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用于唾液葡萄糖监测的抗污互穿聚合物网络水凝胶膜的研制。

The development of an antifouling interpenetrating polymer network hydrogel film for salivary glucose monitoring.

机构信息

School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, P. R. China.

出版信息

Nanoscale. 2020 Nov 19;12(44):22787-22797. doi: 10.1039/d0nr05854h.

Abstract

Owing to its rapid response and broad detection range, a phenylboronic acid (PBA)-functionalized hydrogel film-coated quartz crystal microbalance (QCM) sensor is used to non-invasively monitor salivary glucose in diabetic patients. However, nonspecific protein adsorption on the PBA-functionalized hydrogel film can cause dramatic loss of sensitivity and accuracy of the sensor. A traditional zwitterionic polymer surface with ultra-low protein fouling can hinder the interaction of PBA in the hydrogel matrix with glucose molecules owing to its steric hindrance, resulting in poor glucose sensitivity of the sensor. Herein, we developed a novel hydrogel film that enhanced the antifouling properties and sensitivity of the QCM sensor by infiltrating a glucose-sensitive monomer (i.e., PBA) into a zwitterionic polymer brush matrix to form an interpenetrating polymer network (IPN). The IPN hydrogel film could minimize the glucose sensitivity loss since the antifouling polymer distributed in its matrix. Moreover, a stable hydration layer was formed in this film that could prevent water from transporting out of the matrix, thus further improving its antifouling properties and glucose sensitivity. The experimental results confirmed that the IPN hydrogel film possessed excellent resistance to protein fouling by mucin from whole saliva with reductions in adsorption of nearly 88% and could also enhance the glucose sensitivity by nearly 2 fold, compared to the PBA-functionalized hydrogel film. Therefore, the IPN hydrogel film provides improved antifouling properties and sensitivity of the QCM sensor, which paves the way for non-invasive monitoring of low concentrations of glucose in saliva.

摘要

由于其快速响应和广泛的检测范围,一种苯硼酸(PBA)功能化水凝胶膜涂覆的石英晶体微天平(QCM)传感器被用于非侵入式监测糖尿病患者的唾液葡萄糖。然而,PBA 功能化水凝胶膜上的非特异性蛋白质吸附会导致传感器的灵敏度和准确性急剧下降。传统的具有超低蛋白质污染的两性离子聚合物表面由于空间位阻会阻碍水凝胶基质中的 PBA 与葡萄糖分子的相互作用,从而导致传感器对葡萄糖的灵敏度较差。在此,我们开发了一种新型水凝胶膜,通过将葡萄糖敏感单体(即 PBA)渗透到两性离子聚合物刷基质中形成互穿聚合物网络(IPN),从而提高了 QCM 传感器的抗污性能和灵敏度。由于抗污聚合物分布在其基质中,因此 IPN 水凝胶膜可以最大程度地减少葡萄糖灵敏度的损失。此外,在该膜中形成了稳定的水合层,可以防止水从基质中运出,从而进一步提高其抗污性能和葡萄糖灵敏度。实验结果证实,与 PBA 功能化水凝胶膜相比,IPN 水凝胶膜具有出色的抗全唾液粘蛋白污染能力,其吸附量减少了近 88%,并且还可以将葡萄糖灵敏度提高近 2 倍。因此,IPN 水凝胶膜提高了 QCM 传感器的抗污性能和灵敏度,为非侵入式监测唾液中低浓度葡萄糖铺平了道路。

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