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Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules

In situ analysis of multiple biomarkers in the body provides better diagnosis and enables personalized health management. Since many of these biomarkers are redox-active, electrochemical sensors have shown promising analytical capabilities to measure multiple redox-active molecules. However, the ana...

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Autores principales: Biton Hayun, Stav, Shukla, Rajendra P., Ben-Yoav, Hadar
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8875081/
https://www.ncbi.nlm.nih.gov/pubmed/35215630
http://dx.doi.org/10.3390/polym14040717
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author Biton Hayun, Stav
Shukla, Rajendra P.
Ben-Yoav, Hadar
author_facet Biton Hayun, Stav
Shukla, Rajendra P.
Ben-Yoav, Hadar
author_sort Biton Hayun, Stav
collection PubMed
description In situ analysis of multiple biomarkers in the body provides better diagnosis and enables personalized health management. Since many of these biomarkers are redox-active, electrochemical sensors have shown promising analytical capabilities to measure multiple redox-active molecules. However, the analytical performance of electrochemical sensors rapidly decreases in the presence of multicomponent biofluids due to their limited ability to separate overlapping electrochemical signals generated by multiple molecules. Here we report a novel approach to use charged chitosan-modified electrodes to alter the diffusion of ascorbic acid, clozapine, L-homocysteine, and uric acid—test molecules with various molecular charges and molecular weights. Moreover, we present a complementary approach to use chemometrics to decipher the complex set of overlapping signals generated from a mixture of differentially charged redox molecules. The partial least square regression model predicted three out of four redox-active molecules with root mean square error, Pearson correlation coefficient, and R-squared values of 125 µM, 0.947, and 0.894; 51.8 µM, 0.877, and 0.753; 55.7 µM, 0.903, and 0.809, respectively. By further enhancing our understanding of the diffusion of redox-active molecules in chitosan, the in-situ separation of multiple molecules can be enabled, which will be used to establish guidelines for the effective separation of biomarkers.
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spelling pubmed-88750812022-02-26 Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules Biton Hayun, Stav Shukla, Rajendra P. Ben-Yoav, Hadar Polymers (Basel) Article In situ analysis of multiple biomarkers in the body provides better diagnosis and enables personalized health management. Since many of these biomarkers are redox-active, electrochemical sensors have shown promising analytical capabilities to measure multiple redox-active molecules. However, the analytical performance of electrochemical sensors rapidly decreases in the presence of multicomponent biofluids due to their limited ability to separate overlapping electrochemical signals generated by multiple molecules. Here we report a novel approach to use charged chitosan-modified electrodes to alter the diffusion of ascorbic acid, clozapine, L-homocysteine, and uric acid—test molecules with various molecular charges and molecular weights. Moreover, we present a complementary approach to use chemometrics to decipher the complex set of overlapping signals generated from a mixture of differentially charged redox molecules. The partial least square regression model predicted three out of four redox-active molecules with root mean square error, Pearson correlation coefficient, and R-squared values of 125 µM, 0.947, and 0.894; 51.8 µM, 0.877, and 0.753; 55.7 µM, 0.903, and 0.809, respectively. By further enhancing our understanding of the diffusion of redox-active molecules in chitosan, the in-situ separation of multiple molecules can be enabled, which will be used to establish guidelines for the effective separation of biomarkers. MDPI 2022-02-13 /pmc/articles/PMC8875081/ /pubmed/35215630 http://dx.doi.org/10.3390/polym14040717 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Biton Hayun, Stav
Shukla, Rajendra P.
Ben-Yoav, Hadar
Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules
title Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules
title_full Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules
title_fullStr Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules
title_full_unstemmed Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules
title_short Diffusion- and Chemometric-Based Separation of Complex Electrochemical Signals That Originated from Multiple Redox-Active Molecules
title_sort diffusion- and chemometric-based separation of complex electrochemical signals that originated from multiple redox-active molecules
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8875081/
https://www.ncbi.nlm.nih.gov/pubmed/35215630
http://dx.doi.org/10.3390/polym14040717
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