Department of Synthetic Chemistry and Biological Chemistry, Kyoto University , Katsura, Nishikyo-Ku, Kyoto 615-8510, Japan.
J Am Chem Soc. 2015 Mar 11;137(9):3360-5. doi: 10.1021/ja5131534. Epub 2015 Feb 25.
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 (H2O2)-responsive supramolecular hydrogel (BPmoc-F3), together with other enzymes. The nanostructure and mechanical strength of the hybrid BPmoc-F3 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 H2O2, 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.
多组分超分子水凝胶被构建用于灵敏的、肉眼可见的小分子生物标志物检测。树枝状自毁分子和相应的酶作为信号放大系统被稳定地嵌入到过氧化物酶(H2O2)响应的超分子水凝胶(BPmoc-F3)中,同时还加入了其他酶。在没有目标生物标志物的情况下,这些多种成分的掺入并没有显著降低混合 BPmoc-F3 凝胶的纳米结构和机械强度,但可以通过添加生物标志物破坏,这是因为凝胶基质内的多种酶促和化学级联反应共同作用。通过凝胶-溶胶转变检测到的生物标志物(如 H2O2、葡萄糖和尿酸)的灵敏度通过信号放大系统得到显著增强。由这些多组分水凝胶组成的阵列芯片可以检测人血浆样本中高尿酸血症疾病的水平。