Abstract

A large array of easily available small-molecule (as opposed to industrial oligomeric) triisocyanates and aromatic polyols render polyurethanes a suitable model system for a trend-based systematic study of structure–property relationships in nanoporous matter as a function of the monomer structure. Molecular parameters of interest include rigidity, number of functional groups per monomer (n), and functional group density (number of functional groups per phenyl ring, r). All systems were characterized from gelation to the bulk properties of the final aerogels. Molecular and nanoscopic features of interest, including skeletal composition, porous structure, nanoparticle size, and assembly, were probed with a combination of liquid- and solid-state 13C and 15N NMR, rheometry, N2- and Hg-porosimetry, SEM, and small-angle X-ray scattering (SAXS). Macroscopic properties such as styrofoam-like thermal conductivities (∼0.030 W m–1K–1), foam-like flexibility, or armor-grade energy absorption under compression (up to...

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