Department of Biomedical Engineering, Texas A&M University, College Station, TX, 77843-3120, USA.
Center for Remote Health Technologies Systems, Texas A&M University, College Station, TX, 77843-3120, USA.
J Mater Chem B. 2022 Aug 17;10(32):6118-6132. doi: 10.1039/d2tb01192a.
Glucose biosensors that could be subcutaneously injected and interrogated without a physically connected electrode and transmitter affixed to skin would represent a major advancement in reducing the user burden of continuous glucose monitors (CGMs). Towards this goal, an optical glucose biosensor was formed by strategically tailoring a thermoresponsive double network (DN) membrane to house a phosphorescence lifetime-based glucose sensing assay. This membrane was selected based on its potential to exhibit reduced biofouling 'self-cleaning' due to cyclical deswelling/reswelling . The membrane was strategically tailored to incorporate oxygen-sensitive metalloporphyrin phosphor, Pd -tetra(sulfophenyl)-tetrabenzoporphyrin ([PdPh(SONa)TBP]) (HULK) and glucose oxidase (GOx). Specifically, electrostatic interactions and colvalent bonds were used to stabilize HULK and GOx within the membrane, respectively. Enhancing the oxygen permeability of the membrane was necessary to achieve sensitivity of HULK/GOx to physiological glucose levels. Thus, silicone microparticles were incorporated at two concentrations. Key properties of -0.25 and -0.5 microparticle-containing compositions were compared to a control having no microparticles (-0). The discrete nature of the silicone microparticles maintained the desired thermosensitivity profile and did not impact water content. While the modulus decreased with silicone microparticle content, membranes were more mechanically robust a conventional hydrogel. -0.25, owing to apparent phase separation, displayed greater glucose diffusion and oxygen permeability -0.5. Furthermore, -0.25 biosensors exhibited the greatest glucose sensitivity range of 100 to 300 mg dL only 100 to 150 mg dL for both -0 and -0.5 biosensors.
能够通过皮下注射并在没有物理连接的电极和发射器贴附在皮肤上进行检测的葡萄糖生物传感器,将代表着降低连续血糖监测器(CGM)用户负担的重大进展。为此,通过策略性地调整热响应双网络(DN)膜来容纳基于磷光寿命的葡萄糖传感测定法,形成了光学葡萄糖生物传感器。选择该膜是基于其由于周期性溶胀/再溶胀而表现出减少生物污垢“自清洁”的潜力。该膜经过策略性地调整,以纳入氧敏感的金属卟啉荧光团、钯-四(磺苯基)-四苯并卟啉([PdPh(SONa)TBP])(HULK)和葡萄糖氧化酶(GOx)。具体而言,分别使用静电相互作用和共价键来稳定膜中的 HULK 和 GOx。为了提高膜对氧气的通透性,从而使 HULK/GOx 对生理葡萄糖水平具有敏感性,因此掺入了两种浓度的硅酮微球。比较了含有-0.25 和-0.5 微球的两种组成物的关键特性与不含微球的对照物(-0)。硅酮微球的离散性质保持了所需的热灵敏度特性,并且不影响水含量。尽管随着硅酮微球含量的增加,模量降低,但膜的机械强度比传统水凝胶更高。由于明显的相分离,-0.25 显示出更大的葡萄糖扩散和氧气通透性,而-0.5 则相反。此外,-0.25 生物传感器仅在 100 至 150 mg dL 范围内显示出 100 至 300 mg dL 的最大葡萄糖灵敏度范围,而-0 和-0.5 生物传感器的范围均为 100 至 150 mg dL。