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      Printed, Flexible Lactate Sensors: Design Considerations Before Performing On-Body Measurements

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          Abstract

          This work reports the process of sensor development, optimization, and characterization before the transition to on-body measurements can be made. Sensors using lactate oxidase as a sensing mechanism and tetrathiafulvalene as a mediator were optimized for sporting applications. Optimized sensors show linear range up to 24 mM lactate and sensitivity of 4.8 μA/mM which normalizes to 68  μA*cm −2/mM when accounting for surface area of the sensor. The optimized sensors were characterized 3 different ways: using commercially available reference and counter electrodes, using printed reference and counter electrodes, and using a printed reference electrode with no counter electrode. Sensors intended for measuring sweat must be selective in the presence of sweat constituents. Thus, in addition to traditional characterization in pH 7.0 buffer, we characterized sensor performance in solutions intended to approximate sweat. Sensor performance in pH 7.0 buffer solution was not reflective of sensor performance in artificial sweat, indicating that further characterization is necessary between sensor measurement in pH 7.0 buffer and on-body measurements. Furthermore, we performed enzyme activity measurements and sensor measurements concurrently in five different salts individually, finding that while NH 4Cl and MgCl 2 do not affect enzyme activity or sensor performance in physiologically relevant ranges of salt concentration, NaCl concentration or KCl concentration decreases enzyme activity and sensor current. On the other hand, CaCl 2 induced a nonlinear change in sensor performance and enzyme activity with increasing salt concentration.

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          Electrochemical tattoo biosensors for real-time noninvasive lactate monitoring in human perspiration.

          The present work describes the first example of real-time noninvasive lactate sensing in human perspiration during exercise events using a flexible printed temporary-transfer tattoo electrochemical biosensor that conforms to the wearer's skin. The new skin-worn enzymatic biosensor exhibits chemical selectivity toward lactate with linearity up to 20 mM and demonstrates resiliency against continuous mechanical deformation expected from epidermal wear. The device was applied successfully to human subjects for real-time continuous monitoring of sweat lactate dynamics during prolonged cycling exercise. The resulting temporal lactate profiles reflect changes in the production of sweat lactate upon varying the exercise intensity. Such skin-worn metabolite biosensors could lead to useful insights into physical performance and overall physiological status, hence offering considerable promise for diverse sport, military, and biomedical applications.
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            Nucleation.

            Crystallization starts with nucleation and control of nucleation is crucial for the control of the number, size, perfection, polymorphism and other characteristics of crystalline materials. This is particularly true for crystallization in solution, which is an essential part of processes in the chemical and pharmaceutical industries and a major step in physiological and pathological phenomena. There have been significant recent advances in the understanding of the mechanism of nucleation of crystals in solution. The foremost of these are the two-step mechanism of nucleation and the notion of the solution-crystal spinodal. According to the two-step mechanism, the crystalline nucleus appears inside pre-existing metastable clusters of size several hundred nanometers, which consist of dense liquid and are suspended in the solution. While initially proposed for protein crystals, the applicability of this mechanism has been demonstrated for small molecule organic materials, colloids, polymers, and biominerals. This mechanism helps to explain several long-standing puzzles of crystal nucleation in solution: nucleation rates which are many orders of magnitude lower than theoretical predictions, the significance of the dense protein liquid, and others. At high supersaturations typical of most crystallizing systems, the generation of crystal embryos occurs in the spinodal regime, where the nucleation barrier is negligible. The solution-crystal spinodal helps to understand the role of heterogeneous substrates in nucleation and the selection of crystalline polymorphs. Importantly, these ideas provide powerful tools for control of the nucleation process by varying the solution thermodynamic parameters.
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              The crystal structure of the 1:1 radical cation–radical anion salt of 2,2'-bis-l,3-dithiole (TTF) and 7,7,8,8-tetracyanoquinodimethane (TCNQ)

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                Author and article information

                Contributors
                acarias@eecs.berkeley.edu
                Journal
                Sci Rep
                Sci Rep
                Scientific Reports
                Nature Publishing Group UK (London )
                2045-2322
                23 September 2019
                23 September 2019
                2019
                : 9
                : 13720
                Affiliations
                ISNI 0000 0001 2181 7878, GRID grid.47840.3f, University of California Berkeley, Electrical Engineering and Computer Science, ; Berkeley, CA 94720 United States
                Article
                49689
                10.1038/s41598-019-49689-7
                6757068
                31548553
                aeb9197c-03fc-47a6-9d2e-69d0d15be89b
                © The Author(s) 2019

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 15 May 2019
                : 27 August 2019
                Funding
                Funded by: FundRef https://doi.org/10.13039/100000001, National Science Foundation (NSF);
                Award ID: DGE 1752814
                Award ID: 1610899
                Award ID: DGE 1106400
                Award ID: 1610899
                Award ID: 1610899
                Award Recipient :
                Funded by: FundRef https://doi.org/10.13039/100002418, Intel Corporation (Intel);
                Funded by: Bakar Fellowship
                Categories
                Article
                Custom metadata
                © The Author(s) 2019

                Uncategorized
                biomedical materials,electrical and electronic engineering,enzymes,enzyme mechanisms

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