Hydrogel ionotronics (HI) has been extensively functionalized as artificial skins, soft robotics, and ultra-flexible displays over the recent years, and these applications require the involved materials to sustain prolonged cyclic stretching. However, HI devices suffer from a “shakedown” after prolonged cycling, as the stress-stretch curves change cycle by cycle. This mechanical failure often leads to functional instability of the HI devices, and the current literature discussing their structural origin and associated structure-property-function relationship is scarce. To this end, this work first discloses the molecular network response of HI devices for their shakedown behavior using the in situ small-angle X-ray scattering. Briefly, the stretching-induced orientation of the crosslinked network is unable to be fully relaxed during the cyclic stretching, which in turn leads to the partial disentanglement of the entangled network. Considering this mechanism, a time-dependent constitutive model is then proposed to quantitatively describe the shakedown behavior of HI devices. The model proposed herein precisely predicts the shakedown of HI devices and their corresponding cyclic stress-stretch curves, by using the parameters extracted from initial 70 cycles. Essentially, this work improves the in-depth understanding of fundamental issues related to structure–property-function relationships of HI devices, and thus, provides inspiration and guidance for designing highly stable and functional ionotronic devices.

近年来，水凝胶离子电子学（HI）已被广泛用作人造皮肤、软机器人和超柔性显示器，这些应用需要相关材料来维持长时间的循环拉伸。然而，HI 器件在长时间循环后会出现“震荡”，因为应力-拉伸曲线会逐个循环地变化。这种机械故障通常会导致 HI 设备的功能不稳定，目前讨论它们的结构起源和相关的结构-性能-功能关系的文献很少。为此，这项工作首先揭示了 HI 设备的分子网络响应，用于使用原位的安定行为小角度 X 射线散射。简而言之，在循环拉伸过程中，交联网络的拉伸诱导取向不能完全松弛，这反过来又导致纠缠网络的部分解缠结。考虑到这种机制，然后提出了一个时间相关的本构模型来定量描述 HI 设备的安定行为。本文提出的模型通过使用从最初的 70 个循环中提取的参数，精确地预测了 HI 设备的安定及其相应的循环应力-拉伸曲线。从本质上讲，这项工作提高了对与 HI 器件的结构-性能-功能关系相关的基本问题的深入理解，从而为设计高度稳定和功能强大的离子电子器件提供了灵感和指导。