Robust and Eco-Friendly Superhydrophobic Starch Nanohybrid Materials with Engineered Lotus Leaf Mimetic Multiscale Hierarchical Structures

The use of superhydrophobic surfaces in a broad range of applications is receiving a great deal of attention due to their numerous functionalities. However, fabricating these surfaces using low-cost raw materials through green and fluorine-free routes has been a bottleneck in their industrial deployment. This work presents a facile and environmentally friendly strategy to prepare mechanically robust superhydrophobic surfaces with engineered lotus leaf mimetic multiscale hierarchical structures via a hybrid route combining soft imprinting and spin-coating. Direct soft-imprinting lithography onto starch/polyhydroxyurethane/cellulose nanocrystal (SPC) films formed micro-scaled features resembling the pillar architecture of lotus leaf. Spin-coating was then used to assemble a thin layer of low-surface-energy poly(dimethylsiloxane) (PDMS) over these microstructures. Silica nanoparticles (SNPs) were grafted with vinyltriethoxysilane (VTES) to form functional silica nanoparticles (V-SNPs) and subsequently used for the fabrication of superhydrophobic coatings. A further modification of PDMS@SPC film with V-SNPs enabled the interlocking of V-SNPs microparticles within the cross-linked PDMS network. The simultaneous introduction of hierarchical microscale surface topography, the low surface tension of the PDMS layer, and the nanoscale roughness induced by V-SNPs contributed to the fabrication of a superhydrophobic interface with a water contact angle (WCA) of ∼150° and a sliding angle (SA) of <10°. The PDMS/V-SNP@SPC films showed an ∼52% reduction in water vapor transmission rate compared to that of uncoated films. These results indicated that the coating served as an excellent moisture barrier and imparted good hydrophobicity to the film substrate. The coated film surfaces were able to withstand extensive knife scratches, finger-rubbing, jet-water impact, a sandpaper-abrasion test for 20 cycles, and a tape-peeling test for ∼10 repetitions without losing superhydrophobicity, suggesting superior mechanical durability. Self-cleaning behavior was also demonstrated when the surfaces were cleared of artificial dust and various food liquids. The green and innovative approach presented in the current study can potentially serve as an attractive new tool for the development of robust superhydrophobic surfaces without adverse environmental consequences.