Graphene oxide (GO) sheets have been used to construct various bulk forms of GO and graphene-based materials through solution-based processing techniques. Here, we report a highly cohesive dough state of GO with tens of weight percent loading in water without binder-like additives. The dough state can be diluted to obtain gels or dispersions, and dried to yield hard solids. It can be kneaded without leaving stains, readily reshaped, connected, and further processed to make bulk GO and graphene materials of arbitrary form factors and tunable microstructures. The doughs can be transformed to dense glassy solids of GO or graphene without long-range stacking order of the sheets, which exhibit isotropic and much enhanced mechanical properties due to hindered sliding between the sheets. GO dough is also found to be a good support material for electrocatalysts as it helps to form compliant interface to access the active particles.
Localized corrosion involves the selective attack of a metal at a small, exposed site. This can be particularly devastating for load‐bearing structures, which can fail catastrophically even with very little material loss. Unfortunately, local corrosion is difficult to prevent, predict, and detect. Corrosion can be prevented by barrier coatings, however, imperfections such as pinholes and scratches, can expose small areas of metal and eventually lead to localized corrosion. Herein, a new strategy for self‐healing, damage‐tolerant coatings that can mitigate localized corrosion is presented. The new self‐healing system consists of microcapsule‐thickened low‐viscosity oil and exhibits length scale‐dependent viscosity. Macroscopically, the coating is viscous due to the formation of a 3D particle network, which allows it to stick to vertical metal surfaces against gravity and turbulent flow. Microscopically, the oil exhibits low viscosity and can rapidly flow to damaged areas to re‐establish the particle network. The coating exhibits remarkable barrier properties and protects metal from corrosion for a long time. Moreover, the coating is able to repeatedly self‐heal over the same area hundreds of times over. The strategy described here illustrates how contradicting material properties (e.g., viscosity) co‐exist in a “smart” material system by accommodating them at different length scales.
Low-viscosity oils could potentially act as self-healing barrier coatings because they can readily flow and reconnect to heal minor damage. For the same reason, however, they typically do not form stable coatings on metal surfaces. Increasing viscosity helps to stabilize the oil coating, but it also slows down the healing process. Here, we report a strategy for creating highly stable oil coatings on metal surfaces without sacrificing their remarkable self-healing properties. Low-viscosity oil films can be immobilized on metal surfaces using lightweight microcapsules as thickeners, which form a dynamic network to prevent the creep of the coating. When the coating is scratched, oil around the opening can rapidly flow to cover the exposed area, reconnecting the particle network. Use of these coatings as anticorrosion barriers is demonstrated. The coatings can be easily applied on metal surfaces, including those with complex geometries, both in air or under water, and remain stable even in turbulent water. They can protect metal in corrosive environments for extended periods of time and can self-heal repeatedly when scratched at the same spot. Such a strategy may offer effective mitigation of the dangerous localized corrosion aggravated by minor imperfections or damage in protective coatings, which are typically hard to prevent or detect, but can drastically degrade metal properties.
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