Abstract
Low output in stress and energy in rubbery state has been a bottleneck for wide-spread applications of thermoset shape memory polymers (SMPs). Traditionally, stress or energy storage in thermoset network is through entropy reduction by mechanical deformation or programming. We here report another mechanism for energy storage, which stores energy primarily through enthalpy increase by stretched bonds during programming. As compared to entropy-driven counterparts, which usually have a stable recovery stress from tenths to several MPa and energy output of several tenths MJ/m(3), our rubbery network achieved a recovery stress of 17.0 MPa and energy output of 2.12 MJ/m(3) in bulk form. The giant stress and energy release in the rubbery state will enhance applications of thermoset SMPs in engineering structures and devices.