Four linear polyurea elastomers synthesized from two different diisocyanates, two different chain extenders and a common aliphatic amine-terminated polyether were used as models to investigate the effects of both diisocyanate structure and aromatic disulfide chain extender on hard segmental packing and self-healing ability. Both direct investigation on hard segments and indirect investigation on chain mobility and soft segmental dynamics were carried out to compare the levels of hard segmental packing, leading to agreed conclusions that correlated well with the self-healing abilities of the polyureas. Both diisocyanate structure and disulfide bonds had significant effects on hard segmental packing and self-healing property. Diisocyanate structure had more pronounced effect than disulfide bonds. Bulky alicyclic isophorone diisocyanate (IPDI) resulted in looser hard segmental packing than linear aliphatic hexamethylene diisocyanate (HDI), whereas a disulfide chain extender also promoted self-healing ability through loosening of hard segmental packing compared to its C-C counterpart. The polyurea synthesized from IPDI and the disulfide chain extender exhibited the best self-healing ability among the four polyureas because it had the highest chain mobility ascribed to the loosest hard segmental packing. Therefore, a combination of bulky alicyclic diisocyanate and disulfide chain extender is recommended for the design of self-healing polyurea elastomers.

The electrical percolation threshold of carbon black (CB) in thermoplastic polyurethane (TPU) decreases by 46% with the incorporation of 20 wt% polyamide copolymer (COPA) through selective localization of CB particles at the interface of sea-island structured TPU/COPA blends. Composites with a composition of TPU/20 wt% COPA/9 wt% CB were prepared by four different mixing sequences and their morphologies were investigated by FESEM and TEM. The majority of CB particles were observed at the interface of sea-island structured blends irrespective of the compounding sequence used, although the percentage of CB particles at the interface is considerably less in the composite prepared by adding COPA to premixed TPU/CB. The driving force for the interfacial localization of most CB particles is the hydrogen bonding of CB with both TPU and COPA, which is confirmed by FTIR and DMA investigations. CB particles act like Janus particle-type compatibilizers with bonded TPU molecules toward the TPU phase and bonded COPA chains toward the COPA phase. Highly efficient conductive paths are formed through the CB-covered domains and a short inter-domain distance.