Contact Angle Hysteresis on Graphene Surfaces and Hysteresis-free Behavior on Oil-infused Graphite Surfaces

Contact angle hysteresis (CAH) on graphitic surfaces, including chemical vapor deposition (CVD) graphene, reduced electrophoretic deposition (EPD) graphene, highly oriented pyrolytic graphite (HOPG), and polished graphite sheet, has been investigated. The hysteresis loops of water drops on the first three samples are similar but the receding contact angle is particularly small for the polished graphite sheet.The significant CAH observed on CVD graphene and HOPG associated with atom-scale roughness has to be attributed mainly to adhesion hysteresis (surface relaxation), instead of roughness or defects.The difference of the wetting behavior among those four graphitic samples has been further demonstrated by hexadecane drops. On the surface of HOPG or CVD graphene,the contact line expands continuously with time, indicating total wetting for which the contact angle does not exist and contact line pinning disappears. In contrast, on the surface of reduced EPD graphene, spontaneous spreading is halted by spikes on it and partial wetting with small contact angle (θ≈4°) is obtained. On the surface of polished graphite sheet, the superlipophilicity and porous structure are demonstrated by imbibition and capillary rise of hexadecane. Consequently, an oil-infused graphite surface can be fabricated and the ultralow CAH of water (Δθ≈2°) is achieved.