In situ molecular permeation of liquid cationic polymers into solid anionic polymer films enabling self-adaptive adhesion of hydrogel biosensors

Abstract

Self-adaptive adhesion is essential for hydrogel sensors. However, the traditional protocol involves covering a pre-prepared hydrogel sensor on a tested surface. As a result, the sensor cannot achieve self-adaptive adhesion owing to an air-layer hindrance between the sensor and tested surface, which inevitably leads to the loss of critical biological signals. To address the issue of air-layer hindrance, this work proposes an in situ permeation method that enables the self-adaptive adhesion of hydrogel biosensors on various surfaces. After applying a liquid solution of poly(methacrylamido propyl trimethyl ammonium chloride-co-acrylamide) (poly(MPTAC-co-AM)) on the testing surface, a thin film of poly(acrylic aminoethane sulfonic acid-co-acrylamide) (poly(AASA-co-AM)) is applied, where the electrostatic interaction between –SO₃⁻ and –Me₃N⁺ facilitates rapid permeation of the solution into the solid film, leading to the formation of a hydrogel layer in situ. The coating of liquid poly(MPTAC-co-AM) sweeps away the air layer and works as a natural glue, enabling a strong bonding interaction between the hydrogel layer and the tested surface. Such a hydrogel layer is very thin (microscale), and can retain its self-adaptive adhesion even with deformation of the tested surface. When it is applied on the surface of an active frog heart, the weak heartbeats can be transduced to electrical signals. Moreover, this self-adaptive adhesion can work on both soft and hard surfaces including biological tissues, metals, rubbers, ceramics, and glass. Therefore, this in situ permeation method enables the hydrogel layer to detect weak dynamic changes on various soft and hard surfaces, which might offer a new pathway for physiological signal monitoring.