Biomimetic Strain‐Stiffening Self‐Assembled Hydrogels

Abstract

Supramolecular structures with strain‐stiffening properties are ubiquitous in nature but remain rare in the lab. Herein, we report on strain‐stiffening supramolecular hydrogels that are entirely produced through the self‐assembly of synthetic molecular gelators. The involved gelators self‐assemble into semi‐flexible fibers, which thereby crosslink into hydrogels. Interestingly, these hydrogels are capable of stiffening in response to applied stress, resembling biological intermediate filaments system. Furthermore, strain‐stiffening hydrogel networks embedded with liposomes are constructed through orthogonal self‐assembly of gelators and phospholipids, mimicking biological tissues in both architecture and mechanical properties. This work furthers the development of biomimetic soft materials with mechanical responsiveness and presents potentially enticing applications in diverse fields, such as tissue engineering, artificial life, and strain sensors.

Self‐Foaming Metal‐Organic Gels Based on Phytic Acid and Their Mechanical, Moldable, and Load‐Bearing Properties.

“…Their properties can be tuned by the choice of small molecular gelators [3–5] . and the cross‐linking of gelators [6] . Metal‐organic gels are a kind of supramolecular gels containing metal ions, metal‐organic moieties, and metal nanoparticles [7] .…”

Skin-like mechanoresponsive self-healing ionic elastomer from supramolecular zwitterionic network

“…Stretching such a dynamic network is usually accompanied by crosslinking density reduction and stress relaxation, leading to the remarkable attenuation of material modulus as well as poor elastic recovery from large deformations 14 , 16 – 19 . On the other hand, strain-stiffening materials normally involve two distinct networks with different rigidities that unfold progressively for synergizing softness and firmness 20 – 23 . For instance, bottlebrush elastomers could replicate the strain-stiffening characteristics of biological tissues by unfolding flexible strands at lower forces followed by stretching rigid backbone at higher forces 9 , 21 – 24 .…”

Synthetic Supramolecular Systems in Life-like Materials and Protocell Models

“…139 Another intriguing example has been recently introduced by van Esch and co-workers, who mimicked the strain-stiffening Review response of natural cytoskeletal fibers with synthetic fibrillar networks, which form hydrogels that can be orthogonally self-assembled with liposomes as cells-in-matrix models of biological tissues. 140 Life processes take place in confined microenvironments (i.e., cells and organelles) that coordinate structural and functional tasks in response to their medium. Cell-like communication and adaptation has been engineered synthetically between many supramolecular compartments.…”