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Growing evidence supports a critical role of metal-ligand coordination in many attributes of biological materials including adhesion, self-assembly, toughness, and hardness without mineralization [Rubin DJ, Miserez A, Waite JH (2010) Advances in Insect Physiology: Insect Integument and Color, eds Jérôme C, Stephen JS (Academic Press, London), pp 75-133]. Coordination between Fe and catechol ligands has recently been correlated to the hardness and high extensibility of the cuticle of mussel byssal threads and proposed to endow self-healing properties [Harrington MJ, Masic A, Holten-Andersen N, Waite JH, Fratzl P (2010) Science 328:216-220]. Inspired by the pH jump experienced by proteins during maturation of a mussel byssus secretion, we have developed a simple method to control catechol-Fe³⁺ interpolymer cross-linking via pH. The resonance Raman signature of catechol-Fe³⁺ cross-linked polymer gels at high pH was similar to that from native mussel thread cuticle and the gels displayed elastic moduli (G') that approach covalently cross-linked gels as well as self-healing properties.

Ocular in situ gels are a promising alternative to overcome drawbacks of conventional eye drops because they associate the advantages of solutions such as accuracy and reproducibility of dosing, or ease of administration with prolonged contact time of ointments. Chitosan is a natural polymer suitable for use in ophthalmic formulations due to its biocompatibility, biodegradability, mucoadhesive character, antibacterial and antifungal properties, permeation enhancement and corneal wound healing effects. The combination of chitosan, pH-sensitive polymer, with other stimuli-responsive polymers leads to increased mechanical strength of formulations and an improved therapeutic effect due to prolonged ocular contact time. This review describes in situ gelling systems resulting from the association of chitosan with various stimuli-responsive polymers with emphasis on the mechanism of gel formation and application in ophthalmology. It also comprises the main techniques for evaluation of chitosan in situ gels, along with requirements of safety and ocular tolerability.

Sol–gel process is a very unique wet chemical method for producing advanced materials in various areas of research. An increasingly evolution trend of this process is to combine with other technologies, such as surface modification, hybridization, templating induction, self-assembly, and phase separation, for preparing new materials possessing controllable shape, unique microstructure, superior properties, and special application. The review aims to present the synthesis of several typical sol–gel-derived materials (monodisperse nanoparticles, hybrid coatings, hollow microspheres, aerogels, and porous monoliths) via sol–gel process combining with other technologies . Some examples of application of the sol–gel-derived materials are also included.

The study explored the compatibility between the main product of Portland cement hydration and the main product of the alkali activation of fly ash: C–S–H and N–A–S–H gels, respectively. Both gels were synthesized with laboratory reagents at different pH values. Blends of the two were synthesized as well, using the sol–gel procedure. All the gels were characterized with Fourier transform IR spectroscopy (FTIR). The gels synthesized with this procedure were shown to precipitate together with a silica-rich gel. In addition, the pH level was found to play a determinant role in both C–S–H and N–A–S–H gel synthesis. The C–S–H gel is the major phase formed at pH > 11 and N–A–S–H gel for pH > 12. The results relating to the joint synthesis of the two (C–S–H and N–A–S–H) gels were not conclusive. Technique used for the characterization failed to differentiate between them in the blended material.

To balance cost and performance of geopolymers, alkalinity of activating solution is critical. Alkalinity affects condensation that determines the final gel structures, but this effect is confounded by dissolution and is not understood from direct experimental evidence. In this study, we investigated effects of alkalinity on condensation for gels synthesized via a sol–gel method that eliminates dissolution process. As alkalinity increased, particle sizes of the gels increased as indicated by SEM, Si/Al ratios of the gels decreased but polymerization extent increased as supported by FTIR, 27 Al and 23 Na NMR, and composition analysis. The mechanism for the effects of alkalinity was proposed accordingly: (1) increasing alkalinity lowers the Si/Al ratio (i.e., more incorporation of Al) of the resulting products probably by affecting charging conditions of the Si and Al units; (2) the presence of Al(OH) 4 − units promotes their condensation with nearby species to increase the extent of polymerization; (3) enhanced condensation increases particle sizes of the gels even at microstructural level. This understanding on condensation independent of dissolution provides ways to control gel structures and Si/Al ratios and thus tailor properties accordingly, as well as to suggest a strategy (by altering Si/Al ratios during condensation) to develop kinetics-controlling admixtures. Highlights Condensation of geopolymer gel was studied independently of dissolution. Increasing alkalinity lowers Si/Al ratio (i.e., more incorporation of Al) of gel. More incorporated Al units enhance condensation with Si species. Enhanced condensation increases particle sizes of the gel at microstructural level.

Gels formed via metal–ligand coordination typically have very low branch functionality, f , as they consist of ∼2–3 polymer chains linked to single metal ions that serve as junctions. Thus, these materials are very soft and unable to withstand network defects such as dangling ends and loops. We report here a new class of gels assembled from polymeric ligands and metal–organic cages (MOCs) as junctions. The resulting ‘polyMOC’ gels are precisely tunable and may feature increased branch functionality. We show two examples of such polyMOCs: a gel with a low f based on a M 2 L 4 paddlewheel cluster junction and a compositionally isomeric one of higher f based on a M 12 L 24 cage. The latter features large shear moduli, but also a very large number of elastically inactive loop defects that we subsequently exchanged for functional ligands, with no impact on the gel's shear modulus. Such a ligand substitution is not possible in gels of low f , including the M 2 L 4 -based polyMOC. Gels formed by metal–ligand coordination typically consist of single metal ions linked together by polymer chains. Now, metal–organic cages have been used as junctions instead. A gel was prepared that features a large number of polymer chains at each junction, including loops that further serve to functionalize the material.

Cellulose is the most abundant biopolymer on Earth, found in trees, waste from agricultural crops and other biomass. The fibres that comprise cellulose can be broken down into building blocks, known as fibrillated cellulose, of varying, controllable dimensions that extend to the nanoscale. Fibrillated cellulose is harvested from renewable resources, so its sustainability potential combined with its other functional properties (mechanical, optical, thermal and fluidic, for example) gives this nanomaterial unique technological appeal. Here we explore the use of fibrillated cellulose in the fabrication of materials ranging from composites and macrofibres, to thin films, porous membranes and gels. We discuss research directions for the practical exploitation of these structures and the remaining challenges to overcome before fibrillated cellulose materials can reach their full potential. Finally, we highlight some key issues towards successful manufacturing scale-up of this family of materials. Opportunities for the application of fibrillated cellulose materials—which can be extracted from renewable resources—and broader manufacturing issues of scale-up, sustainability and synergy with the paper-making industry are discussed.

In this study, we report a metallogel developed based on metal-phenolic coordination of natural low-cost polyphenolic molecule and metal ions. Gelation occurs by mixing tannic acid (TA) and group (IV) titanium ions (Ti IV ) to form TA-Ti IV gel. The TA-Ti IV gel exhibits good capability to incorporate diverse metal ions by in situ co-gelation. Herein, five antimicrobial metal ions, i.e. ferric (Fe III ), copper (Cu II ), zinc (Zn II ), cobalt (Co II ) and nickel (Ni II ) ions, were employed to include in TA-Ti IV gels for developing intelligent dressings for infected wounds. The chemical and coordinative structures of TA-Ti IV metallogels were characterized by UV-Vis and Fourier-transform infrared (FT-IR) spectroscopies. Cytotoxicity of antimicrobial metallogels was explored by MTT assay with NIH 3T3 fibroblasts. The release of metal ions was evaluated by inductively coupled plasma mass spectrometry (ICP-MS), indicating the different releasing profiles upon the coordinative interactions of metal ions with TA. The formation and disassembly of metallogels are sensitive to the presence of acid and an oxidizer, H 2 O 2 , which are substances spontaneously generated in infected wounds due to the metabolic activity of bacteria and the intrinsic immune response. The Cu II releasing rates of TA-Ti IV -Cu II metallogels at different pH values of 5.5, 7.4 and 8.5 have been studied. In addition, addition of H 2 O 2 trigger fast release of Cu II as a result of oxidation of galloyl groups in TA. Consequently, the antimicrobial potency of TA-Ti IV -Cu II metallogels can be simultaneously activated while the wounds are infected and healing. The antimicrobial property of metallogels against Gram-negative Escherichia coli , and Gram-positive Methicillin-Resistant Staphylococcus aureus (USA300) and Staphylococcus epidermidis has been investigated by agar diffusion test. In an animal model, the TA-Ti IV -Cu II metallogels were applied as dressings for infected wounds, indicating faster recovery in the wound area and extremely lower amount of bacteria around the wounds, compared to TA-Ti IV gels and gauze. Accordingly, the intelligent nature derived metallogels is a promising and potential materials for medical applications.

Advances in protein therapy are hindered by the poor stability, inadequate pharmacokinetic (PK) profiles, and immunogenicity of many therapeutic proteins. Polyethylene glycol conjugation (PEGylation) is the most successful strategy to date to overcome these shortcomings, and more than 10 PEGylated proteins have been brought to market. However, anti-PEG antibodies induced by treatment raise serious concerns about the future of PEGylated therapeutics. Here, we demonstrate a zwitterionic polymer network encapsulation technology that effectively enhances protein stability and PK while mitigating the immune response. Uricase modified with a comprehensive zwitterionic polycarboxybetaine (PCB) network exhibited exceptional stability and a greatly prolonged circulation half-life. More importantly, the PK behavior was unchanged, and neither anti-uricase nor anti-PCB antibodies were detected after three weekly injections in a rat model. This technology is applicable to a variety of proteins and unlocks the possibility of adopting highly immunogenic proteins for therapeutic or protective applications.