Tough and Recyclable Phase-Separated Supramolecular Gels via a Dehydration-Hydration Cycle.

Hydrogels are compelling materials for emerging applications including soft robotics and autonomous sensing. Mechanical stability over an extensive range of environmental conditions and considerations of sustainability, both environmentally benign processing and end-of-life use, are enduring challenges. To make progress on these challenges, we designed a dehydration-hydration approach to transform soft and weak hydrogels into tough and recyclable supramolecular phase-separated gels (PSGs) using water as the only solvent. The dehydration-hydration approach led to phase separation and the formation of domains consisting of strong polymer-polymer interactions that are critical for forming PSGs. The phase-separated segments acted as robust, physical cross-links to strengthen PSGs, which exhibited enhanced toughness and stretchability in its fully swollen state. PSGs are not prone to overswelling or severe shrinkage in wet conditions and show environmental tolerance in harsh conditions, e.g., solutions with pH between 1 and 14. Finally, we demonstrate the use of PSGs as strain sensors in air and aqueous environments.

Solvent-induced electrochemistry at an electrically asymmetric carbon Janus particle.

Chemical doping through heteroatom substitution is often used to control the Fermi level of semiconductor materials. Doping also occurs when surface adsorbed molecules modify the Fermi level of low dimensional materials such as carbon nanotubes. A gradient in dopant concentration, and hence the chemical potential, across such a material generates usable electrical current. This opens up the possibility of creating asymmetric catalytic particles capable of generating voltage from a surrounding solvent that imposes such a gradient, enabling electrochemical transformations. In this work, we report that symmetry-broken carbon particles comprised of high surface area single-walled carbon nanotube networks can effectively convert exothermic solvent adsorption into usable electrical potential, turning over electrochemical redox processes in situ with no external power supply. The results from ferrocene oxidation and the selective electro-oxidation of alcohols underscore the potential of solvent powered electrocatalytic particles to extend electrochemical transformation to various environments.