Antibacterial polyurethane foams with quaternized-chitosan as a chain extender for nasal packing and hemostasis.

Endoscopic surgery is an effective and common clinical practice for chronic sinusitis. Nasal packing materials are applied in nasal surgery to prevent hemorrhage and promote wound healing. In this study, a degradable polyurethane foam dressing is successfully developed as a promising nasal packing material with good biocompatibility and antibacterial capability. Specifically, quaternized chitosan (QCS) serves as the crosslinker instead of polyols to offer polyurethane foam (PUF-QCS) antibacterial capability. The PUF-QCS2.0 % (with 2.0 wt% QCS) exhibits satisfactory liquid absorption capacity (19.4 g/g), high compressive strengths at both wet (14.5 kPa) and dry states (7.7 kPa), and a good degradation rate (8.3 %) within 7 days. Meanwhile, PUF-QCS2.0 % retains long-term antibacterial activity for 7 days and kills 97.3 % of S. aureus and 91.8 % of E. coli within 6 hours in antibacterial testing. Furthermore, PUF-QCS2.0 % demonstrates a positive hemostatic response in the rabbit nasal septum mucosa trauma model by reducing hemostatic time over 50.0 % and decreasing blood loss up to 76.1 % compared to the commercial PVA nasal packing sponge. Importantly, PUF-QCS also exhibits a significant antibacterial activity in nasal cavity. This nasal packing material has advantages in post-surgery bleeding control and infection prevention. STATEMENT OF SIGNIFICANCE: The performance of a nasal packing sponge requires good mechanical properties, fast and high liquid absorption rate, effective degradability and strong antibacterial activity. These features are helpful for improving the postoperative recovery and patient healing. However, integrating these into a single polyurethane foam is a challenge. In this study, quaternized chitosan (QCS) is synthesized and used as a chain extender and antibacterial agent in preparing a degradable polyurethane foam (PUF-QCS) dressing. PUF-QCS undergoes partial degradation and exhibits effective broad-spectrum antibacterial activity in 7 days. The reduction of postoperative bleeding and infection observed in the animal experiment further demonstrates that the PUF-QCS developed here outperforms the existing commercial nasal packing materials.

Solution-Processed One-Dimensional Photonic Crystals Based on Hollow Silica Exhibiting High Refractive Index Contrast.

Poor interfacial quality and low refractive index contrast (Δn) are critical challenges for the development of high-performance one-dimensional photonic crystals (1DPhCs) via solution methods that impede their optical efficiency. Herein, we introduce an innovative approach by hybridizing hollow SiO2 with poly(vinyl alcohol), referred to as PHS, followed by alternate assembly with TiO2 via spin-coating, achieving a 1DPhC with Δn = 0.76 at the wavelength of 550 nm. This method circumvents the need for high-temperature treatment and complex curing conditions, resulting in a 1DPhC with superior interfacial and optical characteristics. By adjusting the thickness of the PHS layers, we can finely tune the reflectance spectrum, attaining over 99% reflectance at the photonic band gap. Furthermore, 1DPhC demonstrates excellent adhesion to polycarbonate substrates and retains its optimal optical performance even after rigorous environmental testing, including hygrothermal cycles, exposure to hot water, friction, and solvent sonication. This research paves the way for the facile fabrication of high-performance 1DPhCs under mild conditions, offering new perspectives for photonic material processing.

Transparent ultrahigh-molecular-weight polyethylene/MXene films with efficient UV-absorption for thermal management.

The rational use and conversion of energy are the primary means for achieving the goal of carbon neutrality. MXenes can be used for photothermal conversion, but their opaque appearance limits wider applications. Herein, we successfully develop visible-light transparent and UV-absorbing polymer composite film by solution blending the MXene with polyethylene and then vacuum pressing. The resulting film could be quickly heated to 65 °C under 400 mW cm-2 light irradiation and maintained over 85% visible-light transmittance as well as low haze (<12%). The findings of the indoor heat insulation test demonstrate that the temperature of the glass house model covered by this film was 6-7 °C lower than that of the uncovered model, revealing the potential of transparent film in energy-saving applications. In order to mimic the energy-saving condition of the building in various climates, a typical building model with this film as the outer layer of the window was created using the EnergyPlus building energy consumption software. According to predictions, they could reduce yearly refrigeration energy used by 31-61 MJ m-2, and 3%-12% of the total energy used for refrigeration in such structures. This work imply that the film has wide potential for use as transparent devices in energy-related applications.

Eco-friendly bacterial cellulose/MXene aerogel with excellent photothermal and electrothermal conversion capabilities for efficient separation of crude oil/seawater mixture.

Developing novel absorbent materials targeting high-efficiency, low-energy-consumption, and environmental-friendly oil spill cleanup is still a global issue. Porous absorbents endowed with self-heating function are an attractive option because of that they are able to in-situ heat crude oil and dramatically reduce oil viscosity for efficient remediation. Herein, we facilely prepared an eco-friendly multifunctional bacterial cellulose/MXene aerogel (P-SBC/MXene aerogel) for rapid oil recovery. Thanks to excellent full solar spectrum absorption (average absorbance = 96.6 %), efficient photo-thermal conversion, and superior electrical conductivity (electrical resistance = 36 Ω), P-SBC/MXene aerogel exhibited outstanding photothermal and electrothermal capabilities. Its surface temperature could quickly reach 93 °C under 1.0 kW/m2 solar irradiation and 124 °C under 3.0 V voltage respectively, enabling effective heat transfer toward spilled oil. The produced heat significantly decreased crude oil viscosity, allowing P-SBC/MXene aerogel to rapidly absorb oil. By combining solar heating and Joule heating, P-SBC/MXene aerogel connected to a pump-assisted absorption device was capable of achieving all-weather crude oil removal from seawater (crude oil flux = 630 kg m-2 h-1). More notably, P-SBC/MXene aerogel showed splendid outdoor crude oil separation performance. Based on remarkable crude oil/seawater separation ability, the versatile aerogel provides a promising way to deal with large-area oil spills.

Carboxymethyl cellulose and metal-organic frameworks immobilized into polyacrylamide hydrogel for ultrahigh efficient and selective adsorption U(VI) from seawater.

Metal-organic frameworks (MOF)-polymer hybrid hydrogel solves the processable forming of MOF powder and energy consumption of uranium extraction. However, the hybrid hydrogel by conventional synthesis methods inevitably lead to MOF agglomeration, poor filler-polymer interfacial compatibility and slowly adsorption. Herein, we designed that ZIF-67 was implanted into the carboxymethyl cellulose/polyacrylamide (CMC/PAM) by network-repairing strategy. The carboxyl and amino groups on the surface of CMC/PAM drive the uniform growth of ZIF-67 inside the CMC/PAM, which form an array of oriented and penetrating microchannels through coordination bonds. Our strategy eliminate the ZIF-67 agglomeration, increase the interfacial compatibility between MOF and polymer. The method also improve the free and fast diffusion of uranium in CMC/PAM/ZIF-67 hydrogel. According to the experimental, these enhancements synergistically enabled the CMC/PAM/ZIF-67 have a maximum adsorption capacity of 952 mg g-1. The adsorption process of CMC/PAM/ZIF-67 fits well with pseudo-second-order model and Langmuir isotherm. Meanwhile, the CMC/PAM/ZIF-67 maintain a high removal rate (87.3 %) and chemical stability even during ten adsorption-desorption cycles. It is worth noting that the adsorption amount of CMC/PAM/ZIF-67 in real seawater is 9.95 mg g-1 after 20 days, which is an ideal candidate adsorbent for uranium extraction from seawater.

The Isothermal Melting Kinetics of Ultra-High Molecular Weight Polyethylene Crystals.

The isothermal melting behaviors of ultra-high molecular weight polyethylene (UHMWPE) with different entangled states (i.e., nascent and melt-crystallized samples) are studied. For two kinds of UHMWPE samples, the result shows that the relative content of survived crystals (Xs) exponentially decreases with time and reaches a constant value. It is suggested that such a melting behavior is related to the observed nonlinear growth of crystals induced by the kinetically rejected entanglements accumulated at the growth front. Additionally, the exponential decay of Xs with time provides a characteristic melting time (τ) for the melting process. Compared to the melt-crystallized UHMWPE, the τ value of nascent UHMWPE is generally longer even in a higher temperature range, which is mainly because the former has a larger entanglement density difference. Furthermore, these observations demonstrate that UHMWPEs with different entangled states have an analogous melting mechanism since they exhibit a similar melting activation energy (≈1300 kJ mol-1).

Polyethylene fibers containing directional microchannels for passive radiative cooling.

Passive radiative cooling (PRC) that realizes thermal management without consuming any energy has attracted increasing attention. Unfortunately, polymer fibers with radiative cooling function fabricated via a facile, continuous, large-scale and eco-friendly method have been scarcely reported. Herein, polyethylene fibers containing directional microchannels (PFCDM) are facilely fabricated via melt extrusion and water leaching. Interestingly, fabric based on such hydrophobic PFCDM shows high sunlight reflectivity (93.6%), and mid-infrared emissivity (93.9%), endowing it with remarkable PRC performance. Compared with other reported examples, the as-prepared PFDCM fabric has the highest cooling power (i.e., 104.285 W m-2) and temperature drop (i.e., 27.71 °C). Furthermore, decent self-cleaning performance can keep the PFCDM fabric away from contamination and enable it to retain an excellent radiative cooling effect. The method proposed to fabricate PFCDM in this paper will widen the potential application of thermoplastic polyolefins in the field of radiative cooling.

Visualizing the target estimand in comparative effectiveness studies with multiple treatments.

Aim: Comparative effectiveness research using real-world data often involves pairwise propensity score matching to adjust for confounding bias. We show that corresponding treatment effect estimates may have limited external validity, and propose two visualization tools to clarify the target estimand. Materials & methods: We conduct a simulation study to demonstrate, with bivariate ellipses and joy plots, that differences in covariate distributions across treatment groups may affect the external validity of treatment effect estimates. We showcase how these visualization tools can facilitate the interpretation of target estimands in a case study comparing the effectiveness of teriflunomide (TERI), dimethyl fumarate (DMF) and natalizumab (NAT) on manual dexterity in patients with multiple sclerosis. Results: In the simulation study, estimates of the treatment effect greatly differed depending on the target population. For example, when comparing treatment B with C, the estimated treatment effect (and respective standard error) varied from -0.27 (0.03) to -0.37 (0.04) in the type of patients initially receiving treatment B and C, respectively. Visualization of the matched samples revealed that covariate distributions vary for each comparison and cannot be used to target one common treatment effect for the three treatment comparisons. In the case study, the bivariate distribution of age and disease duration varied across the population of patients receiving TERI, DMF or NAT. Although results suggest that DMF and NAT improve manual dexterity at 1 year compared with TERI, the effectiveness of DMF versus NAT differs depending on which target estimand is used. Conclusion: Visualization tools may help to clarify the target population in comparative effectiveness studies and resolve ambiguity about the interpretation of estimated treatment effects.

Precision medicine analysis of heterogeneity in individual-level treatment response to amyloid beta removal in early Alzheimer's disease.

INTRODUCTION: Alzheimer's disease (AD) is a neurological disorder with variability in pathology and clinical progression. AD patients may differ in individual-level benefit from amyloid beta removal therapy. METHODS: Random forest models were applied to the EMERGE trial to create an individual-level treatment response (ITR) score which represents individual-level benefit of high-dose aducanumab relative to the placebo. This ITR score was used to test the existence of heterogeneity in treatment effect (HTE). RESULTS: We found statistical evidence of HTE in the Clinical Dementia Rating-Sum of Boxes (CDR-SB;P =  0.034). The observed CDR-SB benefit was 0.79 points greater in the group with the top 25% of ITR score compared to the remaining 75% (P = 0.020). Of note, the highest treatment responders had lower hippocampal volume, higher plasma phosphorylated tau 181 and a shorter duration of clinical AD at baseline. DISCUSSION: This ITR analysis provides a proof of concept for precision medicine in future AD research and drug development. HIGHLIGHTS: Emerging trials have shown a population-level benefit from amyloid beta (Aß) removal in slowing cognitive decline in early Alzheimer's disease (AD). This work demonstrates significant heterogeneity of individual-level treatment effect of aducanumab in early AD. The greatest clinical responders to Aß removal therapy have a pattern of more severe neurodegenerative process.

Regulating microstructures of aerogels by controlling phase separation mechanism for improving specific surface area and energy harvesting.

Aerogels with 3D porous structures have been attracting increasing attention among functional materials due to their advantages of being lightweight and high specific surface area. Precise control of the porous structure of aerogel is essential to improve its performance. In this work, polylactic acid (PLA) aerogels with distinctly different microstructures were fabricated by precisely controlling the phase separation behavior of the ternary solution system. Rheological and theoretical analyses have revealed that the interactions between polymer molecules, solvents and non-solvents play a crucial role in determining the nucleation and growth of poor olymer and rich polymer phases. By adjusting the non-solvent type and the solution composition, aerogels with spider network structure, bead-like connected microsphere structure, and cluster petal structure were obtained. Ideal spinodal phase separation conditions were obtained to produce aerogels with a homogeneous fiber network structure. The optimum PLA aerogel achieved an extremely porosity of 96 % and a high specific surface area of 114 m2/g, which rendered it with excellent triboelectric generation performance. Thus, this work provides fundamental insights into the precise regulation of the phase separation behavior and the structure of the aerogel, which can help boost the performance and expand the applications of PLA aerogels.

Ag Nanoparticles-Coated Shish-Kebab Superstructure Film for Wearable Heater.

Passive and active wearable heaters have received widespread attention due to their efficient utilization of solar energy and all-weather heating capabilities, but the current challenges are their preparation processes being time-consuming and equipment expensive. Herein, a simple and facilitated preparation method for the multifunctional wearable heater was developed, which springs Ag nanoparticles on the shish-kebab superstructure film via deposited melanin-like polydopamine as the adhesive. The light absorption ability of the resultant wearable heater in the visible region can be significantly enhanced by the addition of polydopamine, realizing a highly efficient photothermal conversion ability. Accordingly, it can achieve rapid warming ability whether passive heating (up to 45 °C about 60 s at 100 mW/cm2) or active heating (up to 72 °C about 40 s at 0.6 V), compared to ordinary cotton fabric. In addition, it can realize a 6.3 °C temperature difference with Cotton, showing excellent heat preservation ability. This study demonstrates a simple and low-cost approach for the prepared shish-kebab superstructure-based wearable heaters.

Rapid ultra-sensitive nucleic acid detection using plasmonic fiber-optic spectral combs and gold nanoparticle-tagged targets.

Nucleic acid (NA) is a widely-used biomarker for viruses. Accurate quantification of NA can provide a reliable basis for point-of-care diagnosis and treatment. Here, we propose a tilted fiber Bragg grating (TFBG)-based plasmonic fiber-optic spectral comb for fast response and ultralow limit NA detection. The TFBG is coated with a gold film which enables excitation of surface plasmon resonance (SPR), and single-stranded probe NAs with known base sequences are assembled on the gold film. To enhance sensitivity of refractive index (RI) for sensing a chosen combination of probe and target NAs around the TFBG surface, gold nanoparticles (AuNPs) are bonded to the target NA molecules as "RI-labels". The NA combination-induced aggregation of AuNPs induces significant spectral responses in the TFBG that would be below the detection threshold for the NAs in the absence of the AuNPs. The proposed TFBG-SPR NA sensor shows a fast response time of 30 s and an ultra-wide NA detection range from 1 × 10-18 mol/L to 1 × 10-7 mol/L. In the NA concentration range of 1 × 10-12 mol/L (1 pM) to 105 pM, an ultra-high sensitivity of 1.534 dB/lg(pM) is obtained. The sensor achieves an ultra-low limit of detection down to 1.0 × 10-18 mol/L (1 aM), which is more than an order of magnitude lower than the previous reports. The proposed sensor not only shows potentials in practical applications of NA detection, but also provides a new way for TFBG-SPR biochemical sensors to achieve higher RI sensitivity.

In-situ monitoring of refractive index change during water-ice phase transition with a multiresonant fiber grating.

In-situ monitoring of refractive index changes during a liquid-solid phase transition is achieved by measurement of the transmission spectrum from a single tilted fiber Bragg grating immersed in water. Differential wavelength shifts of multiple mode resonances are used to eliminate cross-talk from temperature, throughout the phase transition, and from strains occurring after solidification. The measured sudden shift of refractive index at the phase transition is shown to be consistent with the expected difference from water to ice, in spite of the observed onset of compressive strain on the fiber by the frozen water. Beyond the obvious application to research on the dynamics of liquid-solid phase transitions, this work demonstrates the multiparameter measurement capabilities of multiresonant gratings.

Controllable-morphology polymer blend photonic metafoam for radiative cooling.

Incorporating radiative cooling photonic structures into the cooling systems of buildings presents a novel strategy to mitigate global warming and boost global carbon neutrality. Photonic structures with excellent solar reflection and thermal emission can be obtained by a rational combination of different materials. The current preparation strategies of radiative cooling materials are dominated by doping inorganic micro-nano particles into polymers, which usually possess insufficient solar reflectance. Here, a porous polymer metafoam was prepared with polycarbonate (PC) and polydimethylsiloxane (PDMS) using a simple thermally induced phase separation method. The metafoam exhibits strong solar reflectivity (97%), superior thermal emissivity (91%), and low thermal conductivity (46 mW m-1 K-1) due to the controllable morphology of the randomly dispersed light-scattering air voids. Cooling tests demonstrate that the metafoam could reduce the average temperature by 5.2 °C and 10.2 °C during the daytime and nighttime, respectively. In addition, the simulation of a cooling energy system of buildings indicates that the metafoam can save 3.2-26.7 MJ m-2 per year in different cities, which is an energy-saving percentage of 14.7-41%. The excellent comprehensive performances, including the passive cooling property, thermal insulation and self-cleaning of the metafoam makes it appropriate for practical outdoor applications, exhibiting its great potential as an energy-saving building cooling material.

Mushroom-mimetic 3D hierarchical architecture-based e-skin with high sensitivity and a wide sensing range for intelligent perception.

Electronic skin (e-skin) is one of the most important components of future wearable electronic devices, whose sensing performances can be improved by constructing micropatterns on its sensitive layer. However, in traditional e-skins it is difficult to balance sensitivity and the pressure sensing range, and most micropatterns are generally prepared by some complex technologies. Herein, mushroom-mimetic micropatterns with 3D hierarchical architecture and an interdigital electrode are facilely prepared. The micropatterned sensitive layer is further developed through spraying carbon nanotube (CNT) dispersion on the thermoplastic polyurethane (TPU) film with mushroom-mimetic micropatterns (denoted as MMTC). Thanks to the "interlocking effect" between mushroom-mimetic micropatterns and the interdigital electrode in the as-prepared MMTC/interdigital electrode e-skin, the e-skin exhibits a high sensitivity (up to 600 kPa-1), a wide pressure sensing range (up to 150 kPa), a short response time (<20 ms) and excellent durability (15 000 cycles). The MMTC/interdigital electrode e-skin is capable of precisely monitoring health conditions via the as-acquired physiological parameters in real time. Moreover, such e-skins can be used to monitor gestures wirelessly, sense the trajectory of pressure stimuli and recognize Morse code under water. This study provides a cost-efficient, facile strategy to design e-skin for future-oriented wearable intelligent systems.

Phase morphology, rheological behavior and mechanical properties of supertough biobased poly(lactic acid) reactive ternary blends.

Poly(lactic acid) (PLA) is one of the most promising bio-based polyester with great potential to replace for the petroleum-based polymers, which can significantly reduce greenhouse gas emissions. However, the inherent brittleness of PLA seriously restricts its broad applications. Herein, PLA/poly(ε-caprolactone) (PCL)/ethylene methyl acrylate-glycidyl methacrylate (EMA-GMA) ternary blends with different phase structures were prepared through reactive blending. The reactions between the epoxy groups of EMA-GMA and the carboxyl and hydroxyl end groups of PLA and PCL and were evidenced from the Fourier transform infrared spectroscopy, dynamic mechanical analysis and rheological results. The atomic force microscopy (AFM) images clearly revealed the formation of stack structure of the PCL and EMA-GMA minor phases in PLA/PCL/EMA-GMA (80/15/5) blend, and core-shell particle structures in PLA/PCL/EMA-GMA (80/10/10) and (80/5/15) blends. In terms of elongation at break and impact toughness, PLA/PCL/EMA-GMA (80/5/15) blend presents the best properties among all the compositions. Moreover, it also behaved excellent stiffness-toughness balance. The toughening mechanism can be ascribed to the formation of core-shell structure and the existence of interfacial adhesion in the ternary blends. This work can provide guide for the preparation and design of PLA-based partially renewable supertough materials that can compete with conventional petro-derived plastics.

Development and Validation of the DOAC Score: A Novel Bleeding Risk Prediction Tool for Patients With Atrial Fibrillation on Direct-Acting Oral Anticoagulants.

BACKGROUND: Current clinical decision tools for assessing bleeding risk in individuals with atrial fibrillation (AF) have limited performance and were developed for individuals treated with warfarin. This study develops and validates a clinical risk score to personalize estimates of bleeding risk for individuals with atrial fibrillation taking direct-acting oral anticoagulants (DOACs). METHODS: Among individuals taking dabigatran 150 mg twice per day from 44 countries and 951 centers in this secondary analysis of the RE-LY trial (Randomized Evaluation of Long-Term Anticoagulation Therapy), a risk score was developed to determine the comparative risk for bleeding on the basis of covariates derived in a Cox proportional hazards model. The risk prediction model was internally validated with bootstrapping. The model was then further developed in the GARFIELD-AF registry (Global Anticoagulant Registry in the Field-Atrial Fibrillation), with individuals taking dabigatran, edoxaban, rivaroxaban, and apixaban. To determine generalizability in external cohorts and among individuals on different DOACs, the risk prediction model was validated in the COMBINE-AF (A Collaboration Between Multiple Institutions to Better Investigate Non-Vitamin K Antagonist Oral Anticoagulant Use in Atrial Fibrillation) pooled clinical trial cohort and the Quebec Régie de l'Assurance Maladie du Québec and Med-Echo Administrative Databases (RAMQ) administrative database. The primary outcome was major bleeding. The risk score, termed the DOAC Score, was compared with the HAS-BLED score. RESULTS: Of the 5684 patients in RE-LY, 386 (6.8%) experienced a major bleeding event, within a median follow-up of 1.74 years. The prediction model had an optimism-corrected C statistic of 0.73 after internal validation with bootstrapping and was well-calibrated based on visual inspection of calibration plots (goodness-of-fit P=0.57). The DOAC Score assigned points for age, creatinine clearance/glomerular filtration rate, underweight status, stroke/transient ischemic attack/embolism history, diabetes, hypertension, antiplatelet use, nonsteroidal anti-inflammatory use, liver disease, and bleeding history, with each additional point scored associated with a 48.7% (95% CI, 38.9%-59.3%; P<0.001) increase in major bleeding in RE-LY. The score had superior performance to the HAS-BLED score in RE-LY (C statistic, 0.73 versus 0.60; P for difference <0.001) and among 12 296 individuals in GARFIELD-AF (C statistic, 0.71 versus 0.66; P for difference = 0.025). The DOAC Score had stronger predictive performance than the HAS-BLED score in both validation cohorts, including 25 586 individuals in COMBINE-AF (C statistic, 0.67 versus 0.63; P for difference <0.001) and 11 945 individuals in RAMQ (C statistic, 0.65 versus 0.58; P for difference <0.001). CONCLUSIONS: In individuals with atrial fibrillation potentially eligible for DOAC therapy, the DOAC Score can help stratify patients on the basis of expected bleeding risk.

A Multifunctional Asymmetric Fabric for Sustained Electricity Generation from Multiple Sources and Simultaneous Solar Steam Generation.

Harvesting electrical energy from water and moisture has emerged as a novel ecofriendly energy conversion technology. Herein, a multifunctional asymmetric polyaniline/carbon nanotubes/poly(vinyl alcohol) (APCP) that can produce electric energy from both saline water and moisture and generate fresh water simultaneously is developed. The constructed APCP possesses a negatively charged porous structure that allows continuous generation of protons and ion diffusion through the material, and a hydrophilicity-hydrophobic interface which results in a constant potential difference and sustainable output. A single APCP can maintain stable output for over 130 h and preserve a high voltage of 0.61 V, current of 81 µA, and power density of 82.4 µW cm-3 with 0.15 cm3 unit size in the water-induced electricity generation process. When harvesting moisture energy, the APCP creates dry-wet asymmetries and triggers the spontaneous development of electrical double layer with a current density of 1.25 mA cm-3 , sufficient to power small electronics. A device consisting of four APCP can generate stable electricity of 3.35 V and produce clean water with an evaporation rate of 2.06 kg m-2  h-1 simultaneously. This work provides insights into the fabrication of multifunctional fabrics for multisource energy harvesting and simultaneous solar steam generation.