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In this work, a two component microgel assembly using soft anisometric microgels that interlink to create a 3D macroporous construct for cell growth is reported. Reactive microgel rods with variable aspect ratio are produced via microfluidics in a continuous plug‐flow on‐chip gelation method by photoinitiated free‐radical polymerization of star‐polyethylene glycol‐acrylate with glycidyl methacrylate or 2‐aminoethyl methacrylate comonomers. The resulting complementary epoxy‐ and amine‐functionalized microgels assemble and interlink with each other via a ring opening reaction, resulting in macroporous constructs with pores up to several hundreds of micrometers. The level of crosslinking depends on the functionalization degree of the microgels, which also affects the stiffness and cell adhesiveness of the microgels when modified with the cell‐adhesive GRGDS‐PC peptide. Therefore, 3D spreading and growth of cells inside the macroporous structure is influenced not only by the presence of macropores but also by the mechanical and biochemical properties of the individual microgels. Two types of microgel rods produced in microfluidics bear active groups enable quick and stable rod interlinking when they come in contact in the aqueous phase. This way, macroporous scaffolds with micro‐ to millimeter‐scale pores are formed that support 3D‐cell culture of human fibroblasts and endothelial cells. Cells attach, spread, and grow, filling the macropores, building biological‐like tissue material.

This article provides a systematic review of the crosslinking strategies used to produce microgel particles in microfluidic chips. Various ionic crosslinking methods for the gelation of charged polymers are discussed, including external gelation via crosslinkers dissolved or dispersed in the oil phase; internal gelation methods using crosslinkers added to the dispersed phase in their non-active forms, such as chelating agents, photo-acid generators, sparingly soluble or slowly hydrolyzing compounds, and methods involving competitive ligand exchange; rapid mixing of polymer and crosslinking streams; and merging polymer and crosslinker droplets. Covalent crosslinking methods using enzymatic oxidation of modified biopolymers, photo-polymerization of crosslinkable monomers or polymers, and thiol-ene “click” reactions are also discussed, as well as methods based on the sol−gel transitions of stimuli responsive polymers triggered by pH or temperature change. In addition to homogeneous microgel particles, the production of structurally heterogeneous particles such as composite hydrogel particles entrapping droplet interface bilayers, core−shell particles, organoids, and Janus particles are also discussed. Microfluidics offers the ability to precisely tune the chemical composition, size, shape, surface morphology, and internal structure of microgels by bringing multiple fluid streams in contact in a highly controlled fashion using versatile channel geometries and flow configurations, and allowing for controlled crosslinking.

HighlightsThis review provides a comprehensive summary associated with recent progress in the preparation and application of microgels.The characteristics and applications of microgels and microgel-based scaffolds for cell culture and delivery are elaborated with an emphasis on the advantages of these carriers in cell therapy.This review expounds on the ongoing and foreseeable applications and current limitations of microgels and their aggregate in the field of biomedical engineering.Through stimulating innovative ideas, the present review paves new avenues for expanding the application of microgels in cell delivery techniques.Microgels prepared from natural or synthetic hydrogel materials have aroused extensive attention as multifunctional cells or drug carriers, that are promising for tissue engineering and regenerative medicine. Microgels can also be aggregated into microporous scaffolds, promoting cell infiltration and proliferation for tissue repair. This review gives an overview of recent developments in the fabrication techniques and applications of microgels. A series of conventional and novel strategies including emulsification, microfluidic, lithography, electrospray, centrifugation, gas-shearing, three-dimensional bioprinting, etc. are discussed in depth. The characteristics and applications of microgels and microgel-based scaffolds for cell culture and delivery are elaborated with an emphasis on the advantages of these carriers in cell therapy. Additionally, we expound on the ongoing and foreseeable applications and current limitations of microgels and their aggregate in the field of biomedical engineering. Through stimulating innovative ideas, the present review paves new avenues for expanding the application of microgels in cell delivery techniques.

Living materials bring together material science and biology to allow the engineering and augmenting of living systems with novel functionalities. Bioprinting promises accurate control over the formation of such complex materials through programmable deposition of cells in soft materials, but current approaches had limited success in fine-tuning cell microenvironments while generating robust macroscopic morphologies. Here, we address this challenge through the use of core-shell microgel ink to decouple cell microenvironments from the structural shell for further processing. Cells are microfluidically immobilized in the viscous core that can promote the formation of both microbial populations and mammalian cellular spheroids, followed by interparticle annealing to give covalently stabilized functional scaffolds with controlled microporosity. The results show that the core-shell strategy mitigates cell leakage while affording a favorable environment for cell culture. Furthermore, we demonstrate that different microbial consortia can be printed into scaffolds for a range of applications. By compartmentalizing microbial consortia in separate microgels, the collective bioprocessing capability of the scaffold is significantly enhanced, shedding light on strategies to augment living materials with bioprocessing capabilities. Extrusion bioprinting can be used to produce living materials but controlling cell microenvironments is challenging. Here, the authors use a type of core-shell microgel ink that decouples cell culture from material processing to produce functional materials with a range of potential applications.

Thin films made of deformable micro‐ and nano‐units, such as biological membranes, polymer interfaces, and particle‐laden liquid surfaces, exhibit a complex behavior during drying, with consequences for various applications like wound healing, coating technologies, and additive manufacturing. Studying the drying dynamics and structural changes of soft colloidal films thus holds the potential to yield valuable insights to achieve improvements for applications. In this study, interfacial monolayers of core‐shell (CS) microgels with varying degrees of softness are employed as model systems and to investigate their drying behavior on differently modified solid substrates (hydrophobic vs hydrophilic). By leveraging video microscopy, particle tracking, and thin film interference, this study shed light on the interplay between microgel adhesion to solid surfaces and the immersion capillary forces that arise in the thin liquid film. It is discovered that a dried replica of the interfacial microstructure can be more accurately achieved on a hydrophobic substrate relative to a hydrophilic one, particularly when employing softer colloids as opposed to harder counterparts. These observations are qualitatively supported by experiments with a thin film pressure balance which allows mimicking and controlling the drying process and by computer simulations with coarse‐grained models. The drying of soft colloidal films on solid interfaces is a complex process. In this study, core‐shell (CS) microgels are confined at the air/water interface, and investigated for the drying behavior on solid substrates using video microscopy. Variation in shell softness and substrate wettability reveal the complex interplay of different forces including capillary attraction and adhesion to the substrate influencing the microstructure.

Understanding the adsorption features of polymer microgels with different chemical compositions and structures is crucial in studying the mechanisms of respective emulsion stabilization. Specifically, the use of stimuli-responsive particles can introduce new properties and broaden the application range of such complex systems. Recently, we demonstrated that emulsions stabilized by microgels composed of interpenetrating networks (IPNs) of poly-N-isopropylacrylamide (PNIPAM) and polyacrylic acid (PAA) exhibit higher colloidal stability upon heating compared to PNIPAM homopolymer and other relevant PNIPAM-based copolymer counterparts. In the present work, using pendant drop tensiometry, we studied the evolution of water–tetradecane interfacial tension during the adsorption of PNIPAM-PAA IPN particles, comparing them with single-network P-(NIPAM-co-AA) and PNIPAM microgels. The results showed that, despite having the same chemical composition, copolymer particles exhibit completely different adsorption behavior in comparison to other microgel architectures. The observed disparity can be attributed to the nonuniform distribution of charged acrylic acid groups within the P-(NIPAM-co-AA) network obtained through precipitation polymerization. Oppositely, the presence of IPN architecture provides a uniform distribution of different monomers inside respective microgels. Additionally, hydrogen bonding between PNIPAM and PAA subchains appears to reduce the electrostatic energy barrier, enhancing the ability of IPN particles to successfully cover the liquid interface. Overall, our findings confirm the efficiency of using PNIPAM-PAA IPN microgels for the preparation of oil-in-water emulsions and their stability, even when the temperature rises above the lower critical solution temperature of PNIPAM.

Pollen’s practically-indestructible shell structure has long inspired the biomimetic design of organic materials. However, there is limited understanding of how the mechanical, chemical, and adhesion properties of pollen are biologically controlled and whether strategies can be devised to manipulate pollen beyond natural performance limits. Here, we report a facile approach to transform pollen grains into soft microgel by remodeling pollen shells. Marked alterations to the pollen substructures led to environmental stimuli responsiveness, which reveal how the interplay of substructure-specific material properties dictates microgel swelling behavior. Our investigation of pollen grains from across the plant kingdom further showed that microgel formation occurs with tested pollen species from eudicot plants. Collectively, our experimental and computational results offer fundamental insights into how tuning pollen structure can cause dramatic alterations to material properties, and inspire future investigation into understanding how the material science of pollen might influence plant reproductive success. Pollen is an abundant material; but, currently has limited applications. Here, the authors turn pollen grains into soft microgel by de-esterification of pectin molecules and explore the mechanical and structural changes of the pollen grains using physical and modelling approaches.

One strategy that has gained much attention in the last decades is the understanding and further mimicking of structures and behaviours found in nature, as inspiration to develop materials with additional functionalities. This review presents recent advances in stimuli-responsive gels with emphasis on functional hydrogels and microgels. The first part of the review highlights the high impact of stimuli-responsive hydrogels in materials science. From macro to micro scale, the review also collects the most recent studies on the preparation of hybrid polymeric microgels composed of a nanoparticle (able to respond to external stimuli), encapsulated or grown into a stimuli-responsive matrix (microgel). This combination gave rise to interesting multi-responsive functional microgels and paved a new path for the preparation of multi-stimuli “smart” systems. Finally, special attention is focused on a new generation of functional stimuli-responsive polymer hydrogels able to self-shape (shape-memory) and/or self-repair. This last functionality could be considered as the closing loop for smart polymeric gels.

In todays’ world, there is an increasing number of mature oil fields every year, a phenomenon that is leading to the development of more elegant enhanced oil recovery (EOR) technologies that are potentially effective for reservoir profile modification. The technology of conformance control using crosslinked microgels is one the newest trends that is gaining momentum every year. This is due to the simplicity of the treatment process and its management, as well as the guaranteed effect in the case of the correct well candidate selection. We identified the following varieties of microgels: microspheres, thermo- and pH-responsible microgels, thin fracture of preformed particle gels, colloidal dispersed gels. In this publication, we try to combine the available chemical aspects of microgel production with the practical features of their application at oil production facilities. The purpose of this publication is to gather available information about microgels (synthesis method, monomers) and to explore world experience in microgel application for enhanced oil recovery. This article will be of great benefit to specialists engaged in polymer technologies at the initial stage of microgel development.