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Peer-reviewedCC BY 4.0Macromolecular Rapid Communications

Cononsolvency‐Assisted Fabrication of Hydrogels and Microgels With Tunable Porosity, Diffusivity and Stiffness

  • Maria I. Pieper1,2
  • Daniel D. Stöbener3
  • Bernhard Häßel1,2
  • Richard Hoogenboom3
  • Andrij Pich1,2,4
4 affiliations
  1. 1Institute of Technical and Macromolecular Chemistry RWTH Aachen University Aachen Germany
  2. 2DWI‐Leibniz Institute for Interactive Materials e.V. Aachen Germany
  3. 3Supramolecular Chemistry Group, Centre of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry Ghent University Ghent Belgium
  4. 4Aachen Maastricht Institute for Biobased Materials (AMIBM) Maastricht University, Brightlands Chemelot Geleen The Netherlands
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Abstract

Porous materials including hydrogels offer high potential for applications requiring controlled mass transport, cell infiltration, and mechanical properties, such as tissue engineering, drug delivery, or soft robotics. We report a facile method for the synthesis of hydrogels and microgels with tunable porosity, offering control over diffusivity and mechanical properties. By exploiting the cononsolvency of polymers based on dimethylacrylamide (DMAAm) and hydroxyethylacrylamide (HEAAm) in water‐acetonitrile mixtures, we produce porous networks with adjustable pore sizes up to several micrometers by varying the acetonitrile content in aqueous solution used during synthesis. The adjustment of the pore size by variation of the solvent mixture allows for fine‐tuning of the hydrogel and microgel mechanical and diffusion properties with stiffnesses ranging from a few kPa up to more than 100 kPa and diffusion coefficients of 4 kDa FITC‐dextran varying from 50 to over 130 µm2 s−1. Detailed analyses using optical microscopy, (cryo‐)scanning electron microscopy, rheology, nanoindentation, and fluorescence recovery after photobleaching confirm the dependence of the observed properties on the network morphology and the similarity of the pore size and interconnectivity between hydrogel and microgel samples. The obtained hydrogels and microgels show strong potential for applications in bioengineering, sensing, and responsive materials.

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Cite

BibTeXRIS
BibTeX
@article{pieper2026cononsolvencyassisted,
  title = {{Cononsolvency‐Assisted Fabrication of Hydrogels and Microgels With Tunable Porosity, Diffusivity and Stiffness}},
  author = {Maria I. Pieper and Daniel D. Stöbener and Bernhard Häßel and Richard Hoogenboom and Andrij Pich},
  journal = {Macromolecular Rapid Communications},
  year = {2026},
  month = sep,
  doi = {10.1002/marc.70423},
  url = {https://doi.org/10.1002/marc.70423},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Cononsolvency‐Assisted Fabrication of Hydrogels and Microgels With Tunable Porosity, Diffusivity and Stiffness
AU  - Maria I. Pieper
AU  - Daniel D. Stöbener
AU  - Bernhard Häßel
AU  - Richard Hoogenboom
AU  - Andrij Pich
PY  - 2026
DA  - 2026/09/05
JO  - Macromolecular Rapid Communications
DO  - 10.1002/marc.70423
UR  - https://doi.org/10.1002/marc.70423
AB  - Porous materials including hydrogels offer high potential for applications requiring controlled mass transport, cell infiltration, and mechanical properties, such as tissue engineering, drug delivery, or soft robotics. We report a facile method for the synthesis of hydrogels and microgels with tunable porosity, offering control over diffusivity and mechanical properties. By exploiting the cononsolvency of polymers based on dimethylacrylamide (DMAAm) and hydroxyethylacrylamide (HEAAm) in water‐acetonitrile mixtures, we produce porous networks with adjustable pore sizes up to several micrometers by varying the acetonitrile content in aqueous solution used during synthesis. The adjustment of the pore size by variation of the solvent mixture allows for fine‐tuning of the hydrogel and microgel mechanical and diffusion properties with stiffnesses ranging from a few kPa up to more than 100 kPa and diffusion coefficients of 4 kDa FITC‐dextran varying from 50 to over 130 µm2 s−1. Detailed analyses using optical microscopy, (cryo‐)scanning electron microscopy, rheology, nanoindentation, and fluorescence recovery after photobleaching confirm the dependence of the observed properties on the network morphology and the similarity of the pore size and interconnectivity between hydrogel and microgel samples. The obtained hydrogels and microgels show strong potential for applications in bioengineering, sensing, and responsive materials.
SN  - 1022-1336
SN  - 1521-3927
ER  -