Since
humanity is rapidly moving toward the era of the Internet
of Things (IoT) and artificial intelligence (AI) to achieve a higher
level of comfort and connection, biocompatible, elastic, and self-healable
soft electronic devices such as wearable sensors are needed to overcome
the traditional silicon-based electronics rigidity. Inspired by catecholic
amino acid (l-3,4-dihydroxyphenylalanine, DOPA) from the mussel foot
plaque of marine organisms and Mytilus galloprovincialis mussels, which contribute significantly to the robust underwater
adhesion of mussels to the surfaces, here, we report the synthesis
and fabrication of a library of materials. These materials comprise
adhesive, self-healable, and stretchable gum-like materials, hydrogels,
and aerogels based on cross-linking of three components of the silk
fibroin (SF) biopolymer, MXene (Ti3C2) two-dimensional
nanosheets, and tannic acid (TA). The synthesis relies on the coordination
of oxidized SF (SF-DOPA), TA, and polydopamine (PDA)-modified MXene
nanosheets with ferric ions to fabricate materials with a mussel-inspired
adhesiveness, mechanical flexibility (stretchability), electrical
conductivity, and self-healing features. To control the type of the
obtained materials as well as their resulting properties, namely,
elasticity and electrical conductivity, the molar ratio of TA, MXene,
and Fe(III) cross-linker as well as pH values was carefully varied
to control the gelation kinetics and phase separation. The resulting
optimized materials consist of highly flexible gum to 3D porous homogeneous
hydrogels and subsequently aerogels after freeze-drying. The stretchability,
electrical conductivity (6.5 × 10–4 S cm–1), human motion sensing performance, and significant
strain sensitivity of the final gums confirmed their remarkable performance
as intriguing next-generation materials for soft-electronic devices,
such as electronic skins and piezoresistive wearable pressure sensors.