Molecular-Weight-Dependent Interplay of Brittle-to-Ductile Transition in High-Strain-Rate Cold Spray Deposition of Glassy Polymers

[Image: see text] Based on the cold spray technique, the solvent-free and solid-state deposition of glassy polymers is envisioned. Adiabatic inelastic deformation mechanisms in the cold spray technique are studied through high-velocity collisions (<1000 m/s) of polystyrene microparticles against stationary target substrates of polystyrene and silicon. During extreme collisions, a brittle-to-ductile transition occurs, leading to either fracture- or shear-dominant inelastic deformation of the colliding microparticles. Due to the nonlinear interplay between the adiabatic shearing and the thermal softening of polystyrene, the plastic shear flow becomes the dominant deformation channel over brittle fragmentation when increasing the rigidity of the target substrate. High molecular weights (>20 kDa) are essential to hinder the evolution of brittle fracture and promote shear-induced heating beyond the glass transition temperature of polystyrene. However, an excessively high molecular weight (∼100 kDa) reduces the adhesion of the microparticles to the substrate due to insufficient wetting of the softened polystyrene. Due to the two competing viscoelastic effects, proper selection of molecular weight becomes critical for the cold spray technique of glassy polymers.