Enhanced mass transport in graphene nanofluidic channels
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Enhanced mass transport in carbon-based nanoscale conduits (e.g. carbon nanotubes, graphene nanochannels/capillaries, graphene/graphene oxide membranes) has attracted tremendous interest over the last decade due to its significant implications for water desalination/purification, nanofiltration, electronic cooling, battery/fuel cells, and lab-on-a-chip. Further development of carbon-based nanoscale conduits for practical applications relies on understanding fundamental mechanisms of transport through individual conduits, which have not been well studied due to challenges in fabrication and measurement. In this thesis, the construction of two-dimensional planar graphene nanochannel devices and the studies of enhanced water and ion transport inside the graphene nanochannels are reported for the first time. The graphene nanochannels are fabricated by conformally covering high-quality graphene on the surfaces of silica nanochannels. A new fabrication scheme consisting of graphene wet transfer, graphene patterning and vacuum anodic bonding is developed to create such graphene nanochannels with heights ranging from 24 to 124 nm. Using these nanochannels and a new hybrid nanochannel based capillary flow measurement technique, we successfully measured the hydraulic resistance (water permeability) of single graphene nanochannels. Our results demonstrate that the frictionless surface of graphene induces a boundary slip and enhances water flow inside the graphene nanochannel. The measured slip length of graphene in the graphene nanochannels poses a median value around 16 nm, albeit with a large variation from 0 to 200 nm regardless of the channel height. The small-yet-widely-varying values of the graphene slip length are attributed to the surface charge of graphene and the interaction between graphene and underneath silica substrate, which are in good agreement with the prediction of our molecular dynamics (MD) simulation. In addition, we also investigated enhanced ion transport inside the graphene nanochannels. Higher electroosmotic conductance at low electrolyte concentrations (10-6 M~10-2 M) is observed in graphene nanochannels when compared with silica nanochannels with the same geometry. Our results suggest that the enhanced electroosmotic flow is also due to the boundary slip at the graphene/electrolyte interface. Besides, our analysis shows that the surface charge on the graphene, originating from the dissociation of oxygen-containing functional groups, is crucial to the enhanced electroosmotic flow inside nanochannels.