Robinson, Benjamin James and Bailey, Steven William Dennis and O'Driscoll, Luke J. and Visontai, David and Welsh, Daniel J. and Mostert, Albertus Bernardus and Mazzocco, Riccardo and Rabot, Caroline and Jarvis, Samuel and Kolosov, Oleg Victor and Bryce, Martin R. and Lambert, Colin John (2017) Formation of two-dimensional micelles on graphene : a multi-scale theoretical and experimental study. ACS Nano. ISSN 1936-0851
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Abstract
Graphene and related two-dimensional (2D) materials possess outstanding electronic and mechanical properties, chemical stability and high surface area. However, to realize graphene’s potential for a range of applications in materials science and nanotechnology there is a need to understand and control the interaction of graphene with tailored high-performance surfactants designed to facilitate the preparation, manipulation and functionalization of new graphene systems. Here we report a combined experimental and theoretical study of the surface structure and dynamics on graphene of pyrene-oligoethylene glycol (OEG) -based surfactants, which have previously been shown to disperse carbon nanotubes in water. Molecular self-assembly of the surfactants on graphitic surfaces is experimentally monitored and optimized using a graphene coated quartz crystal microbalance in ambient and vacuum environments. Real-space nanoscale resolution nanomechanical and topographical mapping of sub-monolayer surfactant coverage, using ultrasonic and atomic force microscopies both in ambient and ultra-high vacuum, reveals complex, multi-length-scale self-assembled structures. Molecular dynamics simulations show that at the nanoscale these structures, on atomically-flat graphitic surfaces, are dependent upon the surfactant OEG chain length and are predicted to display a previously unseen class of 2D self-arranged ‘starfish’ micelles (2DSMs). Whilst three-dimensional micelles are well known for their widespread uses ranging from microreactors to drug-delivery vehicles, these 2DSMs possess the highly desirable and tunable characteristics of high surface affinity coupled with unimpeded mobility, opening up strategies for processing and functionalizing 2D materials.