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Published November 2022 | Supplemental Material + Accepted Version
Journal Article Open

A wearable electrochemical biosensor for the monitoring of metabolites and nutrients

Abstract

Wearable non-invasive biosensors for the continuous monitoring of metabolites in sweat can detect a few analytes at sufficiently high concentrations, typically during vigorous exercise so as to generate sufficient quantity of the biofluid. Here we report the design and performance of a wearable electrochemical biosensor for the continuous analysis, in sweat during physical exercise and at rest, of trace levels of multiple metabolites and nutrients, including all essential amino acids and vitamins. The biosensor consists of graphene electrodes that can be repeatedly regenerated in situ, functionalized with metabolite-specific antibody-like molecularly imprinted polymers and redox-active reporter nanoparticles, and integrated with modules for iontophoresis-based sweat induction, microfluidic sweat sampling, signal processing and calibration, and wireless communication. In volunteers, the biosensor enabled the real-time monitoring of the intake of amino acids and their levels during physical exercise, as well as the assessment of the risk of metabolic syndrome (by correlating amino acid levels in serum and sweat). The monitoring of metabolites for the early identification of abnormal health conditions could facilitate applications in precision nutrition.

Additional Information

© 2022 Springer Nature. Received 07 June 2021. Accepted 19 June 2022. Published 15 August 2022. This project was supported by the National Institutes of Health grant R01HL155815, Office of Naval Research grants N00014-21-1-2483 and N00014-21-1-2845, the Translational Research Institute for Space Health through NASA NNX16AO69A, NASA Cooperative Agreement 80NSSC20M0167, High Impact Pilot Research Award T31IP1666 and grant R01RG3746 from the Tobacco-Related Disease Research Program, Caltech-City of Hope Biomedical Initiative Pilot Grant and the Rothenberg Innovation Initiative Program at California Institute of Technology. J.T. was supported by the National Science Scholarship (NSS) from the Agency of Science Technology and Research (A*STAR) Singapore. We gratefully acknowledge critical support and infrastructure provided for this work by the Kavli Nanoscience Institute at Caltech. This project benefitted from the use of instrumentation made available by the Caltech Environmental Analysis Center, and we gratefully acknowledge support on GC–MS from N. Dalleska. We also gratefully acknowledge Z. Wang for the contribution to mobile app development, R. M. Torrente-Rodríguez for the insulin assay optimization and S. Bao for the valuable inputs. These authors contributed equally: Minqiang Wang, Yiran Yang, Jihong Min. Contributions. W.G., M.W., Y.Y. and J.M. initiated the concept and designed the studies; W.G. supervised the work; M.W., Y.Y. and J.M. led the experiments and collected the overall data; Y.S., J.T., D.M., C.Y. and C.X. contributed to sensor characterization, validation and sample analysis; N.H. contributed to the signal processing and app development. J.S.M., T.K.H. and Z.L. contributed to the design of the human studies. W.G., M.W., Y.Y. and J.M. co-wrote the paper. All authors contributed to the data analysis and provided feedback on the manuscript. Data availability. The main data supporting the results in this study are available within the paper and its Supplementary Information. Source data for Figs. 4 and 5 and for Supplementary Figs. 36 and 39–41 are provided with this paper. All raw and analysed datasets generated during the study are available from the corresponding author on request. Source data are provided with this paper. The authors declare no competing interests. Peer review information. Nature Biomedical Engineering thanks the anonymous reviewers for their contribution to the peer review of this work.

Attached Files

Accepted Version - qt2r8949kg.pdf

Supplemental Material - 41551_2022_916_MOESM1_ESM.pdf

Supplemental Material - 41551_2022_916_MOESM2_ESM.pdf

Supplemental Material - 41551_2022_916_MOESM3_ESM.mp4

Supplemental Material - 41551_2022_916_MOESM4_ESM.mp4

Supplemental Material - 41551_2022_916_MOESM5_ESM.mp4

Supplemental Material - 41551_2022_916_MOESM6_ESM.xlsx

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Additional details

Created:
August 22, 2023
Modified:
December 6, 2023