Simple lignin-based, light-driven shape memory polymers with excellent mechanical properties and wide range of glass...

Lignin is the most abundant biomass source of aromatic hydrocarbons but, at present, is not effectively utilized. The development of simple and efficient methods for producing lignin-based polymers to replace petroleum-based products is an important strategy for promoting environmentally friendly and sustainable materials and controlling carbon emissions. In this work, lignin-based, light-driven shape memory polymers (ELIDs) with improved mechanical properties have been prepared from enzymatic hydrolysis lignin, itaconic acid and 1,12-dodecanediol, without any chemical modification of the lignin. The polymers contain large proportions of lignin (20-40 wt%, designated ELID20 to ELID40) and their mechanical properties are dependent on the lignin content. Maximum tensile strength (46.9 MPa) was achieved with ELID30, maximum elongation at break (93.7 %) was achieved with ELID20 and highest fracture energy (10.75 J cm^-3) was achieved with ELID25. These excellent mechanical properties are accompanied by good thermal stability and a wide range of glass transition temperatures (21.2-157.3 °C), supporting a broad range of applications. The shape fixation rate (R_f) and shape recovery rate (R_r) were highest for ELID30 (98.7 % and 97.4 %, respectively). Under 1 sun simulated solar irradiation, ELID20 reached a temperature exceeding the glass transition temperature in 15 s and, under 3 sun simulated solar irradiation, ELID30 reached a temperature of 130 °C and shape recovered in 60 s. The excellent mechanical properties and good light-driven shape memory of ELIDs provide inspiration for the development and utilization of lignin-based polymers.