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Previous studies have demonstrated that films of sequence‐controlled amphiphilic copolymers display contact angles that depend on microblock size. This suggests that microblock length may provide a means of tuning surface and interfacial properties. In this work, the interfacial rheology of a series of sequence‐controlled copolymers, prepared through the addition of bicyclo[4.2.0]oct‐1(8)‐ene‐8‐carboxamide (monomer A) and cyclohexene (monomer B) to generate sequences up to 24 monomeric units composed of (AmBn)i microblocks, where m, n, and i range from 1 to 6. Interfacial rheometry is used to measure the mechanical properties of an air–water interface with these copolymers. As the microblock size increases, the interfacial storage modulus, G′, increases, which may be due to an increase in the size of interfacial hydrophobic domains. Small‐angle X‐ray scattering shows that the copolymers have a similar conformation in solution, suggesting that any variations in the mechanics of the interface are due to assembly at the interface, and not on solution association or bulk rheological properties. This is the first study demonstrating that microblock size can be used to control interfacial rheology of amphiphilic copolymers. Thus, the results provide a new strategy for controlling the dynamics of fluid interfaces through precision sequence‐controlled polymers. [ABSTRACT FROM AUTHOR]

We report the structural and mechanical behavior of multicomponent hydrogels comprising the commercial poly(ethylene oxide)–poly(propylene oxide)–poly(ethylene oxide) block copolymer F127 and alginate. Previous studies on this system have shown thermoreversible behavior in shear rheology. Here we explore the properties of these materials under compression and large deformations, relevant to applications such as wound dressings that require mechanical robustness. For gels with lower F127 concentration, we find that the stiffness of the gels can be ascribed to the alginate network, and that the Young's modulus and fracture stress do not strongly depend on temperatures. However, for gels with an F127 concentration of 30 wt %, the Young's modulus is enhanced at higher temperatures. Under large deformations, the fracture stress and fracture strain of the materials can be independently varied using the alginate and F127 concentrations, respectively; without the trade‐off in these properties that is often observed in rigid polymer networks. Small‐angle X‐ray scattering shows a power‐law dependence scattering intensity on q arising from the alginate network and scattering peaks consistent with rearranging micelles. For gels with lower F127 concentrations, we find a disordered–body‐centered cubic (BCC)‐face‐centered cubic (FCC) progression of states with temperature, and a BCC/FCC mixture for gels with higher F127 concentrations. [ABSTRACT FROM AUTHOR]