Sequentially Moldable and Bondable Four-Dimensional Hydrogels Compatible with Cell Encapsulation


Hydrogels have captivated the attention of several research and industry segments, including bioengineering, tissue engineering, implantable/wearable sensors and actuators, bioactive agent delivery, food processing, and industrial processes optimization. A common limitation of these systems is their fixed shape. The concept of hydrogel moldability is often assigned to the injectability potential of liquid precursors, and this feature is often lost right after hydrogel formation. Hydrogel modulation is a recent trend that advocates the importance of designing materials with shape fitting ability targeting on-demand responses or defect filling purposes. Here, we present a compliant and cell encapsulation-compatible hydrogel prepared from unmodified natural origin polymers with the ability to undergo extreme sequential shape alterations with high recovery of its mechanical properties. Different fragments of these hydrogels could be bonded together in spatiotemporally controlled shape- and formulation-morphing structures. This material is prepared with affordable off-the-shelf polysaccharides of natural origin using a mild and safe processing strategy based solely on polyelectrolyte complexation followed by an innovative partial coacervate compaction and dehydration step. These unique hydrogels hold potential for multifield industrial and healthcare applications. In particular, they may find application as defect filling agents or highly compliant wound healing patches for cargo release and/or cell delivery for tissue regeneration and cell-based therapies.




Biochemistry & Molecular Biology; Chemistry; Polymer Science


Oliveira, MB; Bastos, HXS; Mano, JF

nossos autores


M.B.O. acknowledges the financial support from the Portuguese Foundation for Science and Technology FCT (Grant SFRH/BPD/111354/2015). This work was developed within the scope of the project CICECO-Aveiro Institute of Materials, POCI-01-0145-FEDER-007679 (FCT ref. UID/CTM/50011/2013) financed by national funds through the FCT/MEC and when appropriate cofinanced by FEDER under the PT2020 Partnership Agreement. This work was also supported by European Research Council grant agreement ERC-2014-ADG-669858 (project ATLAS). The authors acknowledge Prof. Jose Maria Ferreira for kindly providing access to the rheometer.

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