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The role of electrostatics on the interfacial properties of polyelectrolytemicrogels has been discussed controversially in the literature. It is not yetclear if, or how, Coulomb interactions affect their behavior under interfacialconfinement. In this work, we combine compression isotherms, atomic forcemicroscopy imaging, and computer simulations to further investigate thebehavior of pH-responsive microgels at oil-water interfaces. At lowcompression, charged microgels can be compressed more than uncharged microgels.The in-plane effective area of charged microgels is found to be smaller incomparison to uncharged ones. Thus, the compressibility is governed by in-planeinteractions of the microgels with the interface. At high compression, however,charged microgels are less compressible than uncharged microgels. Microgelfractions located in the aqueous phase interact earlier for charged than foruncharged microgels because of their different swelling perpendicular to theinterface. Therefore, the compressibility at high compression is controlled byout-of-plane interactions. In addition, the size of the investigated microgelsplays a pivotal role. The charge-dependent difference in compressibility at lowcompression is only observed for small but not for large microgels, while thebehavior at high compression does not depend on the size. Our results highlightthe complex nature of soft polymer microgels as compared to rigid colloidalparticles. We clearly demonstrate that electrostatic interactions affect theinterfacial properties of polyelectrolyte microgels.

Influence of charges on the behavior of polyelectrolyte microgels confined to oil-water interfaces