TY - JOUR A1 - Ihlenburg, Ramona A1 - Mai, Tobias A1 - Thünemann, Andreas F. A1 - Baerenwald, Ruth A1 - Saalwächter, Kay A1 - Koetz, Joachim A1 - Taubert, Andreas T1 - Sulfobetaine hydrogels with a complex multilength-scale hierarchical structure JF - The journal of physical chemistry : B, Condensed matter, materials, surfaces, interfaces & biophysical chemistry N2 - Hydrogels with a hierarchical structure were prepared from a new highly water-soluble crosslinker N,N,N',N'-tetramethyl-N,N'-bis(2-ethylmethacrylate)-propyl-1,3-diammonium dibromide and from the sulfobetaine monomer 2-(N-3-sulfopropyl-N,N-dimethyl ammonium)ethyl methacrylate. The free radical polymerization of the two compounds is rapid and yields near-transparent hydrogels with sizes up to 5 cm in diameter. Rheology shows a clear correlation between the monomer-to-crosslinker ratio and the storage and loss moduli of the hydrogels. Cryo-scanning electron microscopy, low-field nuclear magnetic resonance (NMR) spectroscopy, and small-angle X-ray scattering show that the gels have a hierarchical structure with features spanning the nanometer to the sub-millimeter scale. The NMR study is challenged by the marked inhomogeneity of the gels and the complex chemical structure of the sulfobetaine monomer. NMR spectroscopy shows how these complications can be addressed via a novel fitting approach that considers the mobility gradient along the side chain of methacrylate-based monomers. KW - Defects KW - Hydrogels KW - Nuclear magnetic resonance spectroscopy KW - Scattering KW - X-ray scattering Y1 - 2021 U6 - https://doi.org/10.1021/acs.jpcb.0c10601 SN - 1520-6106 SN - 1520-5207 VL - 125 IS - 13 SP - 3398 EP - 3408 PB - American Chemical Society CY - Washington ER -