Temperature-Invariant Superelastic Multifunctional MXene Aerogels for High-Performance Photoresponsive Supercapacitors and Wearable Strain Sensors

Assembling MXene two-dimensional (2D) nanosheets solely into structurally robust three-dimensional (3D) multifunctional macroarchitectures with temperature-invariant elasticity is significant for widening their potential applications but has remained exceedingly challenging. To this end, a facile freeze-induced co-assembly was developed to allow the disparate integration of MXene 2D nanosheets into the directive heterogeneities to easily customize the controllable 3D architectures for geometry accessibility, structure integrity, and function adaptability. With functionalized cellulose nanocrystal serving as a structural modifier and cross-linking by polyurethane as well as manipulating the directionally ice templating process, multilevel nanostructured configurations with interconnected porous channels could be obtained for biomimetic aerogel electrodes across multiple length scales. Benefiting from the high ion pathway from the low-tortuosity topology, MXene aerogels showed outstanding electrochemical property (225 F/g), high-rate capacity, and temperature-invariant superelasticity (from 0 to 150 °C), which surpassed some of the best reported values. MXene quasi-solid-state supercapacitors presented superior electrochemistry (energy density: 38.5 μWh/cm2) and outstanding cycle ability (86.7% after 4000 cycles). Exhibiting excellent photoresponse capacity, they could be used as an integrated photodetector. More importantly, specially designed bio-mimicking structures with mechanically self-adaptive resilience could promote MXene 3D aerogels to apply in wearable electronic devices, monitoring various human motions. This work will shed light on MXene aerogels for smart and self-powered lightweight electronics.