Electrochemical Diffusion Study in Poly(Ethylene Glycol) Dimethacrylate-Based Hydrogels

E. Melnik, Steffen Kurzhals, G. Mutinati, Valerio Beni, Rainer Hainberger
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Abstract

Hydrogels are of great importance for functionalizing sensors and microfluidics, and poly(ethylene glycol) dimethacrylate (PEG-DMA) is often used as a viscosifier for printable hydrogel precursor inks. In this study, 1–10 kDa PEG-DMA based hydrogels were characterized by gravimetric and electrochemical methods to investigate the diffusivity of small molecules and proteins. Swelling ratios (SRs) of 14.43–9.24, as well as mesh sizes ξ of 3.58–6.91 nm were calculated, and it was found that the SR correlates with the molar concentration of PEG-DMA in the ink (MCI) (SR = 0.1127 × MCI + 8.3256, R2 = 0.9692) and ξ correlates with the molecular weight (Mw) (ξ = 0.3382 × Mw + 3.638, R2 = 0.9451). To investigate the sensing properties, methylene blue (MB) and MB-conjugated proteins were measured on electrochemical sensors with and without hydrogel coating. It was found that on sensors with 10 kDa PEG-DMA hydrogel modification, the DPV peak currents were reduced to 92 % for MB, 73 % for MB-BSA, and 23 % for MB-IgG. To investigate the diffusion properties of MB(-conjugates) in hydrogels with 1–10 kDa PEG-DMA, diffusivity was calculated from the current equation. It was found that diffusivity increases with increasing ξ. Finally, the release of MB-BSA was detected after drying the MB-BSA-containing hydrogel, which is a promising result for the development of hydrogel-based reagent reservoirs for biosensing.
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聚(乙二醇)二甲基丙烯酸酯水凝胶中的电化学扩散研究
水凝胶对于传感器和微流控芯片的功能化具有重要意义,而聚(乙二醇)二甲基丙烯酸酯(PEG-DMA)通常用作可印刷水凝胶前体墨水的增粘剂。本研究采用重量法和电化学法对基于 1-10 kDa PEG-DMA 的水凝胶进行了表征,以研究小分子和蛋白质的扩散性。结果发现,水凝胶的溶胀率(SR)与墨水中 PEG-DMA 的摩尔浓度(MCI)相关(SR = 0.1127 × MCI + 8.3256,R2 = 0.9692),ξ与分子量(Mw)相关(ξ = 0.3382 × Mw + 3.638,R2 = 0.9451)。为了研究传感器的传感特性,在有水凝胶涂层和无水凝胶涂层的电化学传感器上测量了亚甲基蓝(MB)和 MB 共轭蛋白。结果发现,在经过 10 kDa PEG-DMA 水凝胶修饰的传感器上,甲基溴的 DPV 峰值电流降低了 92%,甲基溴-BSA 降低了 73%,甲基溴-IgG 降低了 23%。为了研究甲基溴(-共轭物)在 1-10 kDa PEG-DMA 水凝胶中的扩散特性,根据电流方程计算了扩散率。结果发现,扩散率随着 ξ 的增大而增大。最后,在干燥含 MB-BSA 的水凝胶后,检测到了 MB-BSA 的释放,这对于开发基于水凝胶的生物传感试剂库来说是一个很有前景的结果。
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