Bioprinting microporous functional living materials from protein-based core-shell microgels.

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.

Recent Advances in Microgels: From Biomolecules to Functionality.

The emerging applications of hydrogel materials at different length scales, in areas ranging from sustainability to health, have driven the progress in the design and manufacturing of microgels. Microgels can provide miniaturized, monodisperse, and regulatable compartments, which can be spatially separated or interconnected. These microscopic materials provide novel opportunities for generating biomimetic cell culture environments and are thus key to the advances of modern biomedical research. The evolution of the physical and chemical properties has, furthermore, highlighted the potentials of microgels in the context of materials science and bioengineering. This review describes the recent research progress in the fabrication, characterization, and applications of microgels generated from biomolecular building blocks. A key enabling technology allowing the tailoring of the properties of microgels is their synthesis through microfluidic technologies, and this paper highlights recent advances in these areas and their impact on expanding the physicochemical parameter space accessible using microgels. This review finally discusses the emerging roles that microgels play in liquid-liquid phase separation, micromechanics, biosensors, and regenerative medicine.

Injectable Granular Hydrogels as Colloidal Assembly Microreactors for Customized Structural Colored Objects.

While structural coloration has captured considerable interests across different areas in the past decades, the development of macroscopic objects with tailorable structural colors remains a challenge due to the difficulty of large-scale fabrication of finely ordered nanostructures and poor processability of their constituent materials. In this work, a type of photonic granular hydrogel is developed as a novel printable ink for constructing customized structural colored objects. The magnetochromatic ink exhibits dynamic properties such as shear thinning and self-healing, enabling direct writing of macroscopic structural colored patterns by extrusion 3D printing. Further, the modularity of the photonic ink allows additive color mixing, which obviates the need for arduous nano-synthesis and expands on the color abundance of structural colored materials in a simple yet efficient manner. These characteristics grant novel photonic inks with great applicability to a variety of fields including switchable color displays, sensors, etc.

3D Printed Biocatalytic Living Materials with Dual-Network Reinforced Bioinks.

The field of living materials seeks to harness living cells as microfactories that can construct a material itself or enhance the performance of material in some manner. While recent advances in 3D printing allow microbe manipulation to create bespoke living materials, the effective coupling of these living components in reinforced bioink designs remains a major challenge due to the difficulty in building a robust and cell-friendly microenvironment. Here, a type of dual-network bioink is reported for the 3D printing of living materials with enhanced biocatalysis capabilities, where bioinks are readily printable and provide a biocompatible environment along with desirable mechanical performance. It is demonstrated that integrating microbes into these bioinks enables the direct printing of catalytically living materials with high cell viability and maintains metabolic activity, which those living materials can be preserved and reused. Further, a bacteria-algae coculture system is fabricated for the bioremediation of chemicals, giving rise to its potential field applications.

Droplet microfluidics on analysis of pathogenic microbes for wastewater-based epidemiology.

Infectious diseases caused by pathogenic microbes have posed a major health issue for the public, such as the ongoing COVID-19 global pandemic. In recent years, wastewater-based epidemiology (WBE) is emerging as an effective and unbiased method for monitoring public health. Despite its increasing importance, the advancement of WBE requires more competent and streamlined analytical platforms. Herein we discuss the interactions between WBE and droplet microfluidics, focusing on the analysis of pathogens in droplets, which is hard to be tackled by traditional analytical tools. We highlight research works from three aspects, namely, quantitation of pathogen biomarkers in droplets, single-cell analysis in droplets, and living cell biosensors in droplets, as well as providing future perspectives on the synergy between WBE and droplet microfluidics.

Photonic Plasticines with Uniform Structural Colors, High Processability, and Self-Healing Properties.

Despite the vast variety of colloidal superstructures available in soft matter photonics, it remains challenging to balance the trade-off between their optical microstructures and material processability. By synergizing colloidal photonics and dynamic chemistry, a type of photonic "plasticine" with characteristics of uniform structural colors, high processability, and self-healing is demonstrated. Specifically, a boronate ester bond-based macromonomer is first prepared through complexation between the diols of polyvinyl alcohol and the boronic acid group of 3-(acrylamido) phenylboronic acid in the presence of concentrated silica colloids. Upon photopolymerization, the dynamic photonic plasticine is formed in situ as the result of the crosslinking of the boronate ester bonded networks. The randomly packed colloids inside the plasticine compose the amorphous photonic crystals, giving rise to angle-independent structural colors that would not compromise during subsequent processing steps; the reversible nature of the boronate ester bonds endows the plasticine with self-adaptable and self-healing properties. Further, the plasticine is also compatible with common shaping methods, that is, cutting, molding, and carving, and thus can be facilely processed into 3D structural colored objects, holding great potentials in fields such as bio-encoding, optical filters, anti-counterfeiting, etc.