Carbon nanotube (CNT) forests are highly conductive and possess a large surface area, making them promising as electrode support materials for electrochemical applications including energy storage and water desalination. However, these forests often suffer from mechanical collapse when exposed to liquids, limiting their effectiveness in wet environments. In this study, we explore the use of vapor-phase oxidative molecular layer deposition (oMLD) to deposit thin, redox-active polymer films onto CNT forests to enhance their mechanical and electrochemical properties. We evaluate the mechanical behavior of the polymer-coated CNT forests using nanoindentation compression tests and solvent evaporation tests. The modulus and buckling stress of the forests increase with the thickness of the polymer coating, indicating enhanced mechanical strength conferred by the oMLD process. Furthermore, solvent evaporation tests demonstrate that the morphology of the polymer-coated CNT forests remains undisturbed by surface tension forces, in contrast to uncoated CNT forests which collapse and densify. This preservation of morphology underscores the effectiveness of the polymer coating in protecting the CNT forests from structural degradation in liquid environments. To gain deeper insights, finite element simulations analyze the mechanical properties of both coated and uncoated CNT forests. The simulations reveal that the increase in buckling load scales with the bending stiffness of individual CNTs and their coatings, highlighting the synergistic effect of the polymer coating on the overall forest structure. Finally, electrochemical characterization in aqueous electrolyte indicates an increase in charge capacity with polymer thickness for thin films, and a decrease in charge capacity at high film thicknesses arising from restricted pore volume. This work indicates that oMLD polymer coatings enhance the mechanical strength and electrochemical activity of CNT-based substrates. The findings from this study contribute to the development of more efficient and durable CNT-based electrodes for water desalination and energy storage applications.
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