High stretchability, strength, and toughness of living cells enabled by hyperelastic vimentin intermediate filaments.

In many developmental and pathological processes, including cellular migration during normal development and invasion in cancer metastasis, cells are required to withstand severe deformations. The structural integrity of eukaryotic cells under small deformations has been known to depend on the cytoskeleton including actin filaments (F-actin), microtubules (MT), and intermediate filaments (IFs). However, it remains unclear how cells resist severe deformations since both F-actin and microtubules yield or disassemble under moderate strains. Using vimentin containing IFs (VIFs) as a model for studying the large family of IF proteins, we demonstrate that they dominate cytoplasmic mechanics and maintain cell viability at large deformations. Our results show that cytoskeletal VIFs form a stretchable, hyperelastic network in living cells. This network works synergistically with other cytoplasmic components, substantially enhancing the strength, stretchability, resilience, and toughness of cells. Moreover, we find the hyperelastic VIF network, together with other quickly recoverable cytoskeletal components, forms a mechanically robust structure which can mechanically recover after damage.

Probing Surface Hydration and Molecular Structure of Zwitterionic and Polyacrylamide Hydrogels.

A hydrogel is a hydrophilic cross-linked polymer network which can contain a large amount of water. Hydrogels with distinguished interfacial physical toughness were analyzed for their potential application as antifouling coating materials, utilizing sum frequency generation (SFG) spectroscopy as the interfacial analytical technique. The surface structures of one sulfobetaine (SBMA) zwitterionic hydrogel (ZWHG) and two polysaccharide hydrogels (PHGs) were probed in air; their interfacial structures with silica were examined using SFG in water and protein solutions, respectively. Both ZWHG and PHGs interfaces in water were dominated by strongly hydrogen-bonded water molecules, but the bonding strength associated with ZWHG was much stronger. Although all hydrogels experienced interfacial change in the presence of protein solutions, after cleaning, the zwitterionic hydrogel interface recovered almost completely while the other two hydrogels were subject to irreversible protein adsorption. Additionally, orientational analysis of ZWHG methyl groups in water was conducted and related to the superior hydrogen-bonding strength of water molecules at the ZWHG interface. The interfacial structures of hydrogel materials probed by SFG can be correlated to their antifouling properties. This research highlighted the critical role that hydrogen-bonding strength of interfacial water molecules play for antifouling applications.

Ideal reversible polymer networks.

In this article we introduce the concept of ideal reversible polymer networks, which have well-controlled polymer network structures similar to ideal covalent polymer networks but exhibit viscoelastic behaviors due to the presence of reversible crosslinks. We first present a theory to describe the mechanical properties of ideal reversible polymer networks. Because short polymer chains of equal length are used to construct the network, there are no chain entanglements and the chains' Rouse relaxation time is much shorter than the reversible crosslinks' characteristic time. Therefore, the ideal reversible polymer network behaves as a single Maxwell element of a spring and a dashpot in series, with the instantaneous shear modulus and relaxation time determined by the concentration of elastically-active chains and the dynamics of reversible crosslinks, respectively. The theory provides general methods to (i) independently control the instantaneous shear modulus and relaxation time of the networks, and to (ii) quantitatively measure kinetic parameters of the reversible crosslinks, including reaction rates and activation energies, from macroscopic viscoelastic measurements. To validate the proposed theory and methods, we synthesized and characterized the mechanical properties of a hydrogel composed of 4-arm polyethylene glycol (PEG) polymers end-functionalized with reversible crosslinks. All the experiments conducted by varying pH, temperature and polymer concentration were consistent with the predictions of our proposed theory and methods for ideal reversible polymer networks.

Tough bonding of hydrogels to diverse non-porous surfaces.

In many animals, the bonding of tendon and cartilage to bone is extremely tough (for example, interfacial toughness ∼800 J m(-2); refs ,), yet such tough interfaces have not been achieved between synthetic hydrogels and non-porous surfaces of engineered solids. Here, we report a strategy to design tough transparent and conductive bonding of synthetic hydrogels containing 90% water to non-porous surfaces of diverse solids, including glass, silicon, ceramics, titanium and aluminium. The design strategy is to anchor the long-chain polymer networks of tough hydrogels covalently to non-porous solid surfaces, which can be achieved by the silanation of such surfaces. Compared with physical interactions, the chemical anchorage results in a higher intrinsic work of adhesion and in significant energy dissipation of bulk hydrogel during detachment, which lead to interfacial toughness values over 1,000 J m(-2). We also demonstrate applications of robust hydrogel-solid hybrids, including hydrogel superglues, mechanically protective hydrogel coatings, hydrogel joints for robotic structures and robust hydrogel-metal conductors.

Ingestible hydrogel device.

Devices that interact with living organisms are typically made of metals, silicon, ceramics, and plastics. Implantation of such devices for long-term monitoring or treatment generally requires invasive procedures. Hydrogels offer new opportunities for human-machine interactions due to their superior mechanical compliance and biocompatibility. Additionally, oral administration, coupled with gastric residency, serves as a non-invasive alternative to implantation. Achieving gastric residency with hydrogels requires the hydrogels to swell very rapidly and to withstand gastric mechanical forces over time. However, high swelling ratio, high swelling speed, and long-term robustness do not coexist in existing hydrogels. Here, we introduce a hydrogel device that can be ingested as a standard-sized pill, swell rapidly into a large soft sphere, and maintain robustness under repeated mechanical loads in the stomach for up to one month. Large animal tests support the exceptional performance of the ingestible hydrogel device for long-term gastric retention and physiological monitoring.

3D Printing of Living Responsive Materials and Devices.

3D printing has been intensively explored to fabricate customized structures of responsive materials including hydrogels, liquid-crystal elastomers, shape-memory polymers, and aqueous droplets. Herein, a new method and material system capable of 3D-printing hydrogel inks with programed bacterial cells as responsive components into large-scale (3 cm), high-resolution (30 µm) living materials, where the cells can communicate and process signals in a programmable manner, are reported. The design of 3D-printed living materials is guided by quantitative models that account for the responses of programed cells in printed microstructures of hydrogels. Novel living devices are further demonstrated, enabled by 3D printing of programed cells, including logic gates, spatiotemporally responsive patterning, and wearable devices.

Skin-inspired hydrogel-elastomer hybrids with robust interfaces and functional microstructures.

Inspired by mammalian skins, soft hybrids integrating the merits of elastomers and hydrogels have potential applications in diverse areas including stretchable and bio-integrated electronics, microfluidics, tissue engineering, soft robotics and biomedical devices. However, existing hydrogel-elastomer hybrids have limitations such as weak interfacial bonding, low robustness and difficulties in patterning microstructures. Here, we report a simple yet versatile method to assemble hydrogels and elastomers into hybrids with extremely robust interfaces (interfacial toughness over 1,000 Jm(-2)) and functional microstructures such as microfluidic channels and electrical circuits. The proposed method is generally applicable to various types of tough hydrogels and diverse commonly used elastomers including polydimethylsiloxane Sylgard 184, polyurethane, latex, VHB and Ecoflex. We further demonstrate applications enabled by the robust and microstructured hydrogel-elastomer hybrids including anti-dehydration hydrogel-elastomer hybrids, stretchable and reactive hydrogel-elastomer microfluidics, and stretchable hydrogel circuit boards patterned on elastomer.

Stretchable Hydrogel Electronics and Devices.

Stretchable hydrogel electronics and devices are designed by integrating stretchable conductors, functional chips, drug-delivery channels, and reservoirs into stretchable, robust, and biocompatible hydrogel matrices. Novel applications include a smart wound dressing capable of sensing the temperatures of various locations on the skin, delivering different drugs to these locations, and subsequently maintaining sustained release of drugs.