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Hydrogels are highly cross-linked polymer networks that are heavily swollen with water. Hydrogels have been used as dynamic, tunable, degradable materials for growing cells and tissues. Zhang and Khademhosseini review the advances in making hydrogels with improved mechanical strength and greater flexibility for use in a wide range of applications. Science , this issue p. eaaf3627 Hydrogels are formed from hydrophilic polymer chains surrounded by a water-rich environment. They have widespread applications in various fields such as biomedicine, soft electronics, sensors, and actuators. Conventional hydrogels usually possess limited mechanical strength and are prone to permanent breakage. Further, the lack of dynamic cues and structural complexity within the hydrogels has limited their functions. Recent developments include engineering hydrogels that possess improved physicochemical properties, ranging from designs of innovative chemistries and compositions to integration of dynamic modulation and sophisticated architectures. We review major advances in designing and engineering hydrogels and strategies targeting precise manipulation of their properties across multiple scales.

Hydrogels, networks of water-swollen polymers, are being exploited for the local delivery of cells and biologically relevant molecules. Loebel et al . describe the preparation of supramolecular hydrogels and their characterization. The design of injectable hydrogel systems addresses the growing demand for minimally invasive approaches for local and sustained delivery of therapeutics. We developed a class of hyaluronic acid (HA) hydrogels that form through noncovalent guest–host interactions, undergo disassembly (shear-thinning) when injected through a syringe and then reassemble within seconds (self-healing) when shear forces are removed. Its unique properties enable the use of this hydrogel system for numerous applications, such as injection in vivo (including with cells and therapeutic molecules) or as a 'bioink' in 3D-printing applications. Here, we describe the functionalization of HA either with adamantanes (guest moieties) via controlled esterification or with β-cyclodextrins (host moieties) through amidation. We also describe how to modify the HA derivatives with methacrylates for secondary covalent cross-linking and for reaction with fluorophores for in vitro and in vivo imaging. HA polymers are rationally designed from relatively low-molecular-weight starting materials, with the degree of modification controlled, and have matched guest-to-host stoichiometry, allowing the preparation of hydrogels with tailored properties. This procedure takes 3–4 weeks to complete. We detail the preparation and characterization of the guest–host hydrogels, including assessment of their rheological properties, erosion and biomolecule release in vitro . We furthermore demonstrate how to encapsulate cells in vitro and provide procedures for quantitative assessment of in vivo hydrogel degradation by imaging of fluorescently derivatized materials.

Owing to their ultralow thermal conductivity and open pore structure 1 – 3 , silica aerogels are widely used in thermal insulation 4 , 5 , catalysis 6 , physics 7 , 8 , environmental remediation 6 , 9 , optical devices 10 and hypervelocity particle capture 11 . Thermal insulation is by far the largest market for silica aerogels, which are ideal materials when space is limited. One drawback of silica aerogels is their brittleness. Fibre reinforcement and binders can be used to overcome this for large-volume applications in building and industrial insulation 5 , 12 , but their poor machinability, combined with the difficulty of precisely casting small objects, limits the miniaturization potential of silica aerogels. Additive manufacturing provides an alternative route to miniaturization, but was “considered not feasible for silica aerogel” 13 . Here we present a direct ink writing protocol to create miniaturized silica aerogel objects from a slurry of silica aerogel powder in a dilute silica nanoparticle suspension (sol). The inks exhibit shear-thinning behaviour, owing to the high volume fraction of gel particles. As a result, they flow easily through the nozzle during printing, but their viscosity increases rapidly after printing, ensuring that the printed objects retain their shape. After printing, the silica sol is gelled in an ammonia atmosphere to enable subsequent processing into aerogels. The printed aerogel objects are pure silica and retain the high specific surface area (751 square metres per gram) and ultralow thermal conductivity (15.9 milliwatts per metre per kelvin) typical of silica aerogels. Furthermore, we demonstrate the ease with which functional nanoparticles can be incorporated. The printed silica aerogel objects can be used for thermal management, as miniaturized gas pumps and to degrade volatile organic compounds, illustrating the potential of our protocol. A direct ink writing protocol for silica aerogels enables 3D printing of lightweight, miniaturized objects with complex shapes, with the possibility to easily add functionality by incorporating nanoparticles.

Macroscopic graphene structures such as graphene papers and fibres can be manufactured from individual two-dimensional graphene oxide sheets by a fluidics-enabled assembling process. However, achieving high thermal-mechanical and electrical properties is still challenging due to non-optimized microstructures and morphology. Here, we report graphene structures with tunable graphene sheet alignment and orientation, obtained via microfluidic design, enabling strong size and geometry confinements and control over flow patterns. Thin flat channels can be used to fabricate macroscopic graphene structures with perfectly stacked sheets that exhibit superior thermal and electrical conductivities and improved mechanical strength. We attribute the observed shape and size confinements to the flat distribution of shear stress from the anisotropic microchannel walls and the enhanced shear thinning degree of large graphene oxide sheets in solution. Elongational and step expansion flows are created to produce large-scale graphene tubes and rods with horizontally and perpendicularly aligned graphene sheets by tuning the elongational and extensional shear rates, respectively.Sheet alignment and orientation order of graphene structures induced by microfluidics design enable the optimization of electronic and mechanical properties of macroscopic graphene fibres.

We propose to explain shear-thinning behaviour observed in most concentrated non-Brownian suspensions by variable friction between particles. Considering the low magnitude of the forces experienced by the particles of suspensions under shear flow, it is first argued that rough particles come into solid contact through one or a few asperities. In such a few-asperity elastic–plastic contact, the friction coefficient is expected not to be constant but to decrease with increasing normal load. Simulations based on the force coupling method and including such a load-dependent friction coefficient are performed for various particle volume fractions. The results of the numerical simulations are compared to viscosity measurements carried out on suspensions of polystyrene particles ( $40~\\unicode[STIX]{x03BC}\\text{m}$ in diameter) dispersed in a Newtonian silicon oil. The agreement is shown to be satisfactory. Furthermore, the comparison between the simulations conducted either with a constant or a load-dependent friction coefficient provides a model for the shear-thinning viscosity. In this model the effective friction coefficient $\\unicode[STIX]{x1D707}^{eff}$ is specified by the effective normal contact force which is simply proportional to the bulk shear stress. As the shear stress increases, $\\unicode[STIX]{x1D707}^{eff}$ decreases and the jamming volume fraction increases, leading to the reduction of the viscosity. Finally, using this model, we show that it is possible to evaluate the microscopic friction coefficient for each applied shear stress from the rheometric measurements.

The Li dendrite growth and the liquid electrolyte volatilization under semi-open architecture are intrinsic issues for Li-O 2 battery. In this work, we propose a non-Newtonian fluid quasi-solid electrolyte (NNFQSE) SiO 2 -SO 3 Li/PVDF-HFP, which has both shear-thinning and shear-thickening properties. The component interactions among the sulfonated silica nanoparticles, liquid electrolyte, and polymer network are beneficial for decent Li + conductivity and high liquid electrolyte retention without volatilization. Furthermore, NNFQSE exhibits shear-thinning property to eliminate the stress of dendrite growth during repeated cycling. Meanwhile, when the force suddenly increases, such as a high current rate, the NNFQSE may dynamically turn shear-thickening to respond and mechanically stiffen to inhibit the lithium dendrite penetration. By coupling with the NNFQSE, the lithium symmetrical battery can run over 2000 h under 1 mA cm −2 at room temperature, and the quasi-solid Li-O 2 battery actualizes long life above 5000 h at 100 mA g −1 . Lithium dendrite growth and liquid electrolyte volatilization limit the further development of lithium-oxygen batteries. Here, authors report a non-Newtonian fluid quasi-solid electrolyte to address those issues, which improve the life duration of the lithium-oxygen batteries.

The biofabrication of three-dimensional (3D) tissues that recapitulate organ-specific architecture and function would benefit from temporal and spatial control of cell-cell interactions. Bioprinting, while potentially capable of achieving such control, is poorly suited to organoids with conserved cytoarchitectures that are susceptible to plastic deformation. Here, we develop a platform, termed Spatially Patterned Organoid Transfer (SPOT), consisting of an iron-oxide nanoparticle laden hydrogel and magnetized 3D printer to enable the controlled lifting, transport, and deposition of organoids. We identify cellulose nanofibers as both an ideal biomaterial for encasing organoids with magnetic nanoparticles and a shear-thinning, self-healing support hydrogel for maintaining the spatial positioning of organoids to facilitate the generation of assembloids. We leverage SPOT to create precisely arranged assembloids composed of human pluripotent stem cell-derived neural organoids and patient-derived glioma organoids. In doing so, we demonstrate the potential for the SPOT platform to construct assembloids which recapitulate key developmental processes and disease etiologies. Bioprinting has potential in the biofabrication of three dimensional tissues, but is poorly suited to the manipulation of neural organoids. Here, the authors develop a bioprinting platform to allow the arrangement of organoids to form assembloids.

We study the rheology of dry and wet granular materials in the steady quasistatic regime using the discrete element method in a split-bottom ring shear cell with focus on the macroscopic friction. The aim of our study is to understand the local rheology of bulk flow at various positions in the shear band, where the system is in critical state. We develop a general(ized) rheology, in which the macroscopic friction is factorized into a product of four functions, on top of the classical ( I ) rheology, each of which depends on exactly one dimensionless control parameter, quantifying the relative importance of different micro-mechanical machanisms. These four control parameters relate the time scales of shear rate t γ ˙ , particle stiffness tk, gravity tg and cohesion tc, respectively, with the governing time scale of confining pressure tp. While t γ ˙ is large and thus of little importance for most of the slow flow data studied, it increases the friction in critical state, where the shear rate is high and decreases friction by relaxation (creep) where the shear rate is low. tg and tk are comparable to tp in the bulk, but become more or less dominant relative to tp at the extremes of low pressure at the free surface and high pressure deep inside the bulk, respectively. The effect of wet cohesion on the flow rheology is quantified by tc decreasing with increasing cohesion. Furthermore, the proposed rheological model predicts well the shear thinning behavior both in the bulk and near the free surface; shear thinning rate becomes less near the free surface with increasing cohesion.

Microfluidic tools and techniques for manipulating fluid droplets have become core to many scientific and technological fields. Despite the plethora of existing approaches to fluidic manipulation, non-Newtonian fluid phenomena are rarely taken advantage of. Here we introduce embedded droplet printing—a system and methods for the generation, trapping, and processing of fluid droplets within yield-stress fluids, materials that exhibit extreme shear thinning. This technique allows for the manipulation of droplets under conditions that are simply unattainable with conventional microfluidic methods, namely the elimination of exterior influences including convection and solid boundaries. Because of this, we believe embedded droplet printing approaches an ideal for the experimentation, processing, or observation of many samples in an “absolutely quiescent” state, while also removing some troublesome aspects of microfluidics including the use of surfactants and the complexity of device manufacturing. We characterize a model material system to understand the process of droplet generation inside yield-stress fluids and develop a nascent set of archetypal operations that can be performed with embedded droplet printing. With these principles and tools, we demonstrate the benefits and versatility of our method, applying it toward the diverse applications of pharmaceutical crystallization, microbatch chemical reactions, and biological assays.

Most mono- and co-culture bioprocess applications rely on large-scale suspension fermentation technologies that are not easily portable, reusable, or suitable for on-demand production. Here, we describe a hydrogel system for harnessing the bioactivity of embedded microbes for on-demand small molecule and peptide production in microbial mono-culture and consortia. This platform bypasses the challenges of engineering a multi-organism consortia by utilizing a temperature-responsive, shear-thinning hydrogel to compartmentalize organisms into polymeric hydrogels that control the final consortium composition and dynamics without the need for synthetic control of mutualism. We demonstrate that these hydrogels provide protection from preservation techniques (including lyophilization) and can sustain metabolic function for over 1 year of repeated use. This approach was utilized for the production of four chemical compounds, a peptide antibiotic, and carbohydrate catabolism by using either mono-cultures or co-cultures. The printed microbe-laden hydrogel constructs’ efficiency in repeated production phases, both pre- and post-preservation, outperforms liquid culture. Large scale suspension fermentation technology is not easily portable or reusable. Here the authors describe a hydrogel system suitable for long-term and reusable production with both single and multi-organism consortia.