Information of the relaxation behaviors of polymer film is crucial to judge the durability of emulsion polymer isocyanate (EPI) as a structural adhesive for bonding timber-based products. A sequence of tensile creep tests and free volume evaluation of the cured EPI adhesive films during isothermal condition were carried out by dynamic mechanical analysis and positron annihilation lifetime spectroscopy, respectively. It is the first time to explore the creep response and physical aging of the EPI film, as well as associated microstructural evolution. The results indicate that the creep characteristics of the glassy EPI coating intimately depend upon the crosslinker and elapsed time, and the ideal momentary creep master curve can be constructed in terms of modified horizontal shifting method. Furthermore, the relaxation process is found to be dominated by vacancy diffusion mechanism. In addition, increasing the polymeric isocyanate content can significantly enhance the resistance to creep deformation of EPI films, but also accelerate the physical aging process. Due to a higher packing degree of pure polymer films, the EPI films with aqueous emulsified isocyanate exhibit much better relaxation resistance compared to that with general isocyanate crosslinker.
Keywords: creep; emulsion polymer isocyanate; free volume; physical aging; positron annihilation lifetime spectroscopy.