Two-Dimensional Nanosheet-Enhanced Waterborne Polyurethane Eutectogels with Ultrastrength and Superelasticity for Sensitive Strain Sensors

Sensing materials that are ultrastrong but still superelastic and highly sensitive are crucial for meeting the requirements of future flexible sensors. However, these requirements are challenging to satisfy simultaneously due to the internal constraints among these properties. Here, an ultrastrong and superelastic eutectogel is designed and prepared using a waterborne polyurethane (WPU) network enhanced by two-dimensional (2D) nanosheets in a deep eutectic solvent. The 2D nanosheet-induced noncovalent cross-linking endows the prepared eutectogel with superelasticity and flexibility, and its elongation at break reaches 2071%, higher than those of most polymers (<1000%). Meanwhile, this eutectogel also exhibits a high tensile strength (21.6 MPa), which is strong enough to support 20 000 times its own weight. Such a composite design provides a feasible route for preparing eutectogels with outstanding comprehensive functions without trade-offs among these features. In addition, the eutectogel-assembled sensor possesses a high ionic conductivity of 0.225 S/m and a high strain sensitivity of 1.18 kPa–1. Furthermore, it can be integrated into the sensing arrays for multidimensional signal monitoring without diminishing its pristine strength and flexibility. Surprisingly, the eutectogel can be quickly disintegrated in ethanol due to the WPU’s pseudoplastic behavior, providing a competitive way to dispose of waste electronic devices.