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Smart hydrogels based on self-assembled amphiphilic copolymers

Smart Hydrogels based on self assembled amphiphilic copolymers

By tempering the hydrophobic blocks of block and grafted amphiphilic copolymers (that is by incorporating hydrophilic subunits inside them), we have been able to obtain self-assemblies and hydrogels at thermodynamic equilibrium whereas non tempered amphiphilic block copolymers display mostly the formation of frozen self-assemblies. When the hydrophilic subunits are pH sensitive, the dynamics of the resulting hydrogels can be tuned in a reversible way with pH over 11 orders of magnitude. Dynamic self-assemblies can be blended easily to achieve mixed micelles and hydrogels of controlled properties through the stoechiometry of the blends. We can also achieve interpenetrated self-assembled networks responsive to various stimuli when mixing appropriate block copolymers. This approach has been exemplified with a great variety of amphiphilic copolymers.



  • Lazhar Benyahia
  • Christophe Chasseneiux
  • Olivier Colombani
  • Erwan Nicol
  • Taco Nicolaï

Related papers

  • Tsitsilianis, C.; Serras, G.; Ko, C.-H.; Jung, F.; Papadakis, C. M.; Rikkou-Kalourkoti, M.; Patricicios, C. S.; Schweins, R.; Chassenieux, C. Thermoresponsive Hydrogels Based on Telechelic Polyelectrolytes: From Dynamic to "Frozen" Networks. Macromolecules 2018, 51, (6), 2169-2179. doi: 10.1021/acs.macromol.8b00193.
  • Nicol, E.; Nicolai, T.; Zhao, J.; Narita, T. Photo-Cross-Linked Self-Assembled Poly(ethylene oxide)-Based Hydrogels Containing Hybrid Junctions with Dynamic and Permanent Cross-Links. Acs Macro Letters 2018, 7, 683-687. doi: DOI: 10.1021/acsmacrolett.8b00317.
  • Lauber, L.; Santarelli, J.; Boyron, O.; Chassenieux, C.; Colombani, O.; Nicolai, T. pH- and Thermoresponsive Self-Assembly of Cationic Triblock Copolymers with Controlled Dynamics. Macromolecules 2017, 50, (1), 416-423. doi: 10.1021/acs.macromol.6b02201.
  • Lauber, L.; Depoorter, J.; Nicolai, T.; Chassenieux, C.; Colombani, O. Viscoelastic Properties of Hydrogels Based on Self-Assembled Multisticker Polymers Grafted with pH-Responsive Grafts. Macromolecules 2017, 50, (20), 8178-8184. doi: 10.1021/acs.macromol.7b01585.
  • Wright, D. B.; Patterson, J. P.; Gianneschi, N. C.; Chassenieux, C.; Colombani, O.; O'Reilly, R. K. Blending block copolymer micelles in solution; obstacles of blending. Polymer Chemistry 2016, 7, (8), 1577-1583. doi: 10.1039/c5py02006a.
  • Lauber, L.; Colombani, O.; Nicolai, T.; Chassenieux, C. pH-Controlled Rheological Properties of Mixed Amphiphilic Triblock Copolymers. Macromolecules 2016, 49, (19), 7469-7477. doi: 10.1021/acs.macromol.6b01600.
  • Chassenieux, C.; Tsitsilianis, C. Recent trends in pH/thermo-responsive self-assembling hydrogels: from polyions to peptide-based polymeric gelators. Soft Matter 2016, 12, (5), 1344-1359. doi: 10.1039/c5sm02710a.
  • Wright, D. B.; Patterson, J. P.; Pitto-Barry, A.; Lu, A.; Kirby, N.; Gianneschi, N. C.; Chassenieux, C.; Colombani, O.; O'Reilly, R. K. The Copolymer Blending Method: A New Approach for Targeted Assembly of Micellar Nanoparticles. Macromolecules 2015, 48, (18), 6516-6522. doi: 10.1021/acs.macromol.5b01426.
  • Wright, D. B.; Patterson, J. P.; Pitto-Barry, A.; Cotanda, P.; Chassenieux, C.; Colombani, O.; O'Reilly, R. K. Tuning the aggregation behavior of pH-responsive micelles by copolymerization. Polymer Chemistry 2015, 6, (14), 2761-2768. doi: 10.1039/c4py01782j.
  • Lauber, L.; Chassenieux, C.; Nicolai, T.; Colombani, O. Highlighting the Role of the Random Associating Block in the Self-Assembly of Amphiphilic Block-Random Copolymers. Macromolecules 2015, 48, (20), 7613-7619. doi: 10.1021/acs.macromol.5b01626.
  • Klymenko, A.; Nicolai, T.; Benyahia, L.; Chassenieux, C.; Colombani, O.; Nicol, E. Multiresponsive Hydrogels Formed by Interpenetrated Self-Assembled Polymer Networks. Macromolecules 2014, 47, (23), 8386-8393. doi: 10.1021/ma501990r.


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