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Finding new ways to tune the behavior of thermoresponsive microgels in bulkand confined at 2D liquid interfaces is key to achieve a deeper understandingand control of these smart materials. We studied the interaction of positivelycharged pNIPAM microgels with the Keggin-type polyoxometalate$Na_{3}PW_{12}O_{40}$ (POM). In bulk, we observed charge inversions below andabove the volume phase transition temperature (VPTT) at significantly low POMconcentrations as $5\cdot10^{-5}$ M. In the presence of POM, the microgelsexhibited a deswelling-swelling-deswelling behaviour below the VPTT, and atwo-step further deswelling above the VPTT. When microgels were confined at 2Dwater/air interfaces, adding $10^{-5}$ M of POM below the VPTT was equivalentto heat above the VPTT and compress the monolayer from $5$ to $20\,\text{mNm$^{-1}$}$. Above the VPTT, the diameter at the interface did not change whilethe portion immersed in the subphase further deswelled, in agreement with thebehavior in bulk. Adding more POM did not change the diameter at the interfacenor the height of the microgels, showing a saturation effect in 2D. Therestructuring of the pNIPAM polymeric network by the POM was characterized byEDS mapping and XPS. The microgel monolayers with POM improved their resistanceto plasma etching, which could be useful for soft colloidal lithography.

Tuning the bulk behavior and 2D interfacial self-assembly of microgels by Keggin-type polyoxometalate ionic specificity