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Closed Bipolar Electrode-Enabled Electrochromic Sensing of Multiple Metabolites in Whole Blood

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    Closed Bipolar Electrode-Enabled Electrochromic Sensing of Multiple Metabolites in Whole Blood
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    • Christiana Oh
      Christiana Oh
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana46556, United States
      More by Christiana Oh
      Orcidhttps://orcid.org/0000-0002-6018-920X
    • Bumjun Park
      Bumjun Park
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana46556, United States
      More by Bumjun Park
      Orcidhttps://orcid.org/0000-0002-3779-1315
    • Vignesh Sundaresan
      Vignesh Sundaresan
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana46556, United States
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    • Jennifer L. Schaefer
      Jennifer L. Schaefer
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana46556, United States
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    • Paul W. Bohn*
      Paul W. Bohn
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana46556, United States
      Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana46556, United States
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-9052-0349
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    ACS Sensors

    Cite this: ACS Sens. 2023, 8, 1, 270–279
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    https://doi.org/10.1021/acssensors.2c02140
    Published December 22, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    We report a closed bipolar electrode (CBE)-based sensing platform for the detection of diagnostic metabolites in undiluted whole human blood. The sensor is enabled by electrode chemistry based on: (1) a mixed layer of blood-compatible adsorption-resistant phosphorylcholine (PPC) and phenylbutyric acid (PBA), (2) ferrocene (Fc) redox mediators, and (3) immobilized redox-active enzymes. This scheme is designed to overcome nonspecific protein adsorption and amplify sensing currents in whole human fluids. The scheme also incorporates a diffusing mediator to increase electronic communication between the immobilized redox enzyme and the working electrode. The use of both bound and freely diffusing mediators is synergistic in producing the electrochemical response. The sensor is realized by linking the analyte cell, containing the specific electrode surface architecture, through a CBE to a reporter cell containing the electrochromic reporter, methyl viologen (MV). The colorless-to-purple color change accompanying the 1e– reduction of MV2+ is captured using a smartphone camera. Subsequent red-green-blue analysis is performed on the acquired images to determine cholesterol, glucose, and lactate concentrations in whole blood. The CBE blood metabolite sensor produces a linear color change at clinically relevant concentration ranges for all metabolites with good reproducibility (∼5% or better) and with limits of detection of 79 μM for cholesterol, 59 μM for glucose, and 86 μM for lactate. Finally, metabolite concentration measurements from the CBE blood metabolite sensor are compared with results from commercially available FDA-approved blood cholesterol, glucose, and lactate meters, with an average difference of ∼3.5% across all three metabolites in the ranges studied.

    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/acssensors.2c02140.

    • Details of sensor fabrication along with electrochemical, XPS, and EIS characterization, comparison of CBE sensor working curves using a microscope and smartphone camera, linear regression parameters for sensor working curves for all three metabolites, and data comparing CBE blood metabolite sensor and commercial metabolite meters for blood glucose and lactate detection (PDF)

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    This article is cited by 14 publications.

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    2. Chen Chen, Mei-Hua Wang, Meng-Han Zhu, Fu-Xing Zhao, Bang Yu, Qian-Hao Pan, Xin Guo, Si-Zhe Sheng, Zhen He, Jin-Long Wang, Shu-Hong Yu. Electrochromic Pressure-Sensitive Device for In Situ and Instantaneous Pressure Visualization. Nano Letters 2025, 25 (11) , 4154-4162. https://doi.org/10.1021/acs.nanolett.4c05064
    3. Shuyun Meng, Na Dong, Shuda Liu, Zuo Chen, Mingzhen Zhu, Xueping Zhang, Dong Liu, Tianyan You. Referenced-Closed Bipolar Electrode to Enable the Photoelectrochemical-Electrochromic Synchronous Biosensing. Analytical Chemistry 2025, 97 (8) , 4533-4541. https://doi.org/10.1021/acs.analchem.4c06205
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    7. Hongkun Li, Qianqian Cai, Zhikang Li, Guifen Jie, Hong Zhou. A spatial-potential resolved bipolar electrode electrochemiluminescence biosensor based on polarity conversion for dual-mode detection of miRNA-122 and CEA. Biosensors and Bioelectronics 2024, 255 , 116258. https://doi.org/10.1016/j.bios.2024.116258
    8. David Probst, Koji Sode. Development of closed bipolar electrode based L-lactate sensor employing quasi-direct electron transfer type enzyme with cyclic voltammetry. Biosensors and Bioelectronics 2024, 254 , 116197. https://doi.org/10.1016/j.bios.2024.116197
    9. Anna Dettlaff, Joshua J. Tully, Georgia Wood, Deep Chauhan, Ben G. Breeze, Lijiang Song, Julie V. Macpherson. A closed bipolar electrochemical cell for the interrogation of BDD single particles: Electrochemical advanced oxidation. Electrochimica Acta 2024, 485 , 144035. https://doi.org/10.1016/j.electacta.2024.144035
    10. Lu Li, Weiyi Chen, Meng Wang, Xinjiang Shi, Shiming Zhang, Debao Xiao. Hole-transporting materials boost optoelectronic performance: Their first application in electrochromic device based on 1,1′-Bis(3-sulfopropyl) viologen. Chemical Physics Letters 2024, 840 , 141143. https://doi.org/10.1016/j.cplett.2024.141143
    11. Zahra Damirchi, Ali Firoozbakhtian, Morteza Hosseini, Mohammad Reza Ganjali. Ti3C2/Ni/Sm-based electrochemical glucose sensor for sweat analysis using bipolar electrochemistry. Microchimica Acta 2024, 191 (3) https://doi.org/10.1007/s00604-024-06209-3
    12. Yipu Du, Julius Reitemeier, Qiang Jiang, Md Omarsany Bappy, Paul W. Bohn, Yanliang Zhang. Hybrid Printing of Fully Integrated Microfluidic Devices for Biosensing. Small 2024, 20 (5) https://doi.org/10.1002/smll.202304966
    13. Nurul Asyikeen Ab Mutalib, Hiroaki Suzuki. Evolution in the development of next generation electrochemical microdevices via bipolar electrochemistry. Current Opinion in Electrochemistry 2024, 43 , 101424. https://doi.org/10.1016/j.coelec.2023.101424
    14. Christopher Mwanza, Shou-Nian Ding. Newly Developed Electrochemiluminescence Based on Bipolar Electrochemistry for Multiplex Biosensing Applications: A Consolidated Review. Biosensors 2023, 13 (6) , 666. https://doi.org/10.3390/bios13060666
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    ACS Sensors

    Cite this: ACS Sens. 2023, 8, 1, 270–279
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acssensors.2c02140
    Published December 22, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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