TY - JOUR
T1 - Naked-Eye Thiol Analyte Detection via Self-Propagating, Amplified Reaction Cycle
AU - Klemm, Benjamin
AU - Roshanasan, Ardeshir
AU - Piergentili, Irene
AU - van Esch, Jan H.
AU - Eelkema, Rienk
PY - 2023
Y1 - 2023
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85174080447&partnerID=8YFLogxK
U2 - 10.1021/jacs.3c02937
DO - 10.1021/jacs.3c02937
M3 - Article
C2 - 37748772
AN - SCOPUS:85174080447
SN - 0002-7863
VL - 145
SP - 21222
EP - 21230
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 39
ER -