School of Chemistry and Molecular Engineering, Shanghai Key Laboratory for Urban Ecological Processes and Eco-Restoration , East China Normal University , 500 Dongchuan Road , Shanghai 200241 , People's Republic of China.
Anal Chem. 2019 Nov 5;91(21):14029-14035. doi: 10.1021/acs.analchem.9b03646. Epub 2019 Oct 25.
The great pain and stress from finger-prick glucose measurements have resulted in great motivation to find noninvasive glucose monitoring technologies where salivary glucose measurement is desirable. However, the relative low concentration of glucose and coexisting chemicals in saliva challenges the sensitive and selective salivary glucose detection. In this article, we have rationally designed and constructed a salivary glucose sensor by modifying the inner wall of the Au-decorated glass nanopore with stimuli-responsive copolymer poly(3-(acryloylthioureido) phenylboronic acid---isopropylacrylamide) (denoted as PATPBA--PNIPAAm) via Au-S interaction. Notably, upon recognition of glucose, the copolymer could undergo a wettability switch and pa shifts in the boronic acid functional groups, which significantly regulated the ion transport through nanopores, thus showing improved sensitivity with the detection limit of 1 nM. Moreover, benefiting from the multivalent boronic acid-glucose interaction and the cooperation of thiourea units, the copolymer exhibited good selectivity for glucose detection against the coexisting saccharides and other biological molecules in saliva. The nanopores with well-demonstrated analytical performance were finally applied for monitoring glucose in saliva. Together, this work unveiled a new platform for glucose detection in saliva, and promised to provide a new strategy for detecting other biomolecules in accessible biofluid involved in physiological and pathological events.
指尖血糖测量带来的巨大疼痛和压力，促使人们积极寻求非侵入性血糖监测技术，而唾液血糖测量则是理想的选择。然而，唾液中葡萄糖浓度相对较低，且共存的化学物质种类繁多，这对敏感且具有选择性的唾液葡萄糖检测提出了挑战。在本文中，我们通过 Au-S 相互作用，将响应型共聚体聚（3-（丙烯酰硫脲基）苯基硼酸-异丙基丙烯酰胺）（记为 PATPBA--PNIPAAm）修饰在 Au 修饰的玻璃纳米孔内壁，合理设计并构建了一种唾液葡萄糖传感器。值得注意的是，共聚体在识别葡萄糖后，能够发生润湿性转变和硼酸官能团的 pA 位移，这显著调节了纳米孔中的离子传输，从而表现出更好的灵敏度，检测限低至 1 nM。此外，得益于多价硼酸-葡萄糖相互作用和硫脲单元的协同作用，该共聚体对唾液中存在的共存糖类和其他生物分子表现出良好的选择性。最后，具有良好分析性能的纳米孔被用于监测唾液中的葡萄糖。综上所述，本工作为唾液中的葡萄糖检测提供了一个新平台，并有望为检测涉及生理和病理事件的其他可及生物体液中的生物分子提供一种新策略。
