ABSTRACT
Surface-associated bacterial communities, known as biofilms, are responsible for a broad spectrum of infections in humans. Recent studies have indicated that surfaces containing nanoscale protrusions, like those in dragonfly wings, create a hostile niche for bacterial colonization and biofilm growth. This functionality has been mimicked on metals and semiconductors by creating nanopillars and other high aspect ratio nanostructures at the interface of these materials. However, bactericidal topographies have not been reported on clinically relevant hydrogels and highly compliant polymers, mostly because of the complexity of fabricating nanopatterns in hydrogels with precise control of the size that can also resist aqueous immersion. Here, we report the fabrication of bioinspired bactericidal nanostructures in bacterial cellulose (BC) hydrogels using low-energy ion beam irradiation. By challenging the currently accepted view, we show that the nanostructures grown in BC affect preferentially stiff membranes like those of the Gram-positive bacteria Bacillus subtilis in a time-dependent manner and, to a lesser extent, the more deformable and softer membrane of Escherichia coli. Moreover, the nanostructures in BC did not affect the viability of murine preosteoblasts. Using single-cell analysis, we demonstrate that indeed B. subtilis requires less force than E. coli to be penetrated by nanoprobes with dimensions comparable to those of the nanostructured BC, providing the first direct experimental evidence validating a mechanical model of membrane rupture via a tension-induced mechanism within the activation energy theory. Our findings bridge the gap between mechano-bactericidal surfaces and low-dimensional materials, including single-walled carbon nanotubes and graphene nanosheets, in which a higher bactericidal activity toward Gram-positive bacteria has been extensively reported. Our results also demonstrate the ability to confer bactericidal properties to a hydrogel by only altering its topography at the nanoscale and contribute to a better understanding of the bacterial mechanobiology, which is fundamental for the rational design bactericidal topographies.
ABSTRACT
Nanoscale carbon lubricants such as graphene, have garnered increased interest as protective surface coatings for devices, but its tribological properties have been shown to depend on its interactions with the underlying substrate surface and its degree of surface conformity. This conformity is especially of interest as real interfaces exhibit roughness on the order of â¼10 nm that can dramatically impact the contact area between the graphene film and the substrate. To examine the combined effects of surface interaction strength and roughness on the frictional properties of graphene, a combination of Atomic Force Microscopy (AFM) and Raman microspectroscopy has been used to explore substrate interactions and the frictional properties of single and few-layer graphene as a coating on silica nanoparticle films, which yield surfaces that mimic the nanoscaled asperities found in realistic devices. The interactions between the graphene and the substrate have been controlled by comparing their binding to hydrophilic (silanol terminated) and hydrophobic (octadecyltrichlorosilane modified) silica surfaces. AFM measurements revealed that graphene only partially conforms to the rough surfaces, with decreasing conformity, as the number of layers increase. Under higher mechanical loading the graphene conformity could be reversibly increased, allowing for a local estimation of the out-of-plane bending modulus of the film. The frictional properties were also found to depend on the number of layers, with the largest friction observed on single layers, ultimately decreasing to that of bulk graphite. This trend however, was found to disappear, depending on the tip-sample contact area and interfacial shear strain of the graphene associated with its adhesion to the substrate.