Underwater Fabrication of Carbon Nanotube/Coacervate Composites

Soft conductive materials are of interest for a wide range of applications, but their syntheses have remained difficult. Herein, we present a convenient route for underwater fabrication of a composite made of carbon nanotubes (CNTs) and mussel-inspired complex coacervates. The key to success of this method is that CNTs were solubilized very effectively in protocoacervates, which are high-concentration solutions of polyelectrolytes at a pH where only one of them is charged, thereby impeding coacervate formation. Composite materials were formed by the simple injection of CNT-dispersed protocoacervate solutions into water under ambient conditions. The method is simple, fast, and ecofriendly, and composites of CNT-complex coacervate in the form of films or bulk materials were obtained. The composites demonstrated electrical conductivity and tunable mechanical properties, which depended on the concentration of polyelectrolytes and the CNT:protocoacervate ratio. Hence, the composites can be manipulated to attain diverse properties, for examples, tunable reduced modulus (15 to 32 GPa) and hardness (0.3 to 0.7 GPa) as well as an electrical conductivity of up to 4 × 10³ S m^-1.