“…These tensile properties are significantly higher than those of a majority of reported polyimines whose tensile strength is typically in the range of 20–50 MPa with tensile modulus less than 1.5 GPa, ,,,,,,, and are even comparable to those of some traditional high-performance polyimides (tensile strength: 90–120 MPa, tensile modulus: 2–3 GPa). – ,– On the one hand, the prepared PIIH films contain rigid and large polar imide linkages (Figure S39, Supporting Information), which increases the polymer backbone rigidity and the intermolecular interactions as well as the cohesive energy density, thus endowing the resulting PIIH films with high tensile modulus and tensile strength. On the other hand, the as-synthesized bisimide-containing diamines possess flexible ether linkages, and the cross-linker, tri(2-aminoethyl) amine, also contains elastic methylene units (Figure S39, Supporting Information), which could facilitate the single bond rotation and conformational rearrangement of the polymer network when subjected to external stress, consequently increasing the toughness and robustness of the PIIH networks. ,,,, By contrast, when o -MHBIDA and m -3FBIDA are used to fabricate polyimines, the tensile strength slightly decreases to 88.3 MPa for o -MPIIH and 83.6 MPa for m -3FPIIH . However, an evident reduction in tensile properties is observed for Un -PIIH (tensile strength 71.5% of that of o -DMPIIH and tensile modulus 63.3% of that of o -DMPIIH ) when all substituents are eliminated from the starting diamine monomer Un -HBIDA .…”