Preparation of Self-healing Thermoplastic Polysiloxane–Polyurea/Polyether–Polyurea Elastomer Blends with a Co-continuous Microphase Structure and In-Depth Research on Their Synergistic Effects

Polymer blending has been an important method to create materials with specific properties that have synergistic effects. However, there are few reports on the mechanism of synergistic effects. It is well known that it is quite difficult to obtain ideal blends composed of nonpolar organosilicon polymers and polar polymers. In this paper, thermoplastic polyurea elastomer blends with a co-continuous microphase structure consisting of polysiloxane-polyurea (PDMS-PUA), polyether amine-polyurea (PEA-PUA), and compatibilizer PDMS-PUA-grafted PEA-PUA (PDMS-PUA-g-PEA-PUA) were prepared for the first time. For the first time, introduction of polysiloxane does not sacrifice mechanical properties of thermoplastic polyurea elastomers. For example, the tensile strength of the elastomer blend with 30 wt % PDMS-PUA content reached 25.7 MPa, which is higher than those of PEA-PUA and PDMS-PUA. The blends also show typical outstanding characters such as exceptional heat and water resistance. The mechanism of the synergistic effect on mechanical properties is revealed based on in-depth studies on mutual interphase interaction. In situ variable temperature infrared spectroscopic analysis (VTIR) shows that compatibilization facilitates the construction of a denser hydrogen bonding network at the blend interface, which is thought to play a key role in the co-continuous microphase structure. Microscopic morphological characterization shows that PDMS-PUA and PEA-PUA phases are deformed and oriented together during the stretching process, thus jointly resisting external forces. Moreover, the blends show an exceptional self-healing ability due to their strong and reversible hydrogen bonding network.