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Naked-Eye Thiol Analyte Detection via Self-Propagating, Amplified Reaction Cycle.


ABSTRACT: We present an approach for detecting thiol analytes through a self-propagating amplification cycle that triggers the macroscopic degradation of a hydrogel scaffold. The amplification system consists of an allylic phosphonium salt that upon reaction with the thiol analyte releases a phosphine, which reduces a disulfide to form two thiols, closing the cycle and ultimately resulting in exponential amplification of the thiol input. When integrated in a disulfide cross-linked hydrogel, the amplification process leads to physical degradation of the hydrogel in response to thiol analytes. We developed a numerical model to predict the behavior of the amplification cycle in response to varying concentrations of thiol triggers and validated it with experimental data. Using this system, we were able to detect multiple thiol analytes, including a small molecule probe, glutathione, DNA, and a protein, at concentrations ranging from 132 to 0.132 μM. In addition, we discovered that the self-propagating amplification cycle could be initiated by force-generated molecular scission, enabling damage-triggered hydrogel destruction.

SUBMITTER: Klemm B 

PROVIDER: S-EPMC10557148 | biostudies-literature | 2023 Oct

REPOSITORIES: biostudies-literature

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Naked-Eye Thiol Analyte Detection via Self-Propagating, Amplified Reaction Cycle.

Klemm Benjamin B   Roshanasan Ardeshir A   Piergentili Irene I   van Esch Jan H JH   Eelkema Rienk R  

Journal of the American Chemical Society 20230925 39


We present an approach for detecting thiol analytes through a self-propagating amplification cycle that triggers the macroscopic degradation of a hydrogel scaffold. The amplification system consists of an allylic phosphonium salt that upon reaction with the thiol analyte releases a phosphine, which reduces a disulfide to form two thiols, closing the cycle and ultimately resulting in exponential amplification of the thiol input. When integrated in a disulfide cross-linked hydrogel, the amplificat  ...[more]

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