Protein Crystallization-Mediated Self-Strengthening of High-Performance Printable Conducting Organohydrogels

Conductive polymers have many advanced applications, but there is still an important target in developing a general and straightforward strategy for printable, mechanically stable, and durable organohydrogels with typical conducting polymers of, for example, polypyrrole, polyaniline, or poly(3,4-ethylenedioxythiophene). Here we report a protein crystallization-mediated self-strengthening strategy to fabricate printable conducting organohydrogels with the combination of rational photochemistry design. Such organohydrogels are one-step prepared via rapidly and orthogonally controllable photopolymerizations of pyrroles and gelatin protein in tens of seconds. As-prepared conducting organohydrogels are patterned and printed to complicated structures via shadow-mask lithography and 3D extrusion technology. The mild photocatalytic system gives the transition metal carbide/nitride (MXene) component high stability during the oxidative preparation process and storage. Controlling water evaporation promotes gelatin crystallization in the as-prepared organohydrogels that significantly self-strengthens their mechanical property and stability in a broad temperature range and durability against continuous friction treatment without introducing guest functional materials. Also, these organohydrogels have commercially electromagnetic shielding, thermal conducting properties, and temperature- and light-responsibility. To further demonstrate the merits of this simple strategy and as-prepared organohydrogels, prism arrays, as proofs-of-concept, are printed and applied to make wearable triboelectric nanogenerators. This self-strengthening process and 3D-printability can greatly improve their voltage, charge, and current output performances compared to the undried and flat samples.