Hydrophobic and Optical-Barrier Films from Chemically Recycled EPS Reinforced with Cellulose Nanocrystals and Sunflower Oil

Expanded polystyrene (EPS) waste is a major environmental concern, yet practical routes to upgrade it into higher value-added materials remain limited. Here, post-consumer EPS was dissolved in ethyl acetate and solvent-cast into films containing cellulose nanocrystals (CNCs) and a sunflower oil. Three formulations were produced: F-EPS (100% EPS), F-EPS + CEL (80% EPS/20% CNC), and F-EPS + CEL + OIL (80% EPS/15% CNC/5% oil). CNC markedly enhanced optical shielding, reducing transmittance at 400 nm from ≈58% (F-EPS) to ≈18% (CNC containing films). All films remained hydrophobic, showed negligible water uptake, and exhibited low mass loss after 30 days of accelerated weathering (ΔM=1–3%). Tensile testing showed that F-EPS had the highest UTS and elongation at break (10.0 ± 0.6 MPa and 10.5 ± 0.4%), whereas adding cellulose increased the elastic modulus (249.5 ± 29.0 MPa to 358.4 ± 64.8 MPa) but reduced UTS and elongation (8.2 ± 0.2 MPa and 5.4 ± 2.5%). Oil addition led to a further reduction in UTS and elongation (6.2 ± 0.4 MPa and 3.6 ± 0.0%), while the modulus returned to a value statistically similar to neat F-EPS. FTIR and XRD confirmed preservation of the EPS chemical fingerprint and a predominantly amorphous structure (2θ≈20–30°). Overall, EPS + CNC + OIL films combine hydrophobicity, UV-screening, and elastic modulus similar to neat F-EPS, supporting their use as moisture-resistant, UV screening protective topcoats for non-food-contact paperboard packaging.