Abstract
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.
Highlights
Shape-morphing materials are added-value assets for multiple applications, and have been reported as self-folding robots,[1] on-demand drug delivery systems[2], and stimulusresponsive textile devices.[3]
Nanocomposite adhesive hydrogels made of a mussel-inspired polymer and dispersed nanosilicates were suggested as fit-to-shape sealants, introducing moldable hydrogels as functional materials for the healthcare field.[14]
Medium molecular weight chitosan (MMW-CHT; ref.448877; 75% degree of deacetylation calculated by 1H NMR – Figure S1 - Bruker DRX 300 Avance at 300.13 MHz; CHT was dissolved in a solution containing 98% D2O and 2% DCl (v/v)), alginic acid sodium salt
Summary
Shape-morphing materials are added-value assets for multiple applications, and have been reported as self-folding robots,[1] on-demand drug delivery systems[2], and stimulusresponsive textile devices.[3] Four-dimensional (4D) hydrogels are highly hydrated materials able to transform their shape, composition or physical properties after fabrication, and are useful as customized drug delivery systems, controllable actuators or cell-encapsulating devices.[4] The modulation of hydrogels’ shape is often related to on-demand induction of reversible phenomena, often triggered by stimuli-responsive swelling variations[5,6,7] or molecular re-arrangements in response to exposure to temperature,[8,9,10] light[11] and conductivity[12] cycles. Nanocomposite adhesive hydrogels made of a mussel-inspired polymer and dispersed nanosilicates were suggested as fit-to-shape sealants, introducing moldable hydrogels as functional materials for the healthcare field.[14]
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