This review focuses on recent developments in the use of 2D nanomaterials for controlling the frictional properties of surfaces and interfaces. While materials such as MoS 2 and graphite have been investigated for some time, a host of other layered nanomaterials have emerged as alternatives for friction modification. These advanced lubrication schemes provide an opportunity to address growing needs in energy and materials efficiency and device compatibility, offering improved boundary and solid lubrication of contacting and sliding interfaces. Here, we describe both computational and experimental investigations of the mechanisms and implementations of 2D nanomaterials in the lubrication of interfaces.
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 ∼10 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.
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.
The industrial use and widespread application of carbon-based nanomaterials have caused a rapid increase in their production over the last decades. However, toxicity of these materials is not fully known and is still being investigated for potential human and ecological health risks. Detecting carbon-based nanomaterials in the environment using current analytical methods is problematic, making environmental fate and transport modeling a practical way to estimate environmental concentrations and assess potential ecological risks. The Water Quality Analysis Simulation Program 8 (WASP8) is a dynamic, spatially resolved fate and transport model for simulating exposure concentrations in surface waters and sediments. Recently, WASP has been updated to incorporate processes for simulating the fate and transport of nanomaterials including heteroaggregation and phototransformation. This study examines the fate and transport of multiwalled carbon nanotubes (MWCNT), graphene oxide (GO) and reduced graphene oxide (rGO) in four aquatic ecosystems in the southeastern United States. Sites include a seepage lake, a coastal plains river, a piedmont river and an unstratified, wetland lake. A hypothetical 50-year release is simulated for each site-nanomaterial pair to analyze nanomaterial distribution between the water column and sediments. For all nanomaterials, 99% of the mass loaded moves though systems of high and low residence times without being heteroaggregated and deposited in the sediments. However, significant accumulation in the sediments does occur over longer periods of time. Results show that GO and rGO had the highest mass fraction in the water column of all four sites. MWCNT were found predominantly in the sediments of the piedmont river and seepage lake but were almost entirely contained in the water column of the coastal plains river and wetland lake. Simulated recovery periods following the release estimate 37+ years for lakes and 1-4 years Disclaimer This paper has been reviewed in accordance with the U.S. Environmental Protection Agency's peer and administrative review policies and approved for publication. Mention of trade names or commercial products does not constitute endorsement or recommendation for use. The views expressed in this article are those of the authors and do not necessarily represent the views or policies of the USEPA. Appendix A. Supporting Information (SI)
The production of graphene-family nanomaterials (GFNs) has increased appreciably in recent years.
Device-associated infections are one of the deadliest complications accompanying the use of biomaterials, and despite recent advances in the development of anti-biofouling strategies, biomaterials that exhibit both functional tissue restoration and antimicrobial activity have been challenging to achieve. Here, we report the fabrication of bio-inspired bactericidal nanospikes in bacterial cellulose and investigate the mechanism underlying this phenomenon. We demonstrate these structures affects preferentially stiff membranes like those in Gram-positive bacteria, but exhibit cytocompatibility towards mammalian cells, a requisite for tissue restoration. We also reveal the bactericidal activity of the nanospikes is due to a pressure-induced mechanism, which depends on the cell's adherence time, nanospike's geometry and spacing, cell shape, and mechanical properties of the cell wall. Our findings provide a better understanding of the mechanobiology of bacterial cells at the interface with nanoscale structures, which is fundamental for the rational design bactericidal topographies.
Periodic surface structures at the nanometer or micrometer scale have been achieved by various methods, while atomic-scale surface structures over large areas are unavailable. Herein, we report the formation of highly coherent atomic-scale ripple patterns on bulk metallic glass (MG) surfaces by low-energy ion irradiation. The pattern arises through three consecutive stages: emergence of initial random dots, subsequent transition to ripples, and ordering of the ripple pattern through annihilation reactions of mobile defects, while the wavelength and amplitude remain invariant throughout the patterning. No pattern is generated for the crystalline counterpart at the same irradiation condition. These observations suggest a distinct ripple forming process typical of MGs associated with their enhanced surface mobility, which enables a controllable self-organization approach for large-area surface structuring with atomic-scale precision.
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