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Naked-Eye Thiol Analyte Detection via Self-Propagating, Amplified Reaction Cycle
Benjamin Klemm1, Ardeshir Roshanasan1, Irene Piergentili1
1Department of Chemical Engineering, Delft University of Technology, Van der Maasweg 9, 2629 HZ Delft, The Netherlands.
Journal of the American Chemical Society
|September 25, 2023
Summary
This study introduces a novel amplification system for detecting thiol analytes. The system triggers hydrogel degradation, enabling sensitive detection of various thiol-containing molecules.
Area of Science:
- Biomaterials Science
- Analytical Chemistry
- Chemical Engineering
Background:
- Hydrogel scaffolds are widely used in various applications.
- Sensing and detection of thiol analytes are crucial in biological and chemical fields.
- Developing sensitive and efficient detection methods for thiols remains a challenge.
Purpose of the Study:
- To develop a self-propagating amplification system for thiol detection.
- To integrate this system into a hydrogel scaffold for macroscopic degradation.
- To investigate the potential of force-induced hydrogel destruction.
Main Methods:
- A self-propagating amplification cycle involving allylic phosphonium salt and disulfide reduction was designed.
- The amplification system was incorporated into a disulfide cross-linked hydrogel.
- A numerical model was developed to predict system behavior and validated experimentally.
- The system's ability to detect various thiol analytes was tested.
Main Results:
- The amplification cycle exponentially amplifies thiol input, leading to hydrogel degradation.
- Multiple thiol analytes (small molecule, glutathione, DNA, protein) were detected at concentrations from 132 to 0.132 μM.
- The system demonstrated damage-triggered hydrogel destruction initiated by force-generated molecular scission.
Conclusions:
- The developed system offers a sensitive and effective method for detecting thiol analytes.
- Hydrogel degradation serves as a macroscopic signal for thiol presence.
- The discovery of force-induced destruction opens new avenues for smart material applications.
