期刊
ACS SENSORS
卷 8, 期 1, 页码 270-279出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssensors.2c02140
关键词
closed bipolar electrode; blood; biosensor; point-of-care; colorimetric; cholesterol; lactate; glucose
资金
- National Science Foundation [1904196]
- Discovery Fund of Notre Dame's Berthiaume Institute for Precision Health
- Berry Family Fellowship
- Jack and Mary Ann Remick Fellowship
- Notre Dame Center for Environmental Science and Technology Fellowship (CEST)
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1904196] Funding Source: National Science Foundation
We report a closed bipolar electrode (CBE)-based sensing platform for the detection of diagnostic metabolites in undiluted whole human blood. The sensor uses a specific electrode chemistry to overcome nonspecific protein adsorption and amplify sensing currents, and demonstrates good reproducibility and detection limits for measuring cholesterol, glucose, and lactate concentrations.
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 (similar to 5% or better) and with limits of detection of 79 mu M for cholesterol, 59 mu M for glucose, and 86 mu M 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 similar to 3.5% across all three metabolites in the ranges studied.
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