Fully Thermally Decomposable CO2-Based Thermoplastic Polyurethane Encapsulation Films for Photovoltaic Cells: Mechanical, Barrier and Recycling Aspects

The development of sustainable encapsulation materials with tunable thermomechanical properties remains a critical challenge for photovoltaic reliability. Currently, the mainstream encapsulant for polycrystalline silicon solar cells is crosslinked EVA (Ethylene-Vinyl Acetate), which complicates the end-of-life recycling and reuse of modules. There is an urgent need to develop a novel encapsulant that combines excellent barrier properties with thermoplastic recyclability. Herein, we report a novel series of thermally decomposable CO2-based thermoplastic polyurethane (PPC-TE) films engineered through the rational design of soft and hard segments. Utilizing polycarbonate diol (PPCDL) and polyether glycol (PEG) as soft segments, we systematically tailor material properties by modulating PEG-to-PPCDL ratios (5–20 wt%) and PEG molecular weights (1000–4000 g/mol). The optimized PPC-TE films exhibit excellent transmittance (>90%), adjustable glass transition temperature (Tg: 35.1 °C~11.6 °C), and remarkable mechanical adaptability (51~92 HA). The PPC-TE films exhibit water vapor permeability (WVP) as low as 14.8 g·mm·m−2·day−1 and oxygen permeability (OP) of 4.13 cc·mm·m−2 day−1 at 15 wt% PEG content, surpassing commercial ethylene–vinyl acetate (EVA) encapsulants. Notably, these films demonstrate fully thermal decomposition above 350 °C, facilitating eco-friendly photovoltaic device recycling. Superior adhesion to glass substrates is evidenced by peel strengths up to 37 N/cm (PPC-TE2000-20) and the shrinkage rate is as low as 3%. This work contributes to improving the long-term stability of solar cells and has the potential for large-scale production.