Non-Fluorine Oil Repellency: How Low the Intrinsic Wetting Threshold Can Be for Roughness-Induced Contact Angle Amplification?

Surface chemistries for realizing oil repellency are mostly based on perfluoro compounds (PFCs) owing to their low surface energy. However, PFCs are not sustainable because of their persistent and bioaccumulative properties, and their usage, even short-chain ones, has begun to be phased out. To date, studies on non-fluorine oil repellency have been extremely rare, and the obtained oil repellency has been limited. Here, we report the non-fluorine oil repellency of a coating prepared on a tightly woven plain-weave fabric through hydrolysis and polycondensation of difunctional chlorosilane. The coated fabric exhibited a contact angle of 119.0° for castor oil and 81.4° for hexadecane, as well as a contact angle of 51.9° for decane with a surface tension as low as γ_LV = 23.5 mN m^-1. According to the standard ISO 14419:2010, oil repellency was rated Grade 6. The solid surface tension of the coating was calculated to be γ_SV = 22.1 mN m^-1. Through the test of the difference in contact angles between rough and smooth surfaces, the intrinsic wetting threshold (θ_IWT) for such a surface chemistry was determined to be ranging from 8.9 to 14.5°. A study on the effects of surface morphologies suggests that the realization of an oil-repellency rating of 6 and a θ_IWT as low as 8.9-14.5° strongly depends on the roughness topographies. We hope that this study will be useful for the design─and our understanding─of non-fluorine oil repellency for applications including stain-resistant textiles and grease-resistant food packaging.