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Abstract Durable hydrophobic materials have attracted considerable interest in the last century. Currently, the most popular strategy to achieve hydrophobic coating durability is through the combination of a perfluoro-compound with a mechanically robust matrix to form a composite for coating protection. The matrix structure is typically large (thicker than 10 μm), difficult to scale to arbitrary materials, and incompatible with applications requiring nanoscale thickness such as heat transfer, water harvesting, and desalination. Here, we demonstrate durable hydrophobicity and superhydrophobicity with nanoscale-thick, perfluorinated compound-free polydimethylsiloxane vitrimers that are self-healing due to the exchange of network strands. The polydimethylsiloxane vitrimer thin film maintains excellent hydrophobicity and optical transparency after scratching, cutting, and indenting. We show that the polydimethylsiloxane vitrimer thin film can be deposited through scalable dip-coating on a variety of substrates. In contrast to previous work achieving thick durable hydrophobic coatings by passively stacking protective structures, this work presents a pathway to achieving ultra-thin (thinner than 100 nm) durable hydrophobic films. 

Abstract The emergence of two-dimensional (2D) materials as functional surfaces for sensing, electronics, mechanics, and other myriad applications underscores the importance of understanding 2D material–liquid interactions. The thinness and environmental sensitivity of 2D materials induce novel surface forces that drive liquid interactions. This complexity makes fundamental 2D material–liquid interactions variable. In this review, we discuss the (1) wettability, (2) electrical double layer (EDL) structure, and (3) frictional interactions originating from 2D material–liquid interactions. While many 2D materials are inherently hydrophilic, their wettability is perturbed by their substrate and contaminants, which can shift the contact angle. This modulation of the wetting behavior enables templating, filtration, and actuation. Similarly, the inherent EDL at 2D material–liquid interfaces is easily perturbed. This EDL modulation partially explains the wettability modulation and enables distinctive electrofluidic systems, including supercapacitors, energy harvesters, microfluidic sensors, and nanojunction gating devices. Furthermore, nanoconfinement of liquid molecules at 2D material surfaces arising from a perturbed liquid structure results in distinctive hydrofrictional behavior, influencing the use of 2D materials in microchannels. We expect 2D material–liquid interactions to inform future fields of study, including modulation of the chemical reactivity of 2D materials via tuning 2D material–liquid interactions. Overall, 2D material–liquid interactions are a rich area for research that enables the unique tuning of surface properties, electrical and mechanical interactions, and chemistry. 

Abstract Graphene, owing to its inherent chemical inertness, biocompatibility, and mechanical flexibility, has great potential in guiding cell behaviors such as adhesion and differentiation. However, due to the two-dimensional (2D) nature of graphene, the microfabrication of graphene into micro/nanoscale patterns has been widely adopted for guiding cellular assembly. In this study, we report crumpled graphene, i.e., monolithically defined graphene with a nanoscale wavy surface texture, as a tissue engineering platform that can efficiently promote aligned C2C12 mouse myoblast cell differentiation. We imparted out-of-plane, nanoscale crumpled morphologies to flat graphene via compressive strain-induced deformation. When C2C12 mouse myoblast cells were seeded on the uniaxially crumpled graphene, not only were the alignment and elongation promoted at a single-cell level but also the differentiation and maturation of myotubes were enhanced compared to that on flat graphene. These results demonstrate the utility of the crumpled graphene platform for tissue engineering and regenerative medicine for skeletal muscle tissues.