Printable Hydrogel Arrays for Portable and High-Throughput Shear-Mediated Assays.

Hydrogels have been widely used to entrap biomolecules for various biocatalytic reactions. However, solute diffusion in these matrices to initiate such reactions can be a very slow process. Conventional mixing remains a challenge as it can cause irreversible distortion or fragmentation of the hydrogel itself. To overcome the diffusion-limit, a shear-stress-mediated platform named the portable vortex-fluidic device (P-VFD) is developed. P-VFD is a portable platform which consists of two main components, (i) a plasma oxazoline-coated polyvinyl chloride (POx-PVC) film with polyacrylamide and alginate (PAAm/Alg-Ca2+) tough hydrogel covalently bound to its surface and (ii) a reactor tube (L × D: 90 mm × 20 mm) where the aforementioned POx-PVC film could be readily inserted for reactions. Through a spotting machine, the PAAm/Alg-Ca2+ hydrogel can be readily printed on a POx-PVC film in an array pattern and up to 25.4 J/m2 adhesion energy can be achieved. The hydrogel arrays on the film not only offer a strong matrix for entrapping biomolecules such as streptavidin-horseradish peroxidase but are also shear stress-tolerant in the reactor tube, enabling a >6-fold increase in its reaction rate after adding tetramethylbenzidine, relative to incubation. Through using the tough hydrogel and its stably bonded substrate, this portable platform effectively overcomes the diffusion-limit and achieves fast assay detection without causing appreciable hydrogel array deformation or dislocation on the substrate film.

Computational homogenisation based extraction of transverse tensile cohesive responses of cortical bone tissue.

The numerical assessment of fracture properties of cortical bone is important in providing suggestions on patient-specific clinical treatments. We present a generic finite element modelling framework incorporating computational fracture approaches and computational homogenisation techniques. Finite element computations for statistical volume elements (SVEs) at the microscale are performed for different sizes with random osteon packing with a fixed volume fraction. These SVEs are loaded in the transverse direction under tension. The minimal SVE size in terms of ensuring a representative effective cohesive law is suggested to be 0.6 mm. Since cement lines as weak interfaces play a key role in bone fracture, the effects of their fracture properties on the effective fracture strength and toughness are investigated. The extracted effective fracture properties can be used as homogenised inputs to a discrete crack simulation at macroscopic or structural scale. The extrinsic toughening mechanisms observed in the SVE models are discussed with a comparison against experimental observations from the literature, giving beneficial insights to cortical bone failure.

Mechanical Properties of a Supramolecular Nanocomposite Hydrogel Containing Hydroxyl Groups Enriched Hyper-Branched Polymers.

Owing to highly tunable topology and functional groups, hyper-branched polymers are a potential candidate for toughening agents, for achieving supramolecular interactions with hydrogel networks. However, their toughening effects and mechanisms are not well understood. Here, by means of tensile and pure shear testings, we characterise the mechanics of a nanoparticle-hydrogel hybrid system that incorporates a hyper-branched polymer (HBP) with abundant hydroxyl end groups into the matrix of the polyacrylic acid (PAA) hydrogel. We found that the third and fourth generations of HBP are more effective than the second one in terms of strengthening and toughening effects. At a HBP content of 14 wt%, compared to that of the pure PAA hydrogel, strengths of the hybrid hydrogels with the third and fourth HBPs are 2.3 and 2.5 times; toughnesses are increased by 525% and 820%. However, for the second generation, strength is little improved, and toughness is increased by 225%. It was found that the stiffness of the hybrid hydrogel is almost unchanged relative to that of the PAA hydrogel, evidencing the weak characteristic of hydrogen bonds in this system. In addition, an outstanding self-healing feature was observed, confirming the fast reforming nature of broken hydrogen bonds. For the hybrid hydrogel, the critical size of failure zone around the crack tip, where serious viscous dissipation occurs, is related to a fractocohesive length, being about 0.62 mm, one order of magnitude less than that of other tough double-network hydrogels. This study can promote the application of hyper-branched polymers in the rapid evolving field of hydrogels for improved performance.

Hydrogen Bonding-Reinforced Hydrogel Electrolyte for Flexible, Robust, and All-in-One Supercapacitor with Excellent Low-Temperature Tolerance.

Flexible supercapacitors are promising energy storage devices for emerging wearable electronics. However, due to the poor mechanical strength, complicated device manufacturing process, and unsatisfactory low-temperature tolerance, their overall performance for practical applications is hindered. Herein, we report a hydrogen bonding-reinforced, dual-crosslinked poly(vinyl alcohol), acrylic acid, and H2SO4 (PVA-AA-S) hydrogel electrolyte for all-in-one flexible supercapacitors. The PVA-AA-S hydrogel demonstrates excellent compressive/tensile properties and high ionic conductivity. It tolerates compressive stress of 0.53 MPa and is stretchable up to 500%. The hydrogel-based all-in-one supercapacitor shows promising electrochemical performance under various harsh conditions. The device energy density and power density reach up to 14.2 µWh cm-2 and 0.94 mW cm-2, respectively. Furthermore, it retains nearly 80% capacitance after being stored at -35 °C for 23 days. The excellent performance of the hydrogel electrolyte originates from its abundant strong hydrogen bonding between polymer chains and water molecules.