Wikeley, Simon M;
Przybylowski, Jakub;
Gardiner, Jordan E;
James, Tony D;
Fletcher, Philip J;
Isaacs, Mark A;
Lozano-Sanchez, Pablo;
... Marken, Frank; + view all
(2024)
Pyrene-Appended Boronic Acids on Graphene Foam Electrodes Provide Quantum Capacitance-Based Molecular Sensors for Lactate.
ACS Sensor
10.1021/acssensors.4c00027.
(In press).
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Abstract
Molecular recognition and sensing can be coupled to interfacial capacitance changes on graphene foam surfaces linked to double layer effects and coupled to enhanced quantum capacitance. 3D graphene foam film electrodes (Gii-Sens; thickness approximately 40 μm; roughness factor approximately 100) immersed in aqueous buffer media exhibit an order of magnitude jump in electrochemical capacitance upon adsorption of a charged molecular receptor based on pyrene-appended boronic acids (here, 4-borono-1-(pyren-2-ylmethyl)pyridin-1-ium bromide, or abbreviated T1). This pyrene-appended pyridinium boronic acid receptor is employed here as a molecular receptor for lactate. In the presence of lactate and at pH 4.0 (after pH optimization), the electrochemical capacitance (determined by impedance spectroscopy) doubles again. Lactic acid binding is expressed with a Hillian binding constant (Klactate = 75 mol-1 dm3 and α = 0.8 in aqueous buffer, Klactate = 460 mol-1 dm3 and α = 0.8 in artificial sweat, and Klactate = 340 mol-1 dm3 and α = 0.65 in human serum). The result is a selective molecular probe response for lactic acid with LoD = 1.3, 1.4, and 1.8 mM in aqueous buffer media (pH 4.0), in artificial sweat (adjusted to pH 4.7), and in human serum (pH adjusted to 4.0), respectively. The role of the pyrene-appended boronic acid is discussed based on the double layer structure and quantum capacitance changes. In the future, this new type of molecular capacitance sensor could provide selective enzyme-free analysis without analyte consumption for a wider range of analytes and complex environments.
| Type: | Article |
|---|---|
| Title: | Pyrene-Appended Boronic Acids on Graphene Foam Electrodes Provide Quantum Capacitance-Based Molecular Sensors for Lactate |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acssensors.4c00027 |
| Publisher version: | https://doi.org/10.1021/acssensors.4c00027 |
| Language: | English |
| Additional information: | This publication is licensed under CC-BY 4.0.This publication is licensed under CC-BY 4.0. License Summary* You are free to share (copy and redistribute) this article in any medium or format and to adapt (remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: cc licence Creative Commons (CC): This is a Creative Commons license. ny licence Attribution (BY): Credit must be given to the creator. View full license *Disclaimer This summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. cc licence by licence |
| Keywords: | graphene foam, lactate sensor, molecular capacitance, quantum capacitance, wearable sensor |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10189337 |
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