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Graphene-Enabled High-Performance Electrokinetic Focusing and Sensing
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    Graphene-Enabled High-Performance Electrokinetic Focusing and Sensing
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    • Xiao Fan
      Xiao Fan
      Department of Mechanical and Industrial Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
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    • Xiaoyu Zhang
      Xiaoyu Zhang
      Department of Mechanical and Industrial Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      More by Xiaoyu Zhang
    • Jinglei Ping*
      Jinglei Ping
      Department of Mechanical and Industrial Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      Institute of Applied Life Sciences, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      *Email: [email protected]
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    Other Access OptionsSupporting Information (5)

    ACS Nano

    Cite this: ACS Nano 2022, 16, 7, 10852–10858
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    https://doi.org/10.1021/acsnano.2c03054
    Published June 17, 2022
    Copyright © 2022 American Chemical Society

    Abstract

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    Transverse isoelectric focusing, i.e., isoelectric focusing that is normal to the fluid-flow direction, is an electrokinetic method ideal for micro total analysis. However, a major challenge remains: There is no electrode system integrable in a microfluidic device to allow reliable transverse isoelectric focusing and electrokinetic sensing. Here, we overcome this barrier by developing devices that incorporate microelectrodes made of monolayer graphene. We find that the electrolysis stability over time for graphene microelectrodes is >103× improved compared to typical microfabricated inert-metal microelectrodes. Through transverse isoelectric focusing between graphene microelectrodes, within minutes, specific proteins can be separated and concentrated to scales of ∼100 μm. Based on the concentrating effect and the high optical transparency of graphene, we develop a three-dimensional multistream microfluidic strategy for label-free detection of the proteins at same processing position with a sensitivity that is ∼102× higher than those of the state-of-the-art label-free sensors. These results demonstrate the advantage of monolayer-graphene microelectrodes for high-performance electrokinetic analysis to allow lab-on-a-chips of maximal time and size efficiencies.

    Copyright © 2022 American Chemical Society

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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/acsnano.2c03054.

    • Demonstration of the corrosion of a gold electrode (Figure S1); Illustration of a typical triple-stream device (Figure S2); Characterization of the CVD graphene using Raman spectroscopy and atomic force microscopy (Figure S3); pH gradients between two graphene microelectrodes at different voltage biases (Figure S4); Device–device variation (Figure S5); Normalized emission profiles for the BSA molecules and lectin molecules at different times (Figure S6); Emission profiles of the BSA molecules that are electrokinetically focused from Stream 1 to Stream 2 at different times (Figure S7); Fluorescence emission of the recognizers in Stream 3 (Figure S8); Typical sensor intensity change ratios for different unlabeled-BSA concentrations (Figure S9); Protein-detection control experiment (Figure S10); Fluorescence emission for the recognizer molecules mixing with different molecules (Figure S11) (PDF)

    • Movie S1: Generation of pH gradient between two graphene microelectrodes (AVI)

    • Movie S2: Separation of mixed BSA molecules and lectin molecules in a microfluidic channel (AVI)

    • Movie S3: Transfer of BSA molecules from one stream to another in a microfluidic channel (AVI)

    • Movie S4: Fluorescence emission arising from the binding of the recognizer molecules in Stream 3 adjacent to Stream 1 (AVI)

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    ACS Nano

    Cite this: ACS Nano 2022, 16, 7, 10852–10858
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.2c03054
    Published June 17, 2022
    Copyright © 2022 American Chemical Society

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