Mechanochemical Adhesion and Plasticity in Multifiber Hydrogel Networks

Abstract

The extracellular matrix (ECM) has force‐responsive (i.e., mechanochemical) properties that enable adaptation to mechanical loading through changes in fibrous network structure and interfiber bonding. Imparting such properties into synthetic fibrous materials will allow reinforcement under mechanical load, the potential for material self‐adhesion, and the general mimicking of ECM. Multifiber hydrogel networks are developed through the electrospinning of multiple fibrous hydrogel populations, where fibers contain complementary chemical moieties (e.g., aldehyde and hydrazide groups) that form covalent bonds within minutes when brought into contact under mechanical load. These fiber interactions lead to microscale anisotropy, as well as increased material stiffness and plastic deformation. Macroscale structures (e.g., tubes and layered scaffolds) are fabricated from these materials through interfiber bonding and adhesion when placed into contact while maintaining a microscale fibrous architecture. The design principles for engineering plasticity described can be applied to numerous material systems to introduce unique properties, from textiles to biomedical applications.

Mechanochemical Patternable ECM‐Mimetic Hydrogels for Programmed Cell Orientation

“…[ 78 ] Recently, dynamic covalent bonds present in multifiber‐based networks allowed mechanochemical interactions among complementary fiber species upon force‐induced contact. [ 79 ] Herein, we explored this unique behavior on hybrid polysaccharide/polypeptide hydrogels for the first time, which can more closely convey the multifunctional composition of natural matrices.…”

Hydrogel: Diversity of Structures and Applications in Food Science

“…With the increasing requirements for complex functions, homogeneous hydrogels that with uniform bulk properties show more and more limitations, while those hierarchical hydrogels containing multiple layers/ membranes show increasing advantages in terms of structural complexity and functional diversity play crucial role in many fields. [84,[359][360][361][362][363][364] In addition to the traditional photo-polymerization technique, [365,366] in recent years, several effective technology paths have been developed for the fabrication of multi-layered hydrogels, such as layer-by-layer (LBL) technique, [367][368][369][370] step-wise technique (mainly for onion-like multi-layered hydrogels), [359,361,[371][372][373][374] sequential electrospinning technique, [375][376][377][378][379][380][381] and 3D printing (additive manufacturing) technique. [382][383][384][385] Meanwhile, "Janus" structural hydrogels can be regarded as another kind of multi-layered hydrogels (Fig.…”

The emerging technology of biohybrid micro-robots: a review

“…Furthermore, mechanical properties can be tuned by controlling the molecular structure of the polymers and cross-linking agents to recapitulate those of natural tissues [154][155][156]. The microstructures of hydrogels allow the exchange of nutrients and gases, which is essential for cell survival, proliferation, and differentiation [157]; therefore, given their advantages over bioinert polymers, much research has been actively exploring the applications of hydrogels in bio-robotic fields. The hydrogels used for…”