS characterization, XRD patterns, photographs of ECL testing equipment, and EIS characterizations, and tables of comparison results of different biosensors, (PDF)

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    Cite this: Anal. Chem. 2020, 92, 5, 3874–3881
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    https://doi.org/10.1021/acs.analchem.9b05343
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