Construction of Superhydrophobic Surfaces Enhanced by Silanized-CNC-Assisted PVDF/PDMS Microsphere Coating

Coatings based on polyvinylidene fluoride (PVDF) and poly(dimethylsiloxane) (PDMS)-based polymeric microspheres can be easily fabricated via non-solvent-induced phase separation (NIPS) and electrostatic spraying (ES) techniques. Both techniques are promising strategies for constructing superhydrophobic surfaces on various substrates. However, PVDF and PDMS inherently suffer from severe aggregation, which generates oversized particles and inhomogeneous microstructures. Conventionally, costly and environmentally hazardous dispersants are required to alleviate this issue, severely restricting the industrial scalability and practical application of such coatings. In this work, methyltrimethoxysilane-modified cellulose nanocrystals (Si-CNCs) were introduced as a green multifunctional modifier to tackle these issues. The results revealed that as structural building blocks and dispersants, Si-CNCs inhibited polymer aggregation via electrostatic repulsion and steric hindrance, refined the particle size and formed uniform micro/nano hierarchical structures. Increasing Si-CNC loading further improved polymer dispersion and superhydrophobic performance. Coatings fabricated by ES showed better hydrophobicity than those fabricated by NIPS. ES achieved a water contact angle (WCA) of 160–166° and a sliding angle (SA) near 1° on cotton fabric, while NIPS had a WCA of 153.8–158° and an SA of around 2°. Wood and glass substrates also obtained favorable superhydrophobicity, with WCAs above 150° and SAs below 1°. Furthermore, all modified surfaces exhibited excellent abrasion resistance. This work provides a relatively eco-friendly, environmentally sustainable, scalable and substrate-flexible strategy for fabricating high-performance PVDF/PDMS-based superhydrophobic coatings.