ACS Applied Polymer Materials最新文献

Membrane separation technology has garnered significant attention in the oil/water separation field due to its energy-efficient operation and superior separation performance. Nevertheless, the persistent membrane fouling during operation and the widespread use of chemically stable and nondegradable polymer substrates are two critical challenges for membrane separation technology. Therefore, developing an environmentally friendly oil/water separation membrane with self-cleaning properties and degradable characteristics has become a hot spot in current research. In this study, d-CA/PVP/ZnO nanofiber membranes with self-cleaning properties are successfully prepared by introducing photocatalytic ZnO nanoparticles into biodegradable cellulose acetate (CA) and polyvinylpyrrolidone (PVP) matrices using electrostatic spinning technology. The composite membrane exhibits excellent separation performance in treating surfactant-stabilized O/W emulsion with the flux of 16,711 L·m^–2·h^–1·bar^–1 while maintaining a high separation efficiency of 99%. More importantly, the membrane material has excellent photocatalytic properties, and the flux can be restored to 95% of the initial value by UV light irradiation. By combining high separation efficiency, self-cleaning ability, and degradable properties, this membrane material provides a solution for the green and sustainable treatment of oily wastewater.

The practical deployment of aqueous zinc-based energy storage devices is severely hampered by uncontrollable dendrite growth and parasitic reactions at the zinc anode interface. To address these challenges, this work proposes sulfobutyl ether-β-cyclodextrin (SBE-β-CD) as a multifunctional additive for high-performance quasi-solid-state zinc-ion hybrid capacitors (ZHCs). The SBE-β-CD molecule concurrently manipulates the hydrogen-bond network and ion transport properties within the hydrogel electrolyte. Its zincophilic sulfonate motifs establish efficient ion-conduction pathways, endowing the electrolyte with high ionic conductivity and an elevated Zn²⁺ transference number. Simultaneously, the additive restructures the inherent hydrogen-bonding network, effectively suppressing water activity and associated side reactions. Furthermore, it regulates interfacial ion behaviors and guides preferentially oriented zinc deposition along the (002) crystallographic plane, thereby inhibiting dendrite formation and promoting a uniform plating morphology. As a result, the optimized electrolyte enables a Zn||Cu cell to achieve an exceptional average Coulombic efficiency of 99.5% over 800 cycles and a Zn||Zn symmetric cell to maintain stable operation for over 820 h. The assembled ZHC demonstrates remarkable cycling durability with 85.4% capacity retention after 21,700 cycles, alongside feasibility for powering electronics. This molecular engineering strategy offers a versatile and promising pathway for developing flexible and safe zinc-based energy storage systems.

The development of high-performance photoinitiators (PIs) capable of operating under visible light, exhibiting high water solubility and possessing macromolecular characteristics, remains a significant challenge in advancing sustainable photopolymerization technologies. Although recent research strategies focusing on visible-light activation, water solubility, or macromolecular design have achieved notable progress, they have only partially overcome the limitations associated with these properties. A visible-light-responsive, water-soluble, macromolecular photoinitiator (DIDP-mPEG) was developed based on an indole–chalcone core. DIDP-mPEG was synthesized via UV-induced grafting of poly(ethylene glycol) monomethyl ether (mPEG) chains onto a dual-photoresponsive precursor. The resulting initiator exhibited excellent water solubility (up to 5 wt %) and a high molar extinction coefficient at 465 nm. It efficiently initiated the aqueous polymerization of acrylamide, achieving >80% conversion within 360 s, and enabled the digital light processing 3D printing of hydrogels. The initiation mechanism, investigated through nuclear magnetic resonance (NMR) spectroscopy, photolysis, theoretical calculations, and kinetics, is proposed to involve hydrogen abstraction from the PEG chains by the excited chalcone carbonyl. Compared to benchmark macromolecular PIs, such as PEG-BAPO, DIDP-mPEG exhibits an enhanced molar extinction coefficient and superior initiating efficiency, representing a significant advancement toward the design of green, efficient photoinitiating systems for advanced aqueous photopolymerization applications.

Nonisocyanate polyurethane (NIPU) foams provide a sustainable alternative to conventional isocyanate-based systems but remain limited by low mechanical strength and thermal conductivity. Here, Ti₃C₂T_x MXene nanosheets were incorporated into self-blown hybrid NIPU foams synthesized from epoxy–cyclic carbonate precursors via amine-induced polymerization with in situ CO₂ foaming. Systematic variation of MXene loading (1–7 wt %) revealed strong correlations between nanosheet dispersion, cellular morphology, and multifunctional performance. The MXene fillers refined the foam microstructure, by reducing pore size and thickening cell walls, while simultaneously enhancing polymer chain mobility restriction and interfacial heat transport. These effects yielded substantial increases in glass transition temperature, storage modulus, thermal stability, and thermal conductivity. The results demonstrate that MXene nanosheets act as both reinforcing and structural-modifying agents, enabling sustainable polymer foams with tunable thermomechanical and heat-transfer properties. The developed MXene–NIPU foams combine sustainability with high performance, making them suitable for thermal insulation, packaging, and electronic applications.

Long-term physiological electrical signal monitoring requires wearable epidermal electrodes to have excellent skin-conforming ability and environmental stability. Herein, a multifunctional eutectic gel with environmental tolerance, surface adhesion, and self-healing performance was successfully synthesized by copolymerizing N-hydroxyethyl acrylamide (HEAA) and acrylic acid (AA) in a eutectic solvent composed of ethylene glycol (EG) and betaine (Bet) and introducing a small amount of Fe³⁺ simultaneously. Due to the strong hydrogen bonds between the eutectic solvent and the polymer network and the fact that Fe³⁺ can complex with PAA chains and Bet, a high-density hydrogen-bond and coordination-bond cross-linked network can be formed, endowing the eutectic gel with high mechanical properties (144.48 kPa, 1011%) and excellent self-healing properties. In addition, there is a significant number of carboxyl, hydroxyl, and amide groups on the polymer chain, and a significant number of hydrogen-bond donors and acceptors in the network, which enable the eutectic gel to form noncovalent bonds with various surfaces, thereby effectively improving the adhesion ability (123.41 kPa). Based on good adhesion and stretchability, the eutectic gel electrode can form conformal contact and deform with the skin, showing a low interfacial impedance (≈25 kΩ), and can dynamically monitor various physiological electrical signals, exhibiting high sensitivity and long-term stability. It should be noted that even after continuous operation for 10 h, the eutectic gel electrode still exhibits excellent signal stability, and the signal-to-noise ratio (18.87 dB) of the collected physiological signals shows almost no attenuation.

Polylactide (PLA) is a promising biosourced alternative to conventional fossil-fuel-derived plastics, but its widespread adoption is limited by its brittleness and slow degradation rate in most environments. We recently demonstrated that a poly(ethylene oxide)-block-poly(butylene oxide) diblock polymer (PEO–PBO) significantly toughens PLA at 5 wt % loading, a benefit which remains unchanged after 9 months of aging despite oxidative degradation of PEO–PBO to oligomers. In this work, we demonstrate that PLA degradation in aged PEO–PBO/PLA blends submerged in seawater at 50 °C is nearly twice as fast as that in neat PLA under similar conditions. The molar mass of neat PLA exhibits a relatively slow decrease for the first 35 days of degradation under these conditions, at which point the PLA glass transition temperature (T_g) falls below 50 °C, and the rate of molar mass change accelerates. In aged PEO–PBO/PLA under the same conditions, the moderately elevated temperature results in the collapse of the macrophase-separated PEO–PBO domains and migration of the oligomeric polyether oxidative degradation products into the PLA matrix, which depresses the PLA T_g to below 50 °C in less than 1 day. As a result, aged PEO–PBO/PLA immediately exhibits a rate of molar mass change consistent with that observed in the late stages of neat PLA degradation, effectively bypassing the 35 days of relatively slow change. These results suggest that heat-triggered plasticization can expand the range of practical conditions for PLA degradation, potentially including home compost conditions, and demonstrate a design strategy for additives that both toughen PLA and accelerate its degradation.

Poly(p-phenylene benzobisoxazole) (PBO) fibers exhibit poor hydrophilicity, which necessitates the use of highly corrosive acids as solvents during papermaking. This severely restricts the research and development of PBO paper. To address this limitation, the present study proposes an innovative and environmentally benign strategy for fabricating high-performance PBO paper using water as the solvent. In this strategy, nanofibers with excellent hydrophilicity are employed as stabilizers, which adsorb onto the surface of PBO fibers through π–π stacking interactions, thereby significantly improving the aqueous dispersibility of PBO fibers. Furthermore, the interlacing and interconnection of nanofibers effectively enhance the interfacial interactions between PBO fibers, leading to a substantial improvement in the overall performance of PBO paper. Compared with the pristine PBO paper, the modified one exhibits a 23-fold increase in tensile strength and a 1.6-fold increase in electrical breakdown strength, while retaining its inherent flexibility, thermal resistance, dielectric properties, and processability. This work holds great significance for promoting the large-scale production of PBO paper and expanding its applications in fields requiring high thermal resistance, wave transmission capability, and electrical insulation performance.

Passive daytime radiative cooling (PDRC) materials face the pervasive challenge of overcooling at night, which increases heating energy consumption, particularly in climates with high diurnal temperature variation. Here, we demonstrate an ion-track polycarbonate (PC) membrane radiative cooling system with Janus mid-infrared optical properties (J-ITMRC) that achieves all-day passive bilateral thermal management without external energy input. The membrane comprises a PC layer with randomly distributed high-aspect-ratio air columns engineered by multidirectional ion-irradiation and chemical etching on the front side and a thin metallic reflective coating on the back side. This asymmetric structure exhibits distinctive Janus mid-infrared optical properties, with high solar reflectance (R⃖_solar = 95.7%) and MIR emissivity (ε⃖_rad = 96.6%) of the front side for daytime cooling, and high MIR reflectivity (R⃖_rad = 95.4%) of the back side to minimize nocturnal heat loss. Outdoor experiments showed that the J-ITMRC provides a temperature reduction of up to 7.6 °C below ambient during the day, whereas its cavity temperature is up to 2.0 °C above ambient during the night. Building energy simulations across 34 Chinese cities revealed an average 20% reduction in the total HVAC energy consumption. This work highlights the potential of microstructure-engineered polymer membranes based on ion-track technology as high-performance passive materials for intelligent thermal management in energy-saving buildings.

Polymer dielectric materials find extensive application in electrical and electronic systems. However, the energy storage performance of polymer dielectrics sharply decreased above 150 °C, which did not meet the demands of modern capacitor applications. In this paper, a fluorine-containing polyimide (FPI) with a mechanically interlocked structure is synthesized, where β-cyclodextrins are threaded along the axles of FPI chains to generate a self-cross-linking supramolecular polymer network. Based on the mechanically interlocked structure, both the conjugation effect between polymer chains and the phonon-assisted interchain charge transport are weakened, leading to improved breakdown strength and capacitive performance at high temperatures. As a result, the all-organic dielectric films obtained a discharge energy density (U_d) of 8.24 J/cm³ with an efficiency (η) > 90% at 25 °C and 750 MV/m. Besides, the dielectric films exhibit excellent high-temperature capacitive performance; the upper U_ds of the film are 5.03 J/cm³ and 3.02 J/cm³ at 150 and 200 °C (η > 80%), respectively. The obtained result presents an innovative tactic for the synthesis of high-performance all-organic polymer dielectrics that meet the current requirements of extreme environments.

Highly economical and environmentally friendly synthesis of a wide range of hydrophobic and hydrophilic poly(meth)acrylates with a low dispersity of D̵ < 1.3 and an initiation efficiency close to 100% by means of atom transfer radical polymerization (ATRP) is reported. This was possible thanks to the use of 2-propanol, which creates a versatile reaction medium that allows polymerization of monomers showing different hydrophilicities. The developed procedures of polymerization, utilizing metallic copper, ascorbic acid, or tertiary amine groups of monomers in the role of reducing agents, were furthermore applied in synthesis of triblock copolymers (TBC) grafted from the polydimethylsiloxane (PDMS) bifunctional, linear macroinitiator. This way, a series of amphiphilic macromolecules with various PDMS contents, including functional, pH-sensitive, and thermosensitive copolymers, were synthesized and characterized using proton and carbon-13 nuclear magnetic resonance (¹H NMR, ¹³C NMR) and attenuated total reflectance infrared (ATR-IR) spectroscopies. The presence of the flexible PDMS core and hydroxyl groups in the outer blocks further enabled the preparation of copolymers with a complex structure of bottlebrushes with spherical topology, which were visualized using atom force microscopy (AFM). Biocompatibility of the obtained PDMS-based materials was evaluated with lactate dehydrogenase (LDH) cytotoxicity assay toward human dermal fibroblasts (HDF) and retinal pigment epithelium cells (RPE), which demonstrated over 85% cell viability after 7 days of incubation.