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Structural changes induced by thermal denaturation and renaturation of a double-helical polysaccharide xanthan in acidic and basic solutions were investigated mainly by light scattering measurements and circular dichroism spectroscopy. In acidic solution, the renatured components were almost the same as those in native components, while small amounts of aggregates and a hairpin structure were produced via denaturation and renaturation processes. In basic solution, the double helices were dissociated upon heating into the single coils, and high molar mass sample produced a hairpin structure after subsequent renaturation.
The modification of cellulose nanocrystal film using alkyl silane and silane containing tertiary amino groups was performed in a suspension state. Control of the surface structure and functionalization by silane compounds was conducted in the two-stage process. Wettability change property of the silylation-modified CNC triggered by CO2 was demonstrated.
We examined the adsorption behavior of poly(tert-butyl methacrylate) (PtBMA) and poly(ethyl methacrylate) (PEMA), on a silica surface. Time-evolution of the degree of adsorption γ(t) was evaluated with chip nanocalorimetry. γ(t) revealed a two-step profile for both polymers. At the second stage of adsorption, the slope of γ(t) vs. log t increased as adsorption proceeded; this trend has not been reported for other polymers so far. In addition, atomic force microscopy images of the adsorbed layers revealed corresponding evolutions of the morphologies.
The study on the improvement of the crystallinity of cellulose II by post-treatment with dilute NaOH solution showed that the crystallinity was significantly improved by post-treatment with multiple cycles. The NaOH in an aqueous NaOH solution penetrated only inaccessible surface regions, and cellulose rearrangement occurred only in these regions during post-treatment, improving crystal size. In the second and subsequent posttreatment cycles, cellulose rearrangement occurred only at the inaccessible surfaces expanded during the previous post-treatment cycle, crystallization progressed toward amorphous regions away from the initial crystalline regions.
The fluorophore-modified glucan, TPE-6BG3 adopts an extended, random-coiled form in DMSO, which does not fluoresce. The morphology of the TPE-6BG3 chemosensor changes drastically to a dynamic globule in aqueous media. The dynamic, “induced-fit” globule selectively and sensitively recognizes the medicinally-useful tetrasaccharide, acarbose via glucan-saccharide coaggregation.
Free-standing films of trifluoropropyl-substituted open-cage silsesquioxane-pendant polysiloxane by optimizing sol-gel reaction condition of tris(dimethoxysilyl-ethyl-dimethylsiloxy)-heptatrifluoropropyl-substituted open-cage silsesquioxane. Elastic modulus and the decomposition temperature for 5% weight loss under N2 of the product by polycondensation at 180 °C were significantly higher than that by polycondensation at 50 °C. Significant changes in the UV-vis spectra of the resulting transparent films were hardly observed even after 13 days of UV irradiation.
In this short review, we focus on the development of CO2 separation materials consisting of hydrogel particles. The review starts with development of stimuli responsive micro- and nano-gel particles that reversibly absorb CO2 isn response. The next chapter focuses on the development of temperature-responsive hydrogel films consisting of gel particles that reversibly absorb CO2 and the importance of optimizing the pKa values of the amines in the particles. In the end, assembly of defect-free nano-meter-thick CO2 separation membranes consisting of the amine containing hydrogel particles are introduced.
To develop a novel gel catalyst system for a selective reaction, we prepared a variety of gels with homogeneously dispersed crosslinked domain (CD) structures containing iridium complexes with various crosslinking densities. The designed CD gel catalyst catalyzed the N-alkylation of aniline with benzyl alcohol, and the steric effect of the CD structure allowed the selective formation of the secondary amine product by controlling the access of the substrate to the iridium complex.
Photooxidation and fragmentation behaviors of itPP were studied. Photooxidation likely occurred in the amorphous regions of itPP due to the higher oxygen diffusion. Surface deterioration was observed on the UV-exposed itPP films. Pressed films exhibited much denser cracks compared to uniaxially oriented itPP films. Notably, cracks in the uniaxially oriented itPP films were formed along the direction of orientation and decreased with increasing draw ratio. The crystalline structure and oriented molecular chains notably inhibited the photooxidative degradation and fragmentation of the itPP films.
Steam decomposition of poly(lactic acid) (PLA) and poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBH) enhanced the recovery of chemical feedstock compared with simple pyrolysis. Steam enhanced the hydrolysis of PLA and resulted in the formation of short-chain compounds with hydroxyl end groups, and subsequent pyrolysis of them improved lactide recovery. Monomer production from PHBH was also enhanced by simultaneous hydrolysis and pyrolysis under steam decomposition.
Achieving a wearable artificial kidney hinges on overcoming the critical challenge of developing efficient urea adsorption materials for dialysate regeneration. An acidic hollow polystyrene nanoparticle was synthesized by modified emulsion polymerization, DMF etching and sulfuric acid treatment sequentially. The nanoparticles had a urea absorption capacity of up to 1 mmol/g after two hours of adsorption in a 30 mM urea aqueous solution at 37 °C. Additionally, the adsorption capacity dramatically increased with increasing urea concentration, while sharply decreased with increasing ionic strength.
We developed a novel method for synthesizing degradable polymers based on 1,5-shift radical isomerization polymerizations of vinyl ethers with transferable atoms or groups and in-between acid-cleavable ether linkages in the side chains. In particular, vinyl ethers with side chains composed of thiocyano and p-methoxybenzyl ether groups underwent radical isomerization polymerizations via 1,5-shifts, in which a vinyl ether radical abstracted the cyano group intramolecularly to generate a thiyl radical and result in a polymer with a p-methoxybenzyl ether linkage in the main chain.
We report the syntheses of novel marine biodegradable poly(ethylene succinate) (PES)- and poly(butylene succinate) (PBS)-based copolymers containing different dicarboxylic acid (DCA) units with various carbon numbers and different feed ratios. Specifically, the copolymers with longer-chain DCA units, even at low contents, exhibited marine biodegradability. The thermomechanical properties also varied with the DCA contents. These results indicated that the thermomechanical properties and the marine biodegradability of the PES- and PBS-based copolymers were regulated by controlling their structures and DCA contents.
Hydrogels have attracted considerable attention in the biomedical applications because of their high functionalities, biocompatibility and biodegradability. This study on the novel hyaluronic acid (HA) nanogel-based hydrogel comprising HA modified with cholesterol derivatives and maleimide crosslinking groups. Depending on the degree of cholesterol derivative substitution, the properties such as water uptake, gelation behavior and protein encapsulation was investigated. The results suggested that the hydrogels enhanced peptide and protein trapping abilities have potential as a new hyaluronan hydrogel for biomedical applications.
Photochemically adaptable polymer materials are widely used in the fields of medicine, electronics, and engineering due to their precise and remote processability. Diverse designs of light-responsive units have been developed to fabricate various photocontrollable materials with low-energy, rapid, and reversible photoreactivity. Recently, multiple stimuli-responsive materials have been demonstrated to further control their photoreactivity by combining light with another stimulus, leading to advanced photocontrollable capabilities. This Focus Review summarizes the recent progress in developing photochemically adaptable polymer network materials by designing photoresponsive units, focusing on the chemical structures of cleavable moieties.
Photoinduced transitions between the solid, glass, and liquid states based on molecular photoswitches promise an enormous variety of applications, such as photoswitchable adhesives, which contribute to material recycling for a sustainable future in the era of composite materials. In this review, we highlight recent progress in the photoinduced transitions of small molecules and polymers and systematically discuss the molecular designs, mechanisms, applications, merits and demerits, and future challenges in each photoswitch and the whole field.
Overview of the reusable dismantlable adhesion interface system. Heating induces a cleavage reaction of the anthracene photodimer in the molecular layer at the adhesion interface, and the anthracene monomer remains on the substrate surface of the peeled specimen. Photoirradiation to the cleaved molecular layer induces the photodimerization of anthracenes, and the materials exhibit strong adhesion at the adhesion interface.
Fabrication of LCD cell without alignment layer on substrates was achieved via simply adding the chiral polymer nanoparticles into CLC mixtures. The fabricated chiral nanoparticle (CNP) doped CLC cell shows a high contrast 97.4% and a fast response time 7.6 ms.
Aliphatic polycarbonates with ether side groups linked by amide bonds exhibit high hydrolyzability and antiplatelet properties due to enhanced hydration resulting from strong interactions with amide and ether side groups.
Mechanochemistry is a promising technology to tackle current and future polymer waste streams for a sustainable future. With this review, we take into account synthetic, computational, technical, and engineering perspectives to converge trituration and polymer mechanochemistry with a particular focus on the fate of commodity polymers and potential technologies to monitor mechanochemical reactions while they occur. We highlight the need for future transdisciplinary research to tackle the high-leverage parameters governing an eventually successful mechanochemical polymer degradation approach for a circular economy.
