Cui Yaoxuan, Duan Wei, Jin Yao, Wo Fangjie, Xi Fengna, Wu Jianmin
Institute of Analytical Chemistry, Department of Chemistry, Zhejiang University, Hangzhou 310058, China.
Department of Chemistry, Zhejiang Sci-Tech University, Hangzhou 310018, China.
ACS Sens. 2020 Jul 24;5(7):2096-2105. doi: 10.1021/acssensors.0c00718. Epub 2020 Jun 22.
Noninvasive and visual monitoring of glucose is highly desirable for diabetes diagnostics and long-term home-based health management. Owing to the correlation of the glucose level between blood and sweat, on-body sweat glucose detection provides potential for noninvasive healthcare but is highly challenging. Herein, we for the first time demonstrate a wearable skin pad based on the ratiometric fluorescent nanohybrid, which can realize noninvasive and visual monitoring of sweat glucose. Luminescent porous silicon (PSi) particles, which have a porous structure and oxidation-responsive photoluminescence decay, are chosen to load (adsorb or entrap) carbon quantum dots (CQDs) for the construction of the dual fluorescence nanohybrid. Bimetallic (Au and Ag) nanoparticles (BiM) are also co-decorated on the PSi particle to improve detection sensitivity by enhancing PSi's initial fluorescence and oxidation kinetics. Owing to the efficient fluorescence resonance energy transfer effect, BiM-CQDs@PSi initially exhibits PSi's red fluorescence with complete quenching of CQDs's blue fluorescence. The oxidation of PSi triggered by hydrogen peroxide (HO) weakens the FRET effect and decays PSi's fluorescence, causing ratiometric fluorescence to change from red (PSi) to blue (CQDs). A wearable skin pad is easily fabricated by co-immobilization of BiM-CQDs@PSi and glucose oxidase (GOX) in a transparent and biocompatible chitosan film supported by an adhesive polyurethane membrane. When the skin pad is attached on the body, the same ratiometric fluorescence transition (red → blue) is observed upon the stimulation of HO generated in GOX-catalyzed oxidation of sweat glucose. Based on the strong correlation between the ratio of the fluorescence change and sweat glucose level, clinical tests toward diabetics and healthy volunteers can clearly indicate hyperglycemia.
对于糖尿病诊断和长期家庭健康管理而言，对葡萄糖进行无创且可视化监测是非常必要的。由于血液和汗液中葡萄糖水平存在相关性，体表汗液葡萄糖检测为无创医疗保健提供了可能，但极具挑战性。在此，我们首次展示了一种基于比率荧光纳米杂化物的可穿戴皮肤贴片，它能够实现对汗液葡萄糖的无创可视化监测。选择具有多孔结构和氧化响应光致发光衰减特性的发光多孔硅（PSi）颗粒来负载（吸附或包封）碳量子点（CQDs），以构建双荧光纳米杂化物。双金属（Au和Ag）纳米颗粒（BiM）也共修饰在PSi颗粒上，通过增强PSi的初始荧光和氧化动力学来提高检测灵敏度。由于有效的荧光共振能量转移效应，BiM-CQDs@PSi最初呈现PSi的红色荧光，而CQDs的蓝色荧光完全猝灭。过氧化氢（HO）引发的PSi氧化会减弱FRET效应并衰减PSi的荧光，导致比率荧光从红色（PSi）变为蓝色（CQDs）。通过将BiM-CQDs@PSi和葡萄糖氧化酶（GOX）共固定在由粘性聚氨酯膜支撑的透明且生物相容的壳聚糖膜中，可轻松制备可穿戴皮肤贴片。当皮肤贴片附着在身体上时，在GOX催化汗液葡萄糖氧化产生的HO刺激下，会观察到相同的比率荧光转变（红色→蓝色）。基于荧光变化比率与汗液葡萄糖水平之间的强相关性，针对糖尿病患者和健康志愿者的临床试验能够清晰地指示高血糖情况。
