ACS Applied Polymer Materials最新文献

Intrauterine adhesion often leads to complications such as miscarriage and infertility. Owing to the limitations of current mechanical/hormonal interventions, such as risk of retrograde infection and rapid barrier degradation, intrauterine adhesion remains a therapeutic challenge. In this study, a degradable hydrogel film composed of chondroitin sulfate (CS) and chitosan (CHT) was developed. CS has anti-inflammatory functions, while CHT provides antibacterial activity and inhibits cellular fibrosis. The optimized CS/CHT hydrogel, designed to degrade over 7–14 d, exhibited mechanical stability matching the window for endometrial repair. In rat curettage models, the proposed hydrogel significantly reduced endometrial fibrosis, increased endometrial thickness, suppressed pro-inflammatory cytokines (IL-6 and TNF-α), and restored fertility. Its broad-spectrum antibacterial activity further validates its clinical potential. This dual-functional barrier works in synergy with mechanical support and biological activity regulation, providing an innovative solution for intrauterine prevention.

This study presents a pH-responsive hydrogel based on dynamic hydrazone bonds was developed using chitosan, gelatin, and pectin for oral sustained drug delivery. The hydrogel formed rapidly under mild conditions (<5 s for B3 and B5) and showed high water content (∼90%). It degraded slowly in PBS and trypsin but was selectively degradable in pectinase-containing media, adapting to intestinal environments. With BBH as a model drug, all hydrogels achieved >99% encapsulation efficiency (B3: 99.77%; B4: 99.13%). Drug release was well-controlled in gastric fluid (<50% in 2 h for B3) and sustained in colonic fluid (57.93% over 60 h), following Fickian diffusion (Peppas–Sahlin model, R² > 0.98, k₁ ≫ k₂). The hydrogels also exhibited strong antioxidant activity (DPPH scavenging >60%, up to 75% for B2) and low hemolysis ratios, indicating excellent biocompatibility. Overall, the hydrogel demonstrates rapid gelation, high drug loading, pH-responsive sustained release, and biosafety, making it a strong candidate for colon-targeted oral delivery.

Controlling the biodegradation rate is essential for expanding the potential application range of biodegradable polymers. The incorporation of stimuli-responsive bonds (SRBs) in a polymer chain is an effective way to adjust the rate of the initial chain scission process prior to microbial assimilation. Herein, we report a facile modular strategy for controlling the marine biodegradation rate of a highly biodegradable polymer, poly(butylene succinate-co-adipate) (PBSA), by varying the responsiveness of the SRBs without varying their density. Short PBSA chains with boronic acid chain ends were synthesized. Chain extension was achieved by adding various commercially available tetraol linkers, forming boronate esters (BEs), which act as water-sensitive SRBs. The hydrolytic stability of the BE linkage in the polymer could be readily tuned through the choice of the tetraol linker, without the need to change the boronic acid-modified PBSA. While pristine PBSA was brittle and could not be mechanically tested, all the extended polymers displayed improved mechanical properties, with a strain at break of ca. 500% and a stress at break of ca. 20 MPa, regardless of the linker used. Meanwhile, the biodegradation rate in seawater was successfully varied: the biodegradation of unmodified PBSA started rapidly in less than 10 days, whereas the extended polymers showed delayed biodegradation that was directly correlated with the hydrolyzability of the BE. This study will help increasing the range of applications of biodegradable polymers and facilitating synthesis methods, which will benefit plastics of short, yet varying lifetime for applications such as packaging.

The development of sodium-metal batteries (SMBs) is hindered by several limitations associated with conventional organic liquid electrolytes. In this study, we report the synthesis of a novel sodium polyeugenol borate (Na-PEB) salt, which offers low cost and environmental sustainability, synthesized via a cationic polymerization method. Na-PEB was then combined with poly(ethylene glycol) (PEG) 4000 to form the Na-PEB-PEG composite electrolyte. Na-PEB-PEG has perfect thermal stability with an initial decomposition temperature of 376 °C, a satisfactory ionic conductivity of up to 1.5 × 10^–5 S/cm at room temperature, a wide electrochemical window as high as 2.3 V, and a high sodium-ion transference number of >0.96 at 30 °C. It also shows the diffusivity constant in the order of 10^–6 m²/s and ionic mobility in the order of 10^–8 m² v^–1s^–1 at 30 °C. The electrolyte matrix shows a low energy requirement of ionic transport, i.e., 0.266 eV. On behalf of these findings, Na-PEB-PEG-based semisolid polymer electrolyte confirms its potential for application in sodium-ion-based energy storage systems.

In response to the demands of sustainable societal development, the integration of an excellent self-healing capability, adhesive property, recyclability, and desirable mechanical performance is crucial for the application of functional elastomers. In this work, we report a simple construction of a biobased elastomer from carboxylated tung oil polymer and phenolated lignin, which could offer reversible hydrogen bonding networks to achieve outstanding self-healability and dual recyclability. For instance, the biobased elastomer could be recycled rapidly under relatively mild conditions via hot-pressing or solvent-assisted methods, with only a slight decrease observed in its tensile strength. Meanwhile, the abundance of polar groups (especially catechol groups) within the elastomer enables good and reusable adhesion to a variety of substrates. In addition, the adhesion and mechanical properties of the biobased elastomers can be tailored by regulating their building block composition. This work provides an architectural design paradigm for functional elastomers that simultaneously integrate sustainability, self-healing, recyclability, and adhesion, making them suitable for emerging applications like advanced adhesives.

Ionic elastomers are strong candidates to fabricate flexible sensors due to their good electrical properties, flexibility, adhesion, and thermal stability. However, external perturbations significantly affect the signal output of ionic elastomer sensors, and the preparation of ionic elastomer sensors with good damping performance is imminent. Herein, ionic elastomers are prepared from chemical crosslinked perfluorohexylethyl acrylate-isooctyl acrylate-hydroxyethyl acrylate (FEA-EHA-HEA) random copolymers and lithium bis((trifluoromethyl)sulfonyl)azanide (LiTFSI). The coexistence of Li⁺–O and Li⁺–F coordination, and F–F interaction within the ionic elastomer, was evidenced by the solid-state ⁶Li and ¹⁹F NMR spectra. It also indicated that LiTFSI was enriched in FEA-rich microdomains via F–F interaction, and nanoaggregates were formed with effective coordination of Li⁺ and F. Thus, the ionic elastomer with an optimized composition exhibited a good room-temperature damping performance with its loss factor up to 1.44 near 34 °C, high gauge factor (1.84 at 0–150% strain), and high temperature coefficient of resistance (up to −704%·°C^–1 in the range of 0–5 °C). The above characteristics of the ionic elastomer qualify its multimodal sensing in normal and nonconventional states and its potential applications in intelligent response switching, human–machine interface interaction, electronic skin, and so on.

All-in-one hydrogel supercapacitors are promising flexible energy storage devices due to their good flexibility and interfacial stability. However, conventional all-in-one hydrogel supercapacitors (SCs) face fundamental limitations, including complex preparation methods and susceptibility to freezing or drying. Herein, we developed a safe and readily processable approach for fabricating a series of polyacrylamide/sodium carboxymethyl cellulose/polypyrrole (PAM/CMC/PPy) hydrogels tailored for flexible all-in-one SCs. The PAM/CMC/PPy hydrogels demonstrate favorable mechanical elasticity, with a fracture stress of 101 kPa at a strain of 1071%, an exceptional antifreezing point as low as −40.5 °C, and antidrying capability, with 95% water retention after 10 days in open air. Specifically, the optimized PAM/CMC/PPy_2.0 SC achieves a high specific capacitance of 583.3 mF/cm² and a superior energy density of 62.4 μWh/cm² at a power density of 3600 μW/cm². Notably, it retains its structural integrity and electrochemical performance under various deformations. More importantly, its excellent water-retention and antifreezing properties endow the device with remarkable stability across a broad temperature range of −40 to 50 °C, effectively mitigating freezing and drying issues. Furthermore, the SC device boasts an impressive cycle life, with 79% capacitance retention after 3000 cycles at room temperature and 73% retention following 3000 cycles at −20 °C. This study provides a feasible approach for realizing robust, flexible energy storage in harsh operational environments.

A “microaggregation of flame-retardant groups” strategy was utilized to address the inherent flammability of epoxy resin (EP) and the persistent challenge of balancing flame retardant efficiency with mechanical properties in conventional modifications. This approach involved the structural integration of a phosphaphenanthrene derivative ABD with triglycidyl isocyanurate (TGIC) to construct clustered micro-aggregates featuring controllable phosphaphenanthrene density (DE-GAM). The design synergized the regulation of phosphaphenanthrene micro-aggregation with group cooperation. Flame retardancy tests revealed that EP containing only 3 wt % DE-GAM achieved a limiting oxygen index (LOI) of 32.4%, significantly higher than pure EP at 23.7%, and passed the UL-94 V-0 rating with a reduced total burning time of 1.9 s. Furthermore, the EP composite incorporating 3 wt % DE-GAM exhibited a total heat release (THR) of 91.26 kJ/m², which is 19.3% lower than that of the 3 wt % ABD-containing composite. Mechanism studies indicated that the phosphaphenanthrene micro-aggregated structure acted as catalytic centers in the condensed phase, promoting the formation of a dense protective char layer. Simultaneously, it facilitated the targeted release of high-concentration radical scavengers into the gas phase to quench combustion chain reactions. The impact strength of DE-GAM/EP/DDM with 3 wt % loading maintained 81.3% of that of pure EP, implying DE-GAM enhanced interfacial compatibility through the formation of a cross-linked network, effectively alleviating stress concentration and absorbing impact energy.

Poly(potassium acrylate) (PAAK) in high concentration KOH solutions is a promising electrolyte for use in alkaline zinc batteries. Atomistic molecular dynamics simulations are used to investigate the transport mechanisms of hydrogen gas and zincate ions through both KOH solutions and PAAK solutions with comparable concentrations of KOH. Hydrogen molecules do not interact with the ions or the polymer, and simply diffuse through the system. Their diffusion constant decreases with both increasing KOH concentration and when in the polymer, due to the increased viscosity of the solution. By contrast, zincate ions form long-lived clusters with the PAAK chains which significantly slow their diffusion.

Traditionally, hydrophobe-modified, water-soluble cellulose ethers are synthesized in a heterogeneous slurry process using ethylene oxide and long-chain alkyl halides or alkyl glycidyl ethers. In this work, water-soluble cellulose ethers were synthesized homogeneously from glycidyl reagents within a binary ionic liquid system in DMSO. The reaction solvent composition, temperature, and electrophile type were varied to understand the extent of etherification and the solubility of the cellulose ether products. A combination of the ionic liquids 1-ethyl-3-methyl imidazolium acetate (EmimAc) and chloride (EmimCl) resulted in the highest extent of etherification while maintaining an optically clear solution at 8.0 wt % cellulose; the reaction proceeded to completion in 30 min at 100 °C. Additionally, the dual role of weakly basic EmimAc as catalyst and solvent allowed for dissolution and modification of cellulose without the need for additional catalyst or acidic neutralization after the reaction. One-pot synthesis of hydrophobe-modified, water-soluble cellulose ethers exhibited a higher extent of etherification and higher efficiency than previously published heterogeneous reactions conducted with hydrophobic electrophiles of similar length. Rheological measurements of 3.0 wt % aqueous solutions of these cellulose ethers demonstrated a nearly four order-of-magnitude range of solution viscosity from 40 to 15,000 cP. Fully water-soluble cellulose ethers demonstrated an exponential dependence of solution viscosity on the degree of hydrophobe modification, allowing for tunability in a wide array of commercial products. This system demonstrates a versatile method for homogeneously synthesizing water-soluble, hydrophobically modified cellulose ethers in a single step.