Demonstration of Pattern Size Effects on Hydrophobic Nanocellulose Coatings with Regular Micron-Sized Island-like Geometrical Domains Created by Femtosecond Laser Micromachining

As inspired by nature, wettability of bio-based material surfaces can be controlled by combining appropriate surface chemistries and topographies mimicking the structure of plant leaves or animals. The need for bio-based nanocellulose coatings with enhanced hydrophobic properties becomes technically relevant for extending their applications in the technological domain with better protection and lifetime of the coatings. In this work, the water repellence of spray-coated nanocellulose coatings with hydrophobically modified cellulose microfiber (mCMF coatings), or hydrophobically modified cellulose nanofiber (mCNF coatings) was enhanced after femtosecond laser patterning. In particular, the influences of different island-like pattern geometries and pattern sizes were systematically studied. The island-like patterns were experimentally created with single posts that have variable sizes of the valleys (B = 30 to 15 µm) and top surface area (T = 120 to 15 µm), resulting in good resolution of the patterns down to the size of the laser beam diameter (15 µm). Depending on the intrinsic homogeneity and porosity of sprayed mCMF and mCNF coatings, the quality and resolution of the island-like patterns is better for the mCNF coatings with thinner and more homogeneous sizes of the cellulose nanofibrils. The increase in apparent water contact angle on patterned nanocellulose coatings can be estimated from the theoretical Cassie-Baxter state of wetting and shows maximum values up to <i>θ</i>_s = 128° (mCMF coatings), or <i>θ</i>_s = 140° (mCNF coatings), for the smallest pattern sizes in parallel with minimum contact angle hysteresis of Δ<i>θ</i> = 14° (mCMF coatings), or Δ<i>θ</i> < 9° (mCNF coatings). The study demonstrated that femtosecond laser patterning technology provides high flexibility and adaptivity to create surface patterns in appropriate dimensions with enhanced hydrophobicity of nanocellulose coatings.