Development of Redox-Active Nanocomposite Hydrogels for Continuous and Wearable Health Monitoring

开发用于连续可穿戴健康监测的氧化还原活性纳米复合水凝胶

• 批准号: RGPIN-2022-04926
• 负责人: Clifford, Amanda
• 金额: $ 2.4万
• 依托单位: University of British Columbia
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=758188
• 关键词: Development; Redox; Active; Nanocomposite; Hydrogels

Wearable fitness trackers have enabled users to gain insight into their physical health by providing information regarding their activity, sleep, and resting heart rate in real-time. Analogous devices capable of monitoring and managing chronic illnesses such as cancer, cardiovascular, and autoimmune disease would revolutionize medicine by providing patients access to their health data at the point-of-need. Such devices, for example glucose meters, have been developed, but they are limited to detection of analytes that can be directly measured using electroanalytical methods through biocatalytic conversion of the target biomarker (metabolites) or potentiometry (ions). There are limited reports of a wearable device capable of noninvasive monitoring of biomarkers that do not directly produce an electrochemical signal in the presence of target. This is primarily due to the lack of available reagentless assays for biomarkers such as proteins, nucleic acids, and microoorganisms (e.g. bacteria). Most strategies used for portable detection of these biomarkers rely on the use of external reporter molecules and/or reagents, require a separate target-labelling step, or pre-processing of the sample biofluid. Furthermore, the majority are limited to detection of a single biomolecule at one point in time and are highly susceptible to biofouling during operation. The overarching objective of my research program is to enable wearable monitoring of target analytes beyond metabolites and ions by developing new functional materials for reagent-free sensing. My research group will focus on developing new electrochemical strategies, as they are well-suited for translation to wearable monitoring applications. Our approach will be rooted in materials science: rather than using redox-labelled biomolecules as recognition elements, we will explore the use of redox-active (or pseudocapacitive) hydrogels for sensitive and reagentless monitoring of target biomarkers. Previous electrochemical detection strategies used pseudocapacitive gels for voltammetric detection of biomarkers based on amplification of peak current in the presence of analyte. However, they were limited to detection of biomolecules that participated in redox-cycling with the pseudocapacitive transducing element. The proposed work will circumvent this limitation by investigating a previously-unexplored mechanism of detection based on measuring changes in the areal capacitance using cyclic voltammetry. In addition, we will study the effect of tuning both hydrogel chemistry and surface topography, to obtain a surface that is resistant to biofouling and can be deployed in unprocessed sample matrices. This work will benefit all Canadians by ultimately leading to the existence of wearable tools that will eliminate the need for invasive sample collection, expensive equipment, and long wait times for the diagnoses and management of deadly or chronic diseases.

可穿戴健康跟踪器通过实时提供有关他们的活动、睡眠和静息心率的信息，使用户能够深入了解他们的身体健康。能够监测和管理癌症、心血管疾病和自身免疫性疾病等慢性疾病的类似设备将使患者能够在需要时访问他们的健康数据，从而给医学带来革命性的变化。已经开发了这样的设备，例如血糖仪，但它们仅限于对分析物的检测，这些分析物可以通过目标生物标志物(代谢物)或电位法(离子)的生物催化转化，使用电分析方法直接测量。关于一种能够非侵入性地监测生物标志物的可穿戴设备的报道有限，这些生物标志物在靶子存在的情况下不直接产生电化学信号。这主要是由于缺乏对蛋白质、核酸和微生物(例如细菌)等生物标记物的可用的无试剂分析。大多数用于便携式检测这些生物标记物的策略依赖于外部报告分子和/或试剂的使用，需要单独的靶标记步，或样品生物液的前处理。此外，大多数仅限于在一个时间点检测单个生物分子，并且在操作过程中高度容易受到生物污染的影响。我的研究计划的首要目标是通过开发用于无试剂传感的新功能材料，实现对代谢物和离子以外的目标分析物的可穿戴监测。我的研究小组将专注于开发新的电化学策略，因为它们非常适合转换为可穿戴式监控应用。我们的方法将植根于材料科学：我们将探索使用氧化还原活性(或假电容)水凝胶对目标生物标记物进行敏感和无试剂监测，而不是使用氧化还原标记的生物分子作为识别元件。以前的电化学检测策略使用假电容凝胶来检测基于分析物存在下的峰电流放大的生物标志物的伏安。然而，它们仅限于检测与假电容转换元件一起参与氧化还原循环的生物分子。这项拟议的工作将绕过这一限制，通过研究一种以前未探索过的检测机制，该机制基于使用循环伏安法测量面上电容的变化。此外，我们将研究调整水凝胶化学和表面形貌的效果，以获得抗生物污垢和可以部署在未经处理的样品基质中的表面。这项工作将最终导致可穿戴工具的存在，从而使所有加拿大人受益，这些工具将消除对侵入性样本采集、昂贵设备的需求，以及诊断和管理致命或慢性病的漫长等待时间。