Chemically Reactive Supramolecular Hydrogel Coupled with a Signal Amplification System for Enhanced Analyte Sensitivity

摘要

Multicomponent supramolecular hydrogels are constructed for sensitive, naked-eye detection of small-molecule biomarkers. A dendritic self-immolative molecule and the corresponding enzyme as a signal amplification system were stably embedded in a hydrogen peroxide (H_2O_2)-responsive supramolecular hydrogel (BPmoc-F_3), together with other enzymes. The nanostructure and mechanical strength of the hybrid BPmoc-F_3 gel were not substantially diminished by incorporation of these multiple components in the absence of target biomarkers, but could be destroyed by addition of the biomarker through the multiple enzymatic and chemical cascade reactions operating in combination within the gel matrix. The sensitivity to biomarkers such as H_2O_2 glucose, and uric acid, detected by gel-sol transition, was significantly enhanced by the signal amplification system. An array chip consisting of these multicomponent hydrogels enabled the detection of the level of hyperuricemia disease in human plasma samples.