Dataset Structural Changes of Flexible, Small-Sized Polycationic Microgels upon Interaction with Hexacyanoferrate(III) Viewed at an Atomic and a Particle Scale
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| Natura: | Recurso digital |
| Lingua: | inglese |
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2026
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| _version_ | 1866901531139244032 |
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| author | Neubert, Richard Plamper, Felix TU Bergakademie Freiberg |
| author_facet | Neubert, Richard Plamper, Felix TU Bergakademie Freiberg |
| contents | <p>Charged colloid systems pose challenges and offer unexpected chances in their dispersion/solution behaviour because of the interdependence of structural reorganizations, electrostatics and molecular ion binding. Here, strong polyelectrolytic P(NIPAM-co-MAPTAC) microgels/nanogels consisting of N-isopropylacrylamide and methacrylamidopropyltrimethylammonium chloride (quaternized dimethylaminopropylmethacrylamide DMAPMA) with ultrasmall hydrodynamic radius (41 nm, 20°C, 0.1 M KCl; minimum: 25 nm) are prepared and investigated with varying concentrations of multivalent counterions as ionic cargo (i.e. hexacyanoferrate(III)). We combine paramagnetic relaxation enhancement NMR (PRE-NMR), dynamic light scattering DLS, and small angle X-ray scattering SAXS (fuzzy-sphere extended model) with quantum chemical calculations (r²SCAN-3c) to probe binding geometries and structural transitions across varying salt concentrations and temperatures under flooding versus Donnan equilibrium conditions. PRE-NMR reveals selective [Fe(CN)6]3- binding to MAPTAC via secondary amide-hexacyanoferrate coordination. SAXS quantifies ion-induced reorganizations: core contraction, fuzzy shell expansion, and changes in the correlation length upon hexacyanoferrate addition accompanied by a reentrant swelling based on the preferential interaction of hexacyanoferrate with the charged microgel outskirts. This multiscale approach demonstrates that peripheral charge localization enables reversible switching between intra- and interparticle crosslinking, where the thermal history above 55°C can be recorded. Our results could have implications on applications like sensing, controlled release and nanoparticle-templated catalysis.</p> |
| format | Recurso digital |
| id | zenodo_https___doi_org_10_5281_zenodo_18169854 |
| institution | Zenodo |
| language | eng |
| publishDate | 2026 |
| publisher | Zenodo |
| record_format | zenodo |
| spellingShingle | Dataset Structural Changes of Flexible, Small-Sized Polycationic Microgels upon Interaction with Hexacyanoferrate(III) Viewed at an Atomic and a Particle Scale Neubert, Richard Plamper, Felix TU Bergakademie Freiberg Microgels/analysis Microgels/chemistry <p>Charged colloid systems pose challenges and offer unexpected chances in their dispersion/solution behaviour because of the interdependence of structural reorganizations, electrostatics and molecular ion binding. Here, strong polyelectrolytic P(NIPAM-co-MAPTAC) microgels/nanogels consisting of N-isopropylacrylamide and methacrylamidopropyltrimethylammonium chloride (quaternized dimethylaminopropylmethacrylamide DMAPMA) with ultrasmall hydrodynamic radius (41 nm, 20°C, 0.1 M KCl; minimum: 25 nm) are prepared and investigated with varying concentrations of multivalent counterions as ionic cargo (i.e. hexacyanoferrate(III)). We combine paramagnetic relaxation enhancement NMR (PRE-NMR), dynamic light scattering DLS, and small angle X-ray scattering SAXS (fuzzy-sphere extended model) with quantum chemical calculations (r²SCAN-3c) to probe binding geometries and structural transitions across varying salt concentrations and temperatures under flooding versus Donnan equilibrium conditions. PRE-NMR reveals selective [Fe(CN)6]3- binding to MAPTAC via secondary amide-hexacyanoferrate coordination. SAXS quantifies ion-induced reorganizations: core contraction, fuzzy shell expansion, and changes in the correlation length upon hexacyanoferrate addition accompanied by a reentrant swelling based on the preferential interaction of hexacyanoferrate with the charged microgel outskirts. This multiscale approach demonstrates that peripheral charge localization enables reversible switching between intra- and interparticle crosslinking, where the thermal history above 55°C can be recorded. Our results could have implications on applications like sensing, controlled release and nanoparticle-templated catalysis.</p> |
| title | Dataset Structural Changes of Flexible, Small-Sized Polycationic Microgels upon Interaction with Hexacyanoferrate(III) Viewed at an Atomic and a Particle Scale |
| topic | Microgels/analysis Microgels/chemistry |
| url | https://doi.org/10.5281/zenodo.18169854 |