Hierarchically heterostructured ceramic cellular-polymer gradient coatings: Synergistic autonomous ice shedding and extreme-environment durability.

This study hypothesized that engineering ceramic-polymer composites with hierarchical porosity and stress-adaptive silica reservoirs can reconcile the trade-off between icephobicity and mechanical resilience in superhydrophobic coatings, enabling robust anti-icing solutions for aerospace, energy infrastructure, and cryogenic systems. The hierarchical porosity for water confinement and ceramic microspheres for load dissipation is predicted to enable spontaneous ice shedding while resisting abrasive degradation. Methyltrimethoxysilane (MTMS)-tetraethoxysilane (TEOS) co-condensation was leveraged to synthesize mesoporous ceramic microspheres with encapsulated hydrophobic silica reservoirs. Through alternating layer-by-layer spraying, these microspheres were integrated with acrylic resin (AR) to create a gradient modulus coating. The optimized coating achieved ultralow ice adhesion (20.9 ± 0.43 kPa) through nanopore-induced Cassie-state stabilization (contact angle: 161.3 ± 0.31°, hysteresis: 2.3 ± 0.19°). Surface nanopores promoted spontaneous droplet jumping via Laplace pressure differentials and robustly precluded the pinning of supercooled water, thereby triggered ice-droplets self-dislodging via freezing-induced hydrostatic pressure. Mechanical tests demonstrated exceptional durability with <7 % contact angle reduction after sandpaper abrasion, repeated de-icing cycles, tape peeling, acid-base immersion, infrared irradiation, and protracted weathering, attributed to stress-adaptive silica release from fractured ceramic shells. This architecture establishes a materials design paradigm for extreme-environment anti-icing applications.