%0 Journal Article %T Tunable and Processable Shape-Memory Materials Based on Solvent-Free, Catalyst-Free Polycondensation between Formaldehyde and Diamine at Room Temperature %J - %D 2019 %R https://doi.org/10.1021/acsmacrolett.9b00199 %X Compared with traditional thermosets, malleable thermosets have more applications in aerospace, biotechnology, and construction. Here we report a one-step, solvent-free, catalyst-free polycondensation method between diamine and formaldehyde to prepare a series of malleable hemiaminal dynamic covalent networks (HDCNs). The materials have excellent malleability and reprocessability by hot pressing. The Young¡¯s modulus and breaking strength of HDCNs obtained by the polycondensation of formaldehyde and 4,4-diaminodiphenylmethane (MDA) are as high as 1.6 GPa and 60 MPa, respectively, which can be facilely adjusted through the introduction of polyetheramine-400 (PEDA). Moreover, the HDCNs feature the shape memory ability with a recovery ratio above 93.5% and can be recycled by the addition of different monomers. This promising HDCN, prepared from economical raw materials, may have vast applications in industries %U https://pubs.acs.org/doi/10.1021/acsmacrolett.9b00199