Chemical‐Physical Synergistic Assembly of MXene/CNT Nanocoatings in Silicone Foams for Reliable Piezoresistive Sensing in Harsh Environments

Abstract Owing to their high sensitivity across a wide stress range, mechanical reliability, and rapid response time, flexible polymer foam piezoresistive sensors have been extensively used in various fields. The reliable application of these sensors under harsh environments, however, is severely limited by structural devastation and poor interfacial bonding between polymers and conductive nanoparticles. To address the above issues, robust MXene/CNT nanocoatings on the foam surface, where the chemical assembly of MXene nanosheets and the physical anchoring of CNTs lead to strong interfacial bonding, are designed and described, which endows foams with structural reliability and unexpected multi‐functionalities without compromising their instinct properties. The optimized foam nanocomposites thus maintain outstanding wide‐temperature flexibility (−60–210 °C) and elasticity (≈3% residual strain after 1000 cycles). Moreover, the nanocomposites display good sensitivity at a relatively wide stress range of 0–70% and remarkable stability under acidic and alkaline settings. Furthermore, the foams with exceptional fire resistance (UL‐94 V‐0 rating) can provide stable sensing behavior (over 300 cycles) even after being exposed to flames for 5 s, making them one of the most reliable sensing materials so far. Clearly, this work widens applications of flexible piezoresistive sensors based on silicone foam nanocomposites for various harsh environments.