ACS Applied Polymer Materials最新文献

Commercialhemoperfusion adsorbents for hyperbilirubinemia aremainly polystyrene (PS) anion exchange resins due to their high mechanicalstrength, satisfactory physicochemical stability, and low cost, enablingbilirubin removal via electrostatic interactions. However, these resinspose two major issues in clinical use: heparin binding and coagulationactivation. In this work, we developed moderately hydrophilic gigaporouspolystyrene (mHGPS) microspheres with a surface that balances hemocompatibilityand hydrophobic bilirubin adsorption, and then immobilized ZIF-8 insitu to obtain mHGPS@ZIF-8 composite microspheres for synergy-enhancedselective bilirubin adsorption. The composite microspheres were featuredwith through-connected gigapores (∼1.05 μm), high porosity(64.02%), high permeability (7.31 × 10^–11 m²) and satisfactory hemocompatibility with a hemolysis rateof 1.67%. Compared to mHGPS microspheres, the mHGPS@ZIF-8 compositemicrospheres exhibited a 2.6-fold increase in the adsorption capacityfor bilirubin (from 53.1 mg/g to 138.9 mg/g). Notably, an even greater3.1-fold enhancement was achieved for albumin-bound bilirubin (from18.7 mg/g to 57.8 mg/g). Moreover, benefiting from the gigaporousstructure of mHGPS microspheres, mHGPS@ZIF-8 composite microspheresexhibited rapid bilirubin removal kinetics, removing 89.0% of bilirubinwithin 60 min during simulated hemoperfusion, with minimal albuminloss (1.2%). This work establishes a strategy for designing high-performancebilirubin adsorbents with significant potential for treating hyperbilirubinemia.

Conductive polymer hydrogels that integrate mechanicalrobustness,self-healing, adhesion, ionic conductivity, and long-term stabilityare highly desirable for flexible electronics. Herein, a machine learning(ML)-guided strategy was developed to design multifunctional polyacrylamide/chitosandual-network hydrogels incorporating 1-ethyl-3-methylimidazolium tetrafluoroborate([EMIM][BF₄]) and sorbitol. An exploratory ML screeningof 31 literature-derived additives prioritized imidazolium-based ionicliquids (ILs) as promising candidates within the investigated chemicalspace. The optimized hydrogel exhibited a tensile stress of 0.16 MPa,an elongation at break of 688.6%, a tensile-strength recovery of 92.7%after 30 min, an ionic conductivity of 3.2 S m^–1, and a broad-range gauge factor (GF) of 4.277. In situ characterizations,component-removal experiments, density functional theory (DFT) calculations,and molecular dynamics (MD) simulations provided complementary evidencethat hydrogen bonding, Al³⁺-mediated coordination, electrostaticinteractions, and interfacial interactions collectively contributeto the polymer network and ion-transport behavior. The hydrogel enabledreliable human motion monitoring, handwriting recognition, human-machineinteraction (HMI), and flexible supercapacitors with 85% capacitanceretention after 10,000 cycles. This work provides a data-driven polymer-networkdesign strategy for multifunctional conductive hydrogels toward flexibleelectronic applications.

Utilizingagro-industrial wastes/byproducts as feedstocks for functionalpolymers offers a promising approach to alleviating urgent resourceshortages. Herein, elemental sulfur (an oil-refining byproduct) andrenewable diisocyanide/diamine (agrowate derivatives) were employedas monomers to synthesize renewable polythioureas via a sustainablemulticomponent polymerization (MCP) strategy, and the absorption abilityof polythioureas toward mercury ions (Hg²⁺) was thoroughlystudied. The diamine/diisocyanide monomer was prepared from the platformcompound furfurylamine through a consecutive reaction. The effectsof solvent and polymerization time on the molecular weight and yieldof the polythioureas were systematically investigated, and ultrasonicirradiation was applied to accelerate the MCP rates. The thermal propertiesof polythioureas were investigated by using thermogravimetric analysisand differential scanning calorimetry. Cross-linked polythioureaswere prepared through either the direct MCP or the postpolymerizationmodification strategy. The Hg²⁺ removal performances ofthe resulting polythioureas, including absorption kinetics, thermodynamics,mechanism, and reusability, were also studied. The polythioureas showedrapid Hg²⁺ absorption ability (nearly quantitative removalwithin 40 min) and over 99% selectivity for Hg²⁺ in electroplatingwastewater which containing complex metal ions.

Perovskite solarcells (PSCs) hold strong potential forefficientand cost-effective photovoltaic technology, yet their device performanceand stability remain hindered by interfacial limitations. In particular,the hole transport material (HTM) that contacts both the perovskiteand the front contact can often be a bottleneck for device efficiencyand durability. To overcome these challenges, we design and synthesizea series of carbazole- and fluorene-based polymers via palladium-catalyzedBuchwald–Hartwig amination, incorporating tunable N,N-dimethyl aminopropyl (N) and butanoate (COOCH₃) side chains. We systematically investigate how these polarside chains affect the electronic properties of the buried perovskiteinterface and the overall device performance. Our results show thatboth N and COOCH₃-functionalized HTMs significantly enhanceinterfacial compatibility with wide-bandgap perovskites, facilitatingsuperior perovskite film formation and more efficient charge extraction.This enhancement yields wide-bandgap PSCs with a champion power conversionefficiency (PCE) of ∼17%, comparable to devices using commercialpoly-triarylamine (PTAA) HTMs. These findings highlight that targetedside-chain engineering offers a simple and effective strategy to optimizepolymer HTMs for wide-bandgap PSCs, providing valuable insights forthe future design of perovskite optoelectronic devices.

Introducingdynamic covalent networks into conventionalethylene-propylene-dienemonomer (EPDM) rubber offers a promising strategy for developing thermallyreprocessable elastomers; however, it requires the introduction ofreactive functionalities onto the chemically inert hydrocarbon backbone.Herein, ketone-functionalized EPDM (K-EPDM) was prepared through aone-pot strategy combining epoxidation and oxidative cleavage of thedouble bonds in EPDM. Then, K-EPDM was cross-linked with biobasedamines to construct imine-cross-linked elastomers. Exchangeable iminelinkages served as the primary reversible cross-linking motifs, whereasa small fraction of irreversible epoxy-amine cross-links derived fromresidual epoxy groups provided additional constraints for improvingdimensional stability. The resulting elastomers exhibited tunablemechanical properties, good elastic recovery, thermally activatedstress relaxation, reduced creep deformation, thermally induced shapeadaptability, and high retention of mechanical performance after repeatedthermal reprocessing. Hence, this work provides a simple and promisingstrategy to synthesize ketone-functionalized rubber, which can befurther cross-linked with biobased amines to obtain dynamically cross-linkedEPDM elastomers with thermal reprocessability and improved creep resistance.

Polymer gel performance and stability under high-temperature,high-salinityconditions critically constrain their practical applications. Whilegels have been successfully formulated at temperatures exceeding 100°C and brine salinities above 4 × 10⁴ mg·L^–1, the quantitative influence of temperature and brinesalinity on gelation behavior remains poorly understood; consequently,evidence-based guidelines for polymer and cross-linker selection arelacking. This study used hydroquinone (HQ) and hexamethylenetetramine(HMTA) as cross-linkers and AM–AMPS polymers (AM: acrylamide;AMPS: 2-acrylamido-2-methylpropanesulfonic acid) with 25%, 47%, and69% AMPS content as gelling agents (abbreviated as AMPS25, AMPS50,and AMPS70, respectively). Gelation behavior was tested at 110 and130 °C and in brines with salinities of 4.15 × 10⁴ mg·L ^–1 and 2.5 × 10⁵ mg·L^–1. The effects of temperature, brinesalinity, polymer structure, and cross-linker dosage were analyzed.Results show that gel performance in brine is more sensitive to temperaturethan to brine salinity. AMPS25 forms stable gels at 110 °C underboth low- and high-salinity conditions; AMPS50 demonstrates superiorgelation performance compared to AMPS70 at 130 °C in brine witha salinity of 4.15 × 10⁴ mg·L^–1. This is because strong electrostatic repulsion between the polymerand cross-linker impedes the cross-linking reaction, resulting inunsatisfactory gel formation for the lower-concentration AMPS70 underthese conditions. Under conditions of 130 °C and a brine salinityof 2.5 × 10⁵ mg·L^–1, the gelstrength formed by AMPS70 was marginally lower than that of AMPS50,yet its gelation time was longer and thermal stability was enhanced.The study concludes that increasing cross-linker dosage or using higher-AMPS-contentpolymers helps control carboxylate ion formation during thermal treatmentof polymer gels, a key approach to developing temperature- and salt-resistantgels.

The rapid advancement of wearable electronics necessitatesthedevelopment of flexible, durable, and environmentally stable energyand sensing materials. However, conventional hydrogels often sufferfrom poor mechanical robustness, rapid dehydration, and freezing atsubzero temperatures, severely limiting their practical applications.In this work, we fabricate highly stretchable and antifreezing PVA/PAM/NaCl(PPN) organohydrogels by integrating a double-network structure withNaCl doping and glycerol treatment. The resulting PPN organohydrogelsexhibit exceptional stretchability (2320%), high ionic conductivity(5.5 S/m), and remarkable long-term environmental stability (only12% mass loss after 30 days). Furthermore, it maintains excellentmechanical and electrical performance at −20 °C, effectivelysuppressing ice formation. We demonstrate its versatility by utilizingthe PPN organohydrogel in two key applications: (1) as a strain sensorwith an ultrahigh gauge factor (GF = 26.608) for monitoring humanmotion, including subtle pulse signals; (2) as the electrode in atriboelectric nanogenerator (VMO-TENG), achieving a maximum powerdensity of 0.5 W/m². Moreover, by integrating the sensorwith a genetic algorithm-optimized backpropagation neural network(GABP), we realize a high-accuracy gesture recognition system. Thisstudy provides a facile strategy for developing robust flexible electronicssuitable for extreme environments and intelligent human–machineinteraction.

Flexiblecapacitive pressure sensors have attracted considerableattention for wearable electronics, intelligent robotics, and human-machineinterfaces, yet achieving high sensitivity, broad pressure detection,and long-term stability remains challenging. Herein, carbon nanotubes(CNTs)-pinned porous polydimethylsiloxane (PDMS) foam composite dielectricsare developed via a facile one-step emulsion-templating strategy.The CNTs are preferentially distributed along the PDMS skeleton andpore walls, forming a CNTs-pinned architecture that is expected toreduce filler rearrangement during repeated deformation. Benefitingfrom the synergistic low-modulus and high-dielectric effect, the sensorachieves a pressure range of 0–450 kPa with sensitivities of68.9 × 10^–3 kPa^–1, 18.9 ×10^–3 kPa^–1, and 8.7 × 10^–3 kPa^–1 in the low-, medium-, andhigh-pressure regions, respectively. It also exhibits a 31.3-foldenhancement in sensitivity over pristine PDMS, with a detection limitof 8.8 Pa, response/recovery times of 87/92 ms, and robust stabilityover 10,000 cycles. Furthermore, when integrated into a soft roboticgripper, three sensors achieve 99.4% accuracy in fruit-type classificationand 99.7% accuracy in tomato storage-stage classification. This workprovides a scalable strategy for engineering stable porous compositedielectrics and demonstrates the potential of tactile sensing forintelligent fruit monitoring and robotic manipulation.

Small-molecule donor/polymer acceptor (SD/PA) organicsolar cells(OSCs) are attractive for their morphological stability, yet theirefficiencies still lag behind those of mainstream systems. One keydifficulty is that the acceptor must aggregate strongly enough toform ordered electron-transport domains while remaining miscible enoughwith the crystalline donor to avoid oversized phase separation. Here,we address this issue by randomly copolymerizing two Y-series acceptorunits bearing alkoxy and alkyl side chains, which affords four PAs,namely PY-O, PY-22, PY-13, and PY-C. Varying the copolymer compositiontunes optoelectronic properties, aggregation strength, and miscibilitywith the SD BTR-Cl. Among the four acceptors, PY-13 combines relativelystrong and ordered molecular packing with the best compatibility withBTR-Cl, leading to finer nanoscale phase separation and reduced chargerecombination. The BTR-Cl:PY-13 device delivers a power conversionefficiency of 10.39% with an open-circuit voltage of 0.99 V. Theseresults indicate that random copolymerization is an effective approachto balancing PA aggregation with donor–acceptor compatibilityin SD/PA OSCs.

Giventhat daily used electronic devices like mobile phones andtablets are frequently exposed to complex environments possibly involvingpathogens and contaminants, posing a potential risk of disease transmission,the development of antifouling and antibacterial coatings tailoredto the hygiene requirements of these devices is of significant importance.Herein, disulfide-containing cationic polydimethylsiloxane (PDMS)-modifiedpolyurethanes (C_xSi_yPUs) were designed via integrating low-surface-energy PDMSsegments, quaternary ammonium antibacterial units, and labile disulfidebonds for post-cross-linking. Waterborne C_xSi_yPU (WC_xSi_yPU) emulsions were prepared via self-emulsification,yielding C_xSi_yPU nanoparticles with spherical morphology, controllable particlesize, and positively charged surfaces. Leveraging the latent natureof disulfide bonds, a latent isocyanate post-cross-linker was directlyintroduced into the WC_xSi_yPU emulsion to form a one-component emulsion, whichenhanced storage stability and facilitated subsequent application.During thermal curing, disulfide bonds underwent homolytic cleavageand captured hydrogen atoms to generate thiol groups, which furtherreacted with released isocyanate groups to form thiocarbamate cross-links,realizing post-cross-linking via a double latent reaction strategy.The C_xSi_yPUcoatings displayed an ultrasmooth, amorphous, hydrophobic surfacewith enriched PDMS moieties, possessing low surface energy, superiorresistance to bacterial attachment, excellent optical transparency,and room-temperature hydrophobic recovery ability. Furthermore, theoptimal coating delivered favorable cyclic antibacterial durabilityunder repeated water immersion, high surface hardness, good mechanicalabrasion and peeling resistance, and robust substrate adhesion, verifyingits possible long-term service performance in daily use scenarios.The C_xSi_yPUcoatings integrated excellent antipollution with preserved opticaltransparency and interactive performance, making them highly promisingfor transparent, hygienic, protective applications for consumer electronicsto minimize the risk of disease transmission.