Hydrogel for light delivery in biomedical applications.

Traditional optical waveguides or mediums are often silica-based materials, but their applications in biomedicine and healthcare are limited due to the poor biocompatibility and unsuitable mechanical properties. In term of the applications in human body, a biocompatible hydrogel system with excellent optical transparency and mechanical flexibility could be beneficial. In this review, we explore the different designs of hydrogel-based optical waveguides derived from natural and synthetic sources. We highlighted key developments such as light emitting contact lenses, implantable optical fibres, biosensing systems, luminating and fluorescent materials. Finally, we expand further on the challenges and perspectives for hydrogel waveguides to achieve clinical applications.

Nanochitin for sustainable and advanced manufacturing.

Presently, the rapid depletion of resources and drastic climate change highlight the importance of sustainable development. In this case, nanochitin derived from chitin, the second most abundant renewable polymer in the world, possesses numerous advantages, including toughness, easy processability and biodegradability. Furthermore, it exhibits better dispersibility in various solvents and higher reactivity than chitin owing to its increased surface area to volume ratio. Additionally, it is the only natural polysaccharide that contains nitrogen. Therefore, it is valuable to further develop this innovative technology. This review summarizes the recent developments in nanochitin and specifically identifies sustainable strategies for its preparation. Additionally, the different biomass sources that can be exploited for the extraction of nanochitin are highlighted. More importantly, the life cycle assessment of nanochitin preparation is discussed, followed by its applications in advanced manufacturing and perspectives on the valorization of chitin waste.

Hydrogel-Based Flexible Electronics.

Flexible electronics is an emerging field of research involving multiple disciplines, which include but not limited to physics, chemistry, materials science, electronic engineering, and biology. However, the broad applications of flexible electronics are still restricted due to several limitations, including high Young's modulus, poor biocompatibility, and poor responsiveness. Innovative materials aiming for overcoming these drawbacks and boost its practical application is highly desirable. Hydrogel is a class of 3D crosslinked hydrated polymer networks, and its exceptional material properties render it as a promising candidate for the next generation of flexible electronics. Here, the latest methods of synthesizing advanced functional hydrogels and the state-of-art applications of hydrogel-based flexible electronics in various fields are reviewed. More importantly, the correlation between properties of the hydrogel and device performance is discussed here, to have better understanding of the development of flexible electronics by using environmentally responsive hydrogels. Last, perspectives on the current challenges and future directions in the development of hydrogel-based multifunctional flexible electronics are provided.

PVA/pectin composite hydrogels inducing osteogenesis for bone regeneration.

Hydrogels composed from biomolecules have gained great interests as biomaterials for tissue engineering. However, their poor mechanical properties limit their application potential. Here, we synthesized a series of tough composite hydrogels from poly (vinyl alcohol) (PVA) and pectin for bone tissue engineering. With a balance of scaffold stiffness and pore size, PVA-Pec-10 hydrogel enhanced adhesion and proliferation of osteoblasts. The hydrogel significantly promoted osteogenesis in vitro by improving the alkaline phosphates (ALP) activity and calcium biomineralization, as well as upregulating the expressions of osteoblastic genes. The composite hydrogel also accelerated the bone healing process in vivo after transplantation into the femoral defect. Additionally, our study demonstrated that pectin and its Ca2+ crosslinking network play a crucial role of inducing osteogenesis through regulating the Ca2+/CaMKII and BMP-SMAD1/5 signaling. The optimized structure composition and multifunctional properties make PVA-Pec hydrogel highly promising to serve as a candidate for bone tissue regeneration.

Dynamic Grafting of Carboxylates onto Poly(Vinyl Alcohol) Polymers for Supramolecularly-Crosslinked Hydrogel Formation.

Supramolecular hydrogels have attracted considerable interest due to their unique stimuli-responsive and self-healing properties. However, these hydrogel systems are usually achieved by covalent grafting of supramolecular units onto the polymer backbone, which in turn limits their reprocessability. Herein, we prepared a supramolecular hydrogel system by forming dynamic covalent crosslinks between 4-carboxyphenylboronic acid (CPBA) and polyvinyl alcohol (PVA). The system was then further crosslinked with either calcium ions or branched polyethylenimine (PEI) to generate hydrogels with distinctly different properties. Incorporation of calcium ions resulted in the formation of hydrogels with higher storage modulus of 7290 Pa but without self-healing properties. On the other hand, PEI-crosslinked hydrogel (PVA-CPBA-PEI) exhibited >2000% critical strain value, demonstrated high stability over 52 days and showed sustained antibacterial effect. A combination of supramolecular interactions and dynamic covalent crosslinks can be an alternate strategy to fabricate next-generation hydrogel materials.

Cationic Lignin-Based Hyperbranched Polymers to Circumvent Drug Resistance in Pseudomonas Keratitis.

The rise of antimicrobial-resistant bacteria strains has been a global public health concern due to their ability to cause increased patient morbidity and a greater burden on the healthcare system. As one of the potential solutions to overcome such bacterial infections, hyperbranched copolymers with cationic charges were developed. These copolymers were assessed for their antimicrobial efficacy and their bactericidal mechanisms. They were found to be potent against mobile colistin-resistant 1 strains, which was significant as colistin is known to be the last-resort antibiotic against Gram-negative bacteria. Furthermore, there was no sign of mutational resistance developed by E. ColiATCC 25922 and MCR 1+E. Coli against the copolymer even up to 20 passages. The ability to evade inducing resistance would provide invaluable insights for future antibiotic development. Our studies suggest that the bactericidal efficacy comes from the ability to target the outer membrane efficaciously. In vivo study using a Pseudomonas keratitis model showed that the copolymer was compatible with the eye and further supported that the copolymer treatment was effective for complete bacteria elimination.

A New Potent Antimicrobial Metalloporphyrin.

A series of bis-acryl functionalized porphyrins and their corresponding metalloporphyrins (M=Co, Mn) were synthesized and investigated for their antimicrobial properties through MIC screening and bacteria time-kill kinetic studies. The Mn(III) 4-(bis)methylphenyl-substituted-porphyrins showed superior batericidal activities even in the dark with low hemotoxicity and good cytotoxicity profile.

Recycling of spent coffee grounds for useful extracts and green composites.

Large amounts of spent coffee grounds (SCGs) are often discarded and there is a need to find alternative disposal methods due to environmental concerns. This project aims to develop sustainable materials by re-purposing spent coffee grounds (SCGs). Oil extraction was performed using different organic solvents and yielded approximately 10% coffee oil. Coffee oil contains potentially useful chemical compounds such as fatty acids and caffeine. They also exhibited antioxidant properties. Extracted SCGs (ESCGs) were blended with epoxy resin to form composites. ESCG composites displayed a general decrease in mechanical properties relative to epoxy. However, improvements were observed when comparing ESCG composites and SCG composites. The greatest improvement belongs to epoxy composite filled with acetone-ESCGs, where the tensile strength, flexural modulus and flexural strength increased to 23.4 MPa, 3.02 GPa and 42.9 MPa respectively. This study presents a way to exploit waste materials which contributes to the goal of sustainability.

Sanitizing agents for virus inactivation and disinfection.

Viral epidemics develop from the emergence of new variants of infectious viruses. The lack of effective antiviral treatments for the new viral infections coupled with rapid community spread of the infection often result in major human and financial loss. Viral transmissions can occur via close human-to-human contact or via contacting a contaminated surface. Thus, careful disinfection or sanitization is essential to curtail viral spread. A myriad of disinfectants/sanitizing agents/biocidal agents are available that can inactivate viruses, but their effectiveness is dependent upon many factors such as concentration of agent, reaction time, temperature, and organic load. In this work, we review common commercially available disinfectants agents available on the market and evaluate their effectiveness under various application conditions. In addition, this work also seeks to debunk common myths about viral inactivation and highlight new exciting advances in the development of potential sanitizing agents.

Recent innovations in artificial skin.

The skin is a "smart", multifunctional organ that is protective, self-healing and capable of sensing and many forms of artificial skins have been developed with properties and functionalities approximating those of natural skin. Starting from specific commercial products for the treatment of burns, progress in two fields of research has since allowed these remarkable materials to be viable skin replacements for a wide range of dermatological conditions. This review maps out the development of bioengineered skin replacements and synthetic skin substitutes, including electronic skins. The specific behaviors of these skins are highlighted, and the performances of both types of artificial skins are evaluated against this. Moving beyond mere replication, highly advanced artificial skin materials are also identified as potential augmented skins that can be used as flexible electronics for health-care monitoring and other applications.

Cationic Poly([R]-3-hydroxybutyrate) Copolymers as Antimicrobial Agents.

Poly([R]-3-hydroxybutyrate) (PHB), a natural biodegradable polyester, has attracted much attention as a new biomaterial because of its sustainability and good biocompatibility. In this study, it is discovered that PHB can be conveniently functionalized to obtain a number of platform chain architectures that may provide a wide range of functional copolymers. In a transesterification reaction, linear (di-hydroxylated) and star shaped (tri- and tetra-hydroxylated) PHB oligomers are synthesized, followed by copolymerization with 2-(dimethylamino)ethyl methacrylate and quaternization with benzyl bromide to afford antimicrobial properties. The antimicrobial activities of the quaternary salts against clinically relevant pathogens on the interactions with outer and cytoplasmic membranes, lethal mechanisms, multipassage resistance, and synergy effect with antibiotics are investigated. Cationic PHB copolymers show effectiveness as antimicrobial agents, with minimum inhibitory concentration values 0.24-0.65 µm (or µmol dm-3 ) (or 32-128 µg mL-1 ) against Gram-positive and Gram-negative bacteria. Modifying the copolymer architectures into star shapes results in enhanced effectiveness to disrupt the membrane integrity. Synergistic effects are attained for all the quaternized PHB derivatives when they are used together with tobramycin. Multipassage resistance does not occur in both the linear and star derivatives against Gram-negative bacteria after 20 passages.

Using Artificial Skin Devices as Skin Replacements: Insights into Superficial Treatment.

Artificial skin devices are able to mimic the flexibility and sensory perception abilities of the skin. They have thus garnered attention in the biomedical field as potential skin replacements. This Review delves into issues pertaining to these skin-deep devices. It first elaborates on the roles that these devices have to fulfill as skin replacements, and identify strategies that are used to achieve such functionality. Following which, a comparison is done between the current state of these skin-deep devices and that of natural skin. Finally, an outlook on artificial skin devices is presented, which discusses how complementary technologies can create skin enhancements, and what challenges face such devices.

Supramolecular hydrogels for antimicrobial therapy.

The emergence of drug-resistant microbes has become a threat to global health, and microbial infections severely limit the use of healthcare materials. To achieve efficient antimicrobial therapy, supramolecular hydrogels demonstrate unprecedented advantages in medical applications due to the tunable and reversible nature of their supramolecular interactions and the capability of hydrogels to incorporate various therapeutic agents. Herein, antimicrobial hydrogels are categorized according to their inherent antimicrobial properties or based on their roles in encapsulating antimicrobial materials. Moreover, strategies to further enhance the antimicrobial efficacy of hydrogels are highlighted, such as the incorporation of antifouling agents or the enabling of response towards physiological cues. We envision that supramolecular hydrogels, in combination with modern medical technology and devices, will contribute to the development of efficient and safe systems for antimicrobial therapy.

Micellized α-Cyclodextrin-Based Supramolecular Hydrogel Exhibiting pH-Responsive Sustained Release and Corresponding Oscillatory Shear Behavior Analysis.

The fabrication of supramolecular hydrogels from micellized PLLA/DMAEMA/PEGMA polymers with α-CD has been explored to design injectable gel formulations for sustained drug release. The tricomponent hydrogels (5% w/v)/α-CD (10% w/v) were able to sustain protein (BSA and lysozyme) release for 60-120 h at different pH conditions (pH 3, 7 and 10). In-depth rheological analysis highlighted the role of pH in tuning hydrogel behavior upon shear at microscopic level affecting protein release profiles. Protein release involved complex interactions within the network (isoelectric point and diffusion coefficient of the protein, pKa of DMAEMA, and pore size of the hydrogel). Lissajous-Bowditch curves explained the microstructural response to increasing strain which weakened the supramolecular association and collapsed the formation of the porous hydrogel. Power Law was adopted to represent both transport mechanism and drug release phenomena. The release mechanism resulted from a combination of erosion- and diffusion-controlled release (non-Fickian and super case II).

Supramolecular cyclodextrin pseudorotaxane hydrogels: a candidate for sustained release?

In this work, PEO-α-CD pseudorotaxane hydrogels were prepared. The gels were loaded with proteins, BSA and lysozyme, representing proteins with different molecular weights. The kinetics of protein release was studied. Factors such as PEO concentration, protein concentration and exposed surface area of the gels were investigated to understand their effects on the release of the encapsulated cargo. Erosion of the gel surface appeared to be the dominant factor for release of the proteins. Fitting the data to various models supported our hypothesis that the mechanism of release was primarily erosion-driven as the data was best described by zero order, power law and Hopfenberg model. The linear relationship between the amount of mass loss and time establishes the erosion of the polymer gel matrix to be the key factor for drug release.