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1.
  • Ait Benhamou, Anass, et al. (författare)
  • Strong and Flame-Resistant Nanocellulose Sheets Derived from Agrowastes via a Papermaking-Assisted Process
  • 2024
  • Ingår i: acs applied polymer materials. - 2637-6105. ; 6:5, s. 2763-2776
  • Tidskriftsartikel (refereegranskat)abstract
    • In recent decades, the production of nanocellulose has gained significant attention. Nanocellulose-based film materials have found widespread applications in various high-end sectors owing to their remarkable characteristics. Nevertheless, the limitation of certain functional properties, such as resistance to water and fire, has posed challenges to their broader utilization. In this study, we conducted a comparative investigation on the impact of two distinct chemical modifications, namely, TEMPO-mediated oxidation and phosphorylation, on the production of nanocellulose sheets via a papermaking-assisted process. This approach explores the synergistic effects of these modifications in enhancing the properties of cellulose nanofibers for nanopaper production. To achieve this, we proposed utilizing Henna stems as an alternative source of cellulosic material, aiming to harness untapped agricultural residues as a sustainable alternative to conventional sources such as wood and cotton. The phosphorylated Henna nanopaper exhibited substantial enhancements in terms of mechanical properties, wettability, fire resistance, and water vapor permeability when compared to the TEMPO-modified Henna nanopaper. In conclusion, our findings underscore the potential of Henna stems as an environmentally sustainable source of cellulose for nanofiber production, positioning it as a promising alternative to wood and other lignocellulosic sources for advanced applications.
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2.
  • Belaineh, Dagmawi, et al. (författare)
  • Controlling the Organization of PEDOT:PSS on Cellulose Structures
  • 2019
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : AMER CHEMICAL SOC. - 2637-6105. ; 1:9, s. 2342-2351
  • Tidskriftsartikel (refereegranskat)abstract
    • Composites of biopolymers and conducting polymers are emerging as promising candidates for a green technological future and are actively being explored in various applications, such as in energy storage, bioelectronics, and thermoelectrics. While the device characteristics of these composites have been actively investigated, there is limited knowledge concerning the fundamental intracomponent interactions and the modes of molecular structuring. Here, by use of cellulose and poly(3,4-ethylene-dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), it is shown that the chemical and structural makeup of the surfaces of the composite components are critical factors that determine the materials organization at relevant dimensions. AFM, TEM, and GIVVAXS measurements show that when mixed with cellulose nanofibrils, PEDOT:PSS organizes into continuous nanosized beadlike structures with an average diameter of 13 nm on the nanofibrils. In contrast, when PEDOT:PSS is blended with molecular cellulose, a phase-segregated conducting network morphology is reached, with a distinctly relatively lower electric conductivity. These results provide insight into the mechanisms of PEDOT:PSS crystallization and may have significant implications for the design of conducting biopolymer composites for a vast array of applications.
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3.
  • Bergfelt, Andreas, et al. (författare)
  • A Mechanical Robust yet highly Conductive Diblock Copolymer-based Solid Polymer Electrolyte for Room Temperature Structural Battery Applications
  • 2020
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 2:2, s. 939-948
  • Tidskriftsartikel (refereegranskat)abstract
    • In this paper we present a solid polymer electrolyte (SPE) that uniquely combines ionic conductivity and mechanical robustness. This is achieved with a diblock copolymer poly(benzyl methacrylate)-poly(ε-caprolactone-r-trimethylene carbonate). The SPE with 16.7 wt% lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) showed the highest ionic conductivity (9.1×10−6 S cm−1 at 30 °C) and apparent transference number (T+) of 0.64 ± 0.04. Due to the employment of the benzyl methacrylate hard-block, this SPE is mechanically robust with a storage modulus (E') of 0.2 GPa below 40 °C, similar to polystyrene, thus making it a suitable material also for load-bearing constructions. The cell Li|SPE|LiFePO4 is able to cycle reliably at 30 °C for over 300 cycles. The promising mechanical properties, desired for compatibility with Li-metal, together with the fact that BCT is a highly reliable electrolyte material makes this SPE an excellent candidate for next-generation all-solid-state batteries.
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4.
  • Björn, Linnea, 1994, et al. (författare)
  • Process-Induced Structures of Injection-Molded High-Density Polyethylene─Combining X-ray Scattering and Finite Element Modeling
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - 2637-6105. ; 6:8, s. 4852-4864
  • Tidskriftsartikel (refereegranskat)abstract
    • The success of plastics heavily relies on fast melt processing methods used for large-scale industrial manufacturing, including injection molding. The hierarchical structure of the solid polymer depends on material selection combined with processing conditions, making mechanical properties of the injection molded part difficult to predict. Here we show how scanning small- and wide-angle X-ray scattering, birefringence microscopy, and polarized light optical microscopy can be combined with injection molding simulations to shed light on the correlation between the polymer morphology of high-density polyethylene and processing conditions. The scattering data revealed that the complex layered structure highly depends on the pressure during the holding phase of injection molding. Furthermore, we identified specific work of flow as a main parameter to capture the changes in morphology induced by varying the process settings. Overall, a good agreement was found between experimental data and the computational simulations, suggesting that computational simulations can be further used to predict the multiphase morphology of injection molded parts.
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5.
  • Björn, Linnea, 1994, et al. (författare)
  • Scanning Small-Angle X-ray Scattering of Injection-Molded Polymers: Anisotropic Structure and Mechanical Properties of Low-Density Polyethylene
  • 2023
  • Ingår i: ACS Applied Polymer Materials. - 2637-6105. ; 5:8, s. 6429-6440
  • Tidskriftsartikel (refereegranskat)abstract
    • Injection molding is known to create a layered anisotropicmorphologyacross the sample thickness due to varying shear and cooling ratesduring the manufacturing process. In this study, scanning small-angleX-ray scattering was used to visualize and quantify the distributionof hierarchical structures present in injection-molded parts of low-densitypolyethylene (LDPE) with varying viscosities. By combining scatteringdata with results from injection molding simulations and tensile testing,we find that oriented shish-kebab structures, as well as elongatedspherulite structures consisting of semicrystalline ellipsoids, contributeto high ultimate tensile strength along the flow direction. Furthermore,we show that a higher degree of orientation is found close to theinjection gate and in LDPE with higher viscosity, consequently fromelevated shear and cooling rates present during the injection moldingprocess.
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6.
  • Boventi, Matteo, et al. (författare)
  • Porosity of Molecularly Imprinted Polymers Investigated by 129Xe NMR Spectroscopy
  • 2022
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 4:12, s. 8740-8749
  • Tidskriftsartikel (refereegranskat)abstract
    • Molecularly imprinted polymers (MIPs) display intriguing recognition properties and can be used as sensor recognition elements or in separation. In this work, we investigated the formation of hierarchical porosity of compositionally varied MIPs using 129Xe Nuclear Magnetic Resonance (NMR) and 1H Time Domain Nuclear Magnetic Resonance (TD-NMR). Variable temperature 129Xe NMR established the morphological variation with respect to the degree of cross-linking, supported by 1H TDNMR determination of polymer chain mobility. Together, the results indicate that a high degree of cross-linking stabilizes the porous structure: highly cross-linked samples display a significant amount of accessible mesopores that instead collapse in less structured polymers. No significant differences can be detected due to the presence of templated pores in molecularly imprinted polymers: in the dry state, these specific shapes are too small to accommodate xenon atoms, which, instead, probe higher levels in the porous structure, allowing their study in detail. Additional resonances at a high chemical shift are detected in the 129Xe NMR spectra. Even though their chemical shifts are compatible with xenon dissolved in bulk polymers, variable temperature experiments rule out this possibility. The combination of 129Xe and TDNMR data allows attribution of these resonances to softer superficial regions probed by xenon in the NMR time scale. This can contribute to the understanding of the surface dynamics of polymers.
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7.
  • Börjesson, Mikaela, 1987, et al. (författare)
  • Thermoplastic and flexible films from arabinoxylan
  • 2019
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 1:6, s. 1443-1450
  • Tidskriftsartikel (refereegranskat)abstract
    • Current interest in replacing fossil-fuel-derivedpolymers and materials in favor of renewable materials is high.An inherent difficulty with the use of biomass-derivedpolysaccharides and hemicelluloses in this context, however,is their stiffness and lack offlowability at temperatures relevantfor thermal processing, which severely limits their capacity forthermal processing. Here, we present a modification thatenables a heat-processable arabinoxylan (AX). The modifica-tion involves a ring-opening oxidation to a dialdehyde withsubsequent reduction of the aldehydes to alcohol, to increasethe number of OH groups, followed by an etherification withhydrophobic alkyl chains. The modified AX was successfullycompression molded with heat intofilmswhich becomethermoplastic in behavior and highlyflexibleandflows at temperatures above 130°C. Thefilms are stretchable up to 200%,and their strength and strain deformation are controlled by the degree of oxidation and substitution of the AX polymer. Thesefindings are highly encouraging and open up the potential use of modified AX alone or as a composite in applications thatincludefilms, food packaging, and barriers via hot-melt processing techniques.
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8.
  • Fall, Andreas, et al. (författare)
  • Spinning of Stiff and Conductive Filaments from Cellulose Nanofibrils and PEDOT:PSS Nanocomplexes
  • 2022
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 4:6, s. 4119-4130
  • Tidskriftsartikel (refereegranskat)abstract
    • Research in smart textiles is growing due to the increased demand from the healthcare sector and people's urge to keep track of and analyze the signals and metrics from their bodies. Electrically conductive filaments are the most fundamental material for smart textiles. These filaments can be imbued with functionalities and useful in fields like energy storage, sensing, and actuation. To be able to meet the requirements that the latter applications require, fabrication techniques must be developed to provide better processability and sustainability in a cost-effective manner. Here, a mixture of a conductive polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), and biobased cellulose nanofibrils (CNFs) was used to spin filaments utilizing a water-based process. These filaments show electrical conductivities up to 150 S/cm and tensile stiffness of 20 GPa. Interestingly, the PEDOT aligned to a similar degree as the CNFs during the spinning process without a drawing step, which is hypothesized to be caused by the attachment of PEDOT on the CNFs. Lastly, the filaments were tested in an organic electrochemical transistor (OECT) configuration, which resulted in a working device with an on/off ratio approaching 1500. Furthermore, the OECT exhibited stable behavior when changing temperature (20-80 °C) and relative humidity (40-80%). This aqueous spinning method, resulting in filaments with robust electronic properties in different temperature and humidity environments, show greats promise for future innovative smart textiles. 
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9.
  • Gammino, Michele, et al. (författare)
  • Chemical-free Reactive Melt Processing of Biosourced Poly(butylene-succinate-adipate) for Improved Mechanical Properties and Recyclability
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - 2637-6105. ; 6:10, s. 5866-5877
  • Tidskriftsartikel (refereegranskat)abstract
    • Biosourced and biodegradable polyesters like poly(butylene succinate-co-butylene adipate) (PBSA) are gaining traction as promising alternatives to oil-based thermoplastics for single-use applications. However, the mechanical and rheological properties of PBSA are affected by its thermomechanical sensitivity during its melt processing, also hindering PBSA mechanical recycling. Traditional reactive melt processing (RP) methods use chemical additives to counteract these drawbacks, compromising sustainability. This study proposes a green reactive method during melt compounding for PBSA based on a comprehensive understanding of its thermomechanical degradative behavior. Under the hypothesis that controlled degradative paths during melt processing can promote branching/recombination reactions without the addition of chemical additives, we aim to enhance PBSA rheological and mechanical performance. An in-depth investigation of the in-line rheological behavior of PBSA was conducted using an internal batch mixer, exploring parameters such as temperature, screw rotation speed, and residence time. Their influence on PBSA chain scissions, branching/recombination, and cross-linking reactions were evaluated to identify optimal conditions for effective RP. Results demonstrate that specific processing conditions, for example, twelve minutes processing time, 200 °C temperature, and 60 rpm screw rotation speed, promote the formation of the long chain branched structure in PBSA. These structural changes resulted in a notable enhancement of the reacted PBSA rheological and mechanical properties, exhibiting a 23% increase in elastic modulus, a 50% increase in yield strength, and an 80% increase in tensile strength. The RP strategy also improved PBSA mechanical recycling, thus making it a potential replacement for low-density polyethylene (LDPE). Ultimately, this study showcases how finely controlling the thermomechanical degradation during reactive melt processing can improve the material’s properties, enabling reliable mechanical recycling, which can serve as a green approach for other biodegradable polymers.
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10.
  • Georgouvelas, Dimitrios, et al. (författare)
  • Residual Lignin and Zwitterionic Polymer Grafts on Cellulose Nanocrystals for Antifouling and Antibacterial Applications
  • 2020
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 2:8, s. 3060-3071
  • Tidskriftsartikel (refereegranskat)abstract
    • Hybrid materials from nanocellulose, lignin, and surface- grafted zwitterionic poly(sulfobetaine methacrylate) (PSBMA) chains are prepared to attain antifouling bio-based nanomaterials with enhanced antibacterial performance. The grafting of PSBMA from both cellulose and lignocellulose nanocrystals (CNC and LCNC, respectively) is attempted; however, the materials' analysis with FTIR, XPS, and solid-state C-13 NMR reveals that the grafting on LCNC is negligible. Antifouling and antibacterial performances of CNC and LCNC, as well as PSBMA-grafted CNC, are evaluated by using quartz crystal microbalance with dissipation monitoring, confocal microscopy, and the agar diffusion method using bovine serum albumin and E. coli ACTT 8937 as protein model and bacterial model, respectively. The results demonstrate that the grafting of CNC with PSBMA improves the antifouling and antibacterial activity of the material compared to pristine CNC and LCNC.
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11.
  • Hu, Y. J., et al. (författare)
  • Effect of Chain Lengths on the Antibiofilm and Hemolytic Activities of Main-Chain Alternating Polysulfoniums
  • 2022
  • Ingår i: Acs Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 4:7, s. 4868-4875
  • Tidskriftsartikel (refereegranskat)abstract
    • Unlike antibiotics with accurate chemical structures, polydisperse chain lengths of synthetic polycations usually result in undesirable variations of antibacterial performance, which obstructs their wide applications in many areas. Herein, we propose that mainchain sulfonium-based polymers with alternating sequences may be used as a potential solution to tackle this issue. Through the thiol- epoxy "click" step-growth polymerization and methylation, alternating polysulfoniums can be facilely prepared with polydispersity around 1.5 and a molecular weight ranging from 6000 to 50 000 g/mol. Within this tested range, constant minimum bactericidal concentration (MBC) values against a broad spectrum of clinically relevant bacteria and stable hemocompatibility are observed for polysulfoniums with different chemical compositions. Moreover, the representative polysulfonium can steadily inhibit the biofilm formation (similar to 75- 90%) at 1.25-5 mu g/mL and achieve 97-99.9% reduction of bacteria at 10-40 mu g/mL in the 3 day mature biofilms. We hypothesize that the amphiphilicity of main-chain polysulfoniums displays less susceptibility to the dispersed polymer chains, probably because of their accurate alternating sequence and the location of all functional groups in the polymer main chain. The unique structural nature of the main-chain sulfonium-based alternating polymers can make them serve as a reliable platform for antibacterial applications in the field of synthetic polycations.
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12.
  • Ingverud, Tobias, et al. (författare)
  • Helux : A Heterofunctional Hyperbranched Poly(amido amine) Carboxylate
  • 2019
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : AMER CHEMICAL SOC. - 2637-6105. ; 1:7, s. 1845-1853
  • Tidskriftsartikel (refereegranskat)abstract
    • Herein we present the first scientific report on the commercially available Helux 33/16 - a heterofunctional poly(amido amine carboxylate) hyperbranched polymer (Native Helux). The Native Helux, built from diethyl maleate (DEM) and diaminohexane (HMDA), was characterized, in part aided by reverse engineering of a similar scaffold with the same monomers. Different purification methods resulted in higher molecular weight polymers ranging from 8.4 to 51.7 kDa (M-w), and the Helux considered the purest, having 10 mmol (primary and secondary amines)/g as well as 2-4 mmol carboxylic/g Helux. Additionally, aqueous-mediated postmodifications of Helux were achieved including Michael addition, guanylation, and ring-opening of sultone, as well as water/ethyl acetate-mediated amidation of imidazole-activated pentenoic acid. The inherent heterofunctionality of Helux, amines and carboxylic groups, was further explored by a one-component self-cross-linking approach that yielded a dendritic poly(amido amine) network with autofluorescence-exhibiting properties and a T-g of 59 degrees C. The Helux network exhibited a storage modulus (G') of 7.9 MPa at 25 degrees C and in dry state, and 0.9 MPa (G') when plasticized by 50 wt % swelling (in water) of the network. Finally, dendritic hydrogels based on Helux were produced by a spontaneous NHS-amidation reaction with difunctional 10kPEG-NHS. The mechanical properties of the hydrogels were found to be dependent on the curing temperature for the hydrogel, yielding a G' of 8 and 14.5 kPa, a stress at break of 11.5 and 22.7 kPa, and a strain-at-break of 161 and 163%, at 25 and 37 degrees C, respectively.
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13.
  • Jafari, Mohammad Javad, et al. (författare)
  • Force-Induced Structural Changes in Spider Silk Fibers Introduced by ATR-FTIR Spectroscopy
  • 2023
  • Ingår i: ACS applied polymer materials. - : American Chemical Society. - 2637-6105. ; 5:11, s. 9433-9444
  • Tidskriftsartikel (refereegranskat)abstract
    • Silk fibers have unique mechanical properties, and many studies of silk aim at understanding how these properties are related to secondary structure content, which often is determined by infrared spectroscopy. We report significant method-induced irreversible structural changes to both natural and synthetic spider silk fibers, derived from the widely used attenuated total reflection Fourier-transform infrared (ATR-FTIR) technique. By varying the force used to bring fibers into contact with the internal reflection elements of ATR-FTIR accessories, we observed correlated and largely irreversible changes in the secondary structure, with shape relaxation under pressure occurring within minutes. Fitting of spectral components shows that these changes agree with transformations from the alpha-helix to the beta-sheet secondary structure with possible contributions from other secondary structure elements. We further confirm the findings with IR microspectroscopy, where similar differences were seen between the pressed and unaffected regions of spider silk fibers. Our findings show that ATR-FTIR spectroscopy requires care in its use and in the interpretation of the results.
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14.
  • Jawerth, Marcus, et al. (författare)
  • Mechanical and Morphological Properties of Lignin-Based Thermosets
  • 2020
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : AMER CHEMICAL SOC. - 2637-6105. ; 2:2, s. 668-676
  • Tidskriftsartikel (refereegranskat)abstract
    • The need for renewable alternatives for fossil-based aromatic material constituents is evident for a more sustainable society. Lignin is the largest source of naturally occurring aromatic compounds but has mainly been considered as waste material or energy source in the pulp and paper industry. Developments in extracting lignin from these processes provide a large source for renewable aromatic structures to be used in various applications. Producing thermosets out of lignin is a very promising route to utilize this raw material toward, for example, composite application. The buildup of the molecular network based on oligomeric lignin segments will be different from traditional thermoset analogues, where the constituents often are smaller molecules, and will have an effect on the material properties. In this work LignoBoost Kraft lignin is refined, chemically modified, and used to produce freestanding thermosets with different architectures and properties. These different thermosets are evaluated, and the possibilities to tailor the material properties through work-up and modification are demonstrated. Morphological studies on the formed thermosets using X-ray scattering show systematic differences in molecular stacking and aggregate sizes.
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15.
  • Jugé, Agnès, et al. (författare)
  • Porous Thermoformed Protein Bioblends as Degradable Absorbent Alternatives in Sanitary Materials
  • 2023
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 5:9, s. 6976-6989
  • Tidskriftsartikel (refereegranskat)abstract
    • Protein-based porous absorbent structures can be processed and assembled into configurations suitable for single-use, biodegradable sanitary materials. In this work, a formulation based on a mixture of proteins available as industrial coproducts is processed into continuous porous structures using extrusion and assembled using conventional thermal methods. The experimental design led to formulations solely based on zein-gluten protein bioblends that could be manufactured as liquid absorbent pellets, compressed pads, and/or porous films. The processing versatility is attributed to the synergistic effect of zein as a low viscosity thermoformable protein with gluten as a readily cross-linkable high molecular weight protein. The capillary-driven sorption, the biodegradability of the materials, and the possibility to assemble the products as multilayer components provide excellent performance indicators for their use as microplastic-free absorbents. This work shows the potential of biopolymers for manufacturing sustainable alternatives to current nonbiodegradable and highly polluting disposable items such as pads and diapers.
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16.
  • Karim, Z., et al. (författare)
  • Microscopic Hybrid Membranes Made of Cellulose-Based Materials Tuned for Removing Metal Ions from Industrial Effluents
  • 2021
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society. - 2637-6105. ; 3:8, s. 3733-3746
  • Tidskriftsartikel (refereegranskat)abstract
    • Most of the polymeric membranes used today in water decentralization are synthesized through complicated and expensive processes, contain unrenewable petrochemical building blocks, and are characterized by untailored surfaces. Besides their significant drawbacks, they do not comply with environmental requirements and regulations and thus should be replaced with more eco-friendly products. The urgent need is to create robust and tunable nano/micro materials for confidently designing efficient and selective polymeric water filters with guaranteed sustainability and biodegradability. Active hybrid membranes made of eco-friendly high-grade microfibrillated cellulose (MFC), appropriately functionalized, have shown superior performance during the separation of metal ions from the industrial effluents, and their separation efficiency has been found to be tunable with a proper selection of type and density of the functional groups. On the basis of these findings and needs, we have developed a chemo-enzymatic functionalization strategy for grafting methyl and phosphate groups on the MFC fibers. This methodology can calibrate the interlayer fiber spacing and control the pore-size distribution of the membranes appropriately. We demonstrate this in the present work by characterizing the impact of Mg2+ and Cr3+ ions and their mixture (Mg2+ and Cr3+) on the membrane separation performance extensively by using various experimental techniques and computational methods. Moreover, we have adapted this sustainable, fully water-based system for upscaling the hybrid membranes in continuous mode by resorting to the phosphate-MFC membranes for the spiral-bound modules in cartridge use. We have developed the flow-through (FTM) and flow-over (FOM) modules and tested them to separate metal ions from the industrial effluent, ensuring regeneration and reusability. Our results indicate that these prototype hybrid MFC membranes represent the most promising type of next-generation high-performance filtration devices for a more sustainable society. © 2021 American Chemical Society.
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17.
  • Kimani, Martha, et al. (författare)
  • Imprinted Particles for Direct Fluorescence Detection of Sialic Acid in Polar Media and on Cancer Cells with Enhanced Control of Nonspecific Binding
  • 2021
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 3:5, s. 2363-2373
  • Tidskriftsartikel (refereegranskat)abstract
    • Glycoproteins are abundant on the cell surface of mammals, providing structural support, modulating cell membrane properties, and acting as signaling agents. Variation of glycosylation patterns has been found to indicate various disease states, including cell malignancy. Sialic acid (SA) is present as a terminating group on cell-surface glycans, and its overexpression has been linked to several types of cancer. Detection of SA on the cell surface is therefore critical for detection of cancer in its early stages. In this work, a fluorescent molecularly imprinted polymer layer targeting SA was synthesized on the surface of silica-coated polystyrene (PS) particles. Compared to previous works, a PS core supplies a lighter, lower-density support for improved suspension stability and scattering properties. Moreover, their smaller size provides a higher surface-area-to-volume ratio for binding. The incorporation of a fluorescent monomer in the MIP shell allowed for simple and rapid determination of binding specificity in polar media due to a deprotonation-reprotonation interaction mechanism between the fluorescent monomer and SA, which led to spectral changes. Upon titration of the MIP particles with SA in suspension, an increase in fluorescence emission of the particles was observed, with the MIP particles binding SA more selectively compared to the nonimprinted polymer (NIP) control particles. In cell staining experiments performed by flow cytometry, the binding behavior of the MIP particles compared favorably with that of SA-binding lectins. NIPs prepared with a "dummy" template served as a better negative control in cell binding assays due to the favorable inward orientation of template-binding functional groups in the polymer shell, which reduced nonspecific binding. The results show that fluorescent MIPs targeting SA are a promising tool for in vitro fluorescence staining of cancerous cells and for future diagnosis of cancer at early stages.
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18.
  • Liguori, Anna, et al. (författare)
  • Simple Non-Equilibrium Atmospheric Plasma Post-Treatment Strategy for Surface Coating of Digital Light Processed 3D-Printed Vanillin-Based Schiff-Base Thermosets
  • 2023
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 5:10, s. 8506-8517
  • Tidskriftsartikel (refereegranskat)abstract
    • A simple non-equilibrium atmospheric plasma post-treatment strategy was developed for the surface coating of three-dimensional (3D) structures produced by digital light processing 3D printing. The influence of non-equilibrium atmospheric plasma on the chemical and physical properties of vanillin-derived Schiff-base thermosets and the dip-coating process was investigated and compared to the influence of traditional post-treatment with UV-light. As a comparison, thermosets without post-treatment were also subjected to the coating procedure. The results document that UV post-treatment can induce the completion of the curing of the printed thermosets if complete curing is not reached during printing. Conversely, the plasma post-treatment does not contribute to the curing of the thermoset but causes some opening of the imine bonds and the regeneration of aldehyde functions. As a consequence, no great differences are observed between the not post-treated and plasma post-treated samples in terms of mechanical, thermal, and solvent-resistant properties. In contrast to the UV post-treatment, the plasma post-treatment of the thermosets induces a noticeable increase of the thermoset hydrophilicity ascribed to the reformation of amines on the thermoset surface. The successful coating process and the greatest uniformity of the lignosulfonate coating on the surface of plasma post-treated samples are considered to be due to the presence of these amines and aldehydes. The investigation of the UV shielding properties and antioxidant activities documents the increase of both properties with the increasing amount and uniformity of the formed coating. Interestingly, evident antioxidant properties are also shown by the noncoated thermosets, which are deduced to their chemical structures.
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19.
  • Lin, Jinjian, et al. (författare)
  • Impact of Polyester Dendrimers as Branched Multifunctional Cross-Linking Additives in Triazine-Trione-Based Composites Developed via High-Energy Visible Light Thiol-ene Chemistry
  • 2023
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 5:12, s. 10395-10403
  • Tidskriftsartikel (refereegranskat)abstract
    • Hydroxyapatite (HA) infused triazine-trione (TATO) composites have emerged as an injectable platform for customizable bone fixators due to their fast and benign curing via high-energy visible light-induced thiol-ene chemistry (HEV-TEC), promising mechanical performance, and preclinical outcomes. These composites can overcome many of the existing limitations accompanying metal implants such as poor patient customizability, soft tissue adhesions, and stress shielding. Taking into account that the promising benchmarked TATO composite (BC) is based on stable sulfur-carbon bonds, we herein investigate the impact of introducing polyester dendritic cross-linkers based on bis-MPA as chemically integrated branched additives that display labile esters in a branched configuration. The inclusion of dendrimers, G1 and G3, in concentrations of 1, 3, and 5 wt % in the composite formulations were found to (i) decrease the processing viscosity of the composite formulations, reaching Newtonic and nonshear thinning behavior at 37 degree celsius and (ii) impact the size distribution of bubble cavities in the composite cross sections. The lowest collected T-g for the dendrimer-containing composites was noted to be 73.2 degree celsius, a temperature well above physiological temperature. Additionally, all composites displayed flexural modulus above 6 GPa and flexural strength of ca. 50 MPa under dry conditions. The composites comprising 5 wt % of G1 and G3 dendrimers, with ester bond densities of 0.208 and 0.297 mmol/g, respectively, reached a mass loss up to 0.27% in phosphate buffered saline at 37 degree celsius, which is within the range of established polycaprolactone (PCL). Combined with the nontoxic properties extracted from the cell viability study, polyester dendrimers were determined as promising additives which compatibilized well with the TATO formulation and cross-linked efficiently resulting in strong composites suited for bone fracture fixations.
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20.
  • Melro, E., et al. (författare)
  • Poly(butylene succinate)-Based Composites with Technical and Extracted Lignins from Wood Residues
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 6:2, s. 1169-1181
  • Tidskriftsartikel (refereegranskat)abstract
    • Poly(butylene succinate) (PBS) has been drawing attention as a reliable biodegradable and sustainable alternative to synthetic petroleum-based polymers. In this study, PBS-lignin composites were developed using a recently extracted lignin (LA-lignin) from pine wood residues employing an innovative sustainable approach. These composites were systematically compared with PBS-based composites formed with commonly used technical lignins. The molecular weight of the lignins was evaluated, along with various structural and performance-related properties. The LA-lignin/PBS composites display a remarkably low water solubility (ca. < 2%), water uptake (ca. 100°). Moreover, the rigidity and thermal stability of the LA-lignin-PBS composites were higher than those of the systems formed with technical lignins. Although all composites studied present remarkable antioxidant features, the novel LA-lignin-PBS systems stand out in terms of antiadhesion activity against both Gram-positive and Gram-negative bacteria. Overall, the systematic analysis performed in this work regarding the impact of various lignins on the formed PBS composites enables a better understanding of the essential structural and compositional lignin features for achieving biobased materials with superior properties. 
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21.
  • Nechyporchuk, Oleksandr, et al. (författare)
  • Wet Spinning of Chitosan Fibers : Effect of Sodium Dodecyl Sulfate Adsorption and Enhanced Dope Temperature
  • 2020
  • Ingår i: ACS Appl. Polym. Mater.. - : American Chemical Society. - 2637-6105. ; 2:9, s. 3867-3875
  • Tidskriftsartikel (refereegranskat)abstract
    • Production of fibers from non-thermoplastic polymers, such as chitosan, usually requires dissolution with subsequent fiber formation, for instance via coagulation. Good fiber-forming properties enable simultaneous spinning of multiple fibers into a yarn, which is one of the prerequisites for process scalability. Here, we report a multifilament wet spinning process that eliminates the use of such volatile organic compounds as methanol and acetone, enhances fiber formation and allows producing continuous well separated chitosan fibers after drying. This is achieved by: (i) solidification of the extruded solution by alkali and sodium acetate in the coagulation bath and (ii) further stabilization of the fibers by adsorbing the anionic surfactant, sodium dodecyl sulfate. The obtained fibers have circular cross-section and smooth surface. We demonstrate that it is possible to increase fiber breaking tenacity and Young′s modulus by applying stretching (draw ratios up to 1.77) or by incorporating cellulose nanofibrils (CNF, up to 4 wt% based on chitosan) in the spinning solutions However, the limitation of increased viscosity when adding CNF is needed to be overcome for possible higher reinforcement effects. We demonstrate that fiber breaking tenacity, Young′s modulus and elongation at break can be enhanced even further by increasing the spin dope temperature from 22 °C to 60 °C, simultaneously with increasing the spin dope solids content to keep the same dope viscosity. The fibers with maximum breaking tenacity of ca. 10 cN tex-1 at an elongation at break of ca. 7.5% were obtained.
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22.
  • Ossipov, Dmitri A., et al. (författare)
  • Combination of Coordination and Releasable Covalent Binding for the Delivery of Antisense Therapeutics by BisphosphonateHyaluronan-Oligonucleotide Conjugates
  • 2021
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 3:4, s. 2197-2210
  • Tidskriftsartikel (refereegranskat)abstract
    • To address the current problems of delivery of antisense oligonucleotide (ON) therapeutics, a macromolecular platform was proposed based on the combination of metal-ion coordination and releasable covalent conjugation. Two kinds of therapeutic molecules, bisphosphonate (BP) and antisense ON, were conjugated to a natural polysaccharide hyaluronic acid (HA). The use of two linkers with a set of terminal chemoselective groups including Nhydroxysuccinimide carbonate, 2-dithiopyridyl, and aromatic aldehyde allowed orthogonal conjugation of the two therapeutics with subsequent detachment under potentially different conditions. In this work, disulfide linkages of varied steric accessibility were utilized in the linkers allowing the release of the linked therapeutics with different kinetics upon incubation in a reducing buffer. The therapeutics were conjugated to HA via their amino groups, and the self-immolative feature of the linkers permitted traceless release of both drugs as free amines. The obtained dual macromolecular prodrug was converted into either nanogels or macroscopic hydrogels upon coordination with calcium ions via Ca2+-mediated bridging of BP groups. Macroscopic hydrogels demonstrated self-healing properties which are useful for the noninvasive administration of ONs as biodegradable implants. Moreover, transformation of the macromolecular prodrug into a nanogel under dilute conditions is a useful property to prolong the circulation of the prodrug and protect antisense ON therapeutics against degradation in vivo.
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23.
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24.
  • Patel, Mitul Kumar, et al. (författare)
  • Biopolymer Blends of Poly(lactic acid) and Poly(hydroxybutyrate) and Their Functionalization with Glycerol Triacetate and Chitin Nanocrystals for Food Packaging Applications
  • 2022
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 4:9, s. 6592-6601
  • Tidskriftsartikel (refereegranskat)abstract
    • Polylactic acid (PLA) is a biopolymer that has potential for use in food packaging applications; however, its low crystallinity and poor gas barrier properties limit its use. This study aimed to increase the understanding of the structure property relation of biopolymer blends and their nanocomposites. The crystallinity of the final materials and their effect on barrier properties was studied. Two strategies were performed: first, different concentrations of poly(hydroxybutyrate) (PHB; 10, 25, and 50 wt %) were compounded with PLA to facilitate the PHB spherulite development, and then, for further increase of the overall crystallinity, glycerol triacetate (GTA) functionalized chitin nano crystals (ChNCs) were added. The PLA:PHB blend with 25 wt % PHB showed the formation of many very small PHB spherulites with the highest PHB crystallinity among the examined compositions and was selected as the matrix for the ChNC nanocomposites. Then, ChNCs with different concentrations (0.5, 1, and 2 wt %) were added to the 75:25 PLA:PHB blend using the liquid-assisted extrusion process in the presence of GTA. The addition of the ChNCs resulted in an improvement in the crystallization rate and degree of PHB crystallinity as well as mechanical properties. The nanocomposite with the highest crystallinity resulted in greatly decreased oxygen (O) and carbon dioxide (CO2) permeability and increased the overall mechanical properties compared to the blend with GTA. This study shows that the addition ChNCs in PLA:PHB can be a possible way to reach suitable gas barrier properties for food packaging films.
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25.
  • Poulose, Simi, et al. (författare)
  • A Green High Barrier Solution for Paperboard Packaging based on Potato Fruit Juice, Poly(lactic acid), and Poly(butylene adipate terephthalate)
  • 2022
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 4:6, s. 4179-4188
  • Tidskriftsartikel (refereegranskat)abstract
    • The potential of using potato fruit juice (PFJ), a byproduct from the potato starch industry, was investigated as a barrier paper-coating material. The paperboard was initially hand-coated with PFJ (with and without glycerol as plasticizer) and then extrusioncoated with poly(lactic acid) (PLA) or a blend of PLA and poly(butylene adipate terephthalate) (PBAT). The multilayer coated paperboard was homogeneous in appearance with a glossy finish. The coated paperboard showed, at the most, a ca. 95% reduction in specific water vapor transmission rate compared to the uncoated paperboard. In the presence of the PFJ layer, the extrusion-coated paperboard experienced, at the most, a 98% reduction in oxygen permeability. The grease resistance of the paperboard was also improved significantly with this multilayer coating. PLA- and PFJ-coated samples showed better barrier properties, whereas PFJ with PLA/PBAT layers exhibited better adhesion and heat-sealing properties. The peel strength of the coated samples was moderately good for paper converting applications. The developed coated paperboard also exhibited good creasing properties which is yet again an advantage for packaging applications. The presented barrier properties make the developed multilayer coatings on paperboards a sustainable competitive alternative to several of today's coatings. KEYWORDS: paper coating, barrier coating, bio-based coating, potato fruit juice, poly(lactic acid), poly(butylene adipate terephthalate), barrier properties, peel strength, heat sealing
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26.
  • Qin, Congwen, et al. (författare)
  • Insight into the Keratin Ratio Effect of the Keratin/Cellulose Composite Fiber
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society. - 2637-6105. ; 6:1, s. 265-276
  • Tidskriftsartikel (refereegranskat)abstract
    • In this work, biocompatible composite fibers were prepared from human hair keratin and plant cellulose with different proportions by the wet-spinning method, and their properties and performance, including chemical structures, morphology, mechanical strength, and cell proliferation and attachment, were systematically investigated. It showed that the best proportion of the keratin/cellulose mass ratio was 30:70, and its tensile strength reached 277 MPa (elongation at break can be 27%), which is higher than that of the regenerated cellulose fiber (193 MPa, 12%). Its viability and proliferation of L929 murine fibroblast cells are also better than those of the regenerated cellulose fiber. Atomistic simulations were carried out and demonstrated the formation of hydrogen bonds between keratin and cellulose molecules, clarifying that the ratio of keratin has a significant effect on the aggregation structures in the solution and that the hydrogen bonds formed between keratin and cellulose molecules have a distinct contribution to the biocompatible composites. This work demonstrates the potential of the prepared composite fiber in biomedical applications and provides an innovative way to utilize waste human hair as a high-value raw material.
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27.
  • R. Hinojosa, Diego, et al. (författare)
  • Solubilizing Benzodifuranone-Based Conjugated Copolymers with Single-Oxygen-Containing Branched Side Chains
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - 2637-6105. ; 6:1, s. 457-465
  • Tidskriftsartikel (refereegranskat)abstract
    • Single-oxygen-containing branched side chains are designed and used to solubilize n-type copolymers consisting of BDF (benzodifuranone), isatin, and thiophene-based units. We present a simple synthetic approach to side chains with varying linker distances between the backbone and the branching point. The synthetic pathway is straightforward and modular and starts with commercially available reagents. The side chains give rise to excellent solubilities of BDF-thiophene copolymers of up to 90 mg/mL, while still being moderate in size (26-34 atoms large). The excellent solubility furthermore allows high molar mass materials. BDF-thiophene copolymers are characterized in terms of optoelectronic and thermoelectric properties. The electrical conductivity of chemically doped polymers is found to scale with molar mass, reaching ∼1 S/cm for the highest molar mass and longest backbone-branching point distance.
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28.
  • Rolland, Nicolas, et al. (författare)
  • Can Mobility Negative Temperature Coefficient Be Reconciled with the Hopping Character of Transport in Conducting Polymers?
  • 2019
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : AMER CHEMICAL SOC. - 2637-6105. ; 1:11, s. 2833-2839
  • Tidskriftsartikel (refereegranskat)abstract
    • Poly(3,4-ethylenedioxythiophene) (PEDOT) is a conducting polymer that is used in a wide range of applications such as electronics, optoelectronics, and bio-electronics, where the fundamental understanding of the charge transport, and in particular of the electrical conductivity sigma, is a prerequisite to develop new high performance devices. There are many reports in the literature where the conductivity of archetypical conducting polymer PEDOT doped with tosylate (PEDOT:TOS) exhibits a dry negative temperature coefficient, d sigma/dT < 0, which is strikingly different from the activated-type behavior with d sigma/dT > 0 commonly observed in most conducting polymers. This unusual temperature dependence was attributed to the transition from the photon-assisted hopping to the metallic behavior, which is however difficult to rationalize taking into account that this transition occurs at high temperatures. In order to understand the origin of this unusual behavior, multiscale mobility calculations in PEDOT:TOS for the model of hopping transport were performed, where changes in the morphology and the density of states (DOS) with the temperature were explicitly taken into account. The morphology was calculated using the Molecular Dynamics simulations, and the hopping rates between the chains were calculated quantum-mechanically following the Miller-Abrahams formalism. Our results reproduce the observed negative temperature coefficient, where however the percolation analysis shows that this behavior mainly arises because of the changes in morphology upon heating when the system becomes less ordered. This results in a less efficient pi-pi stacking and hence lower mobility in the system. We therefore conclude that experimentally observed negative mobility temperature coefficient in conducting polymers at high temperatures is consistent with the hopping transport, and does not necessarily reflect the transition to a metallic band-like transport. Based on our multiscale modeling, we introduce a simple Gaussian Disorder Model for the efficient mobility calculations, where the DOS broadening is a function of the temperature, and where the transfer integral distribution is a bimodal distribution evolving with temperature.
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29.
  • Rossi, Ruggero, et al. (författare)
  • Photoswitches in Order : One-Pot Synthesis of Azobenzene Main-Chain and Segmented Copolymers
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 6:2, s. 1563-1572
  • Tidskriftsartikel (refereegranskat)abstract
    • Syntheses of multifunctional polymers aim to engineer a wide range of material properties by adjusting the composition and positioning of functional groups. While manifold syntheses of side-chain-functionalized polymers are known, synthetic protocols for main-chain-functionalized polymers are less common. This work describes a general one-pot strategy to prepare polymers containing multiple functional moieties in their main-chain, e.g., azobenzene units separated by variable oligomers. The polymerization proceeds in two steps, starting from a single azobenzene initiator and commercially available monomers (lactones and cyclic carbonates). Various main-chain-functionalized polymers were obtained with a predictable and adjustable ratio of monomer units (5-20) to photoswitchable azobenzene groups. The thermal properties of these polymers were analyzed and rationalized with regard to the parent polymers' properties and the peculiarities arising from their segmented microstructure. Furthermore, the azobenzenes' ability to undergo light-induced cis/trans-isomerization is confirmed. High isomerization yields of up to 90% were observed for the polymers in solution with a half-life of several days for the cis-isomers in solution. When irradiated as solid films, the azobenzenes still undergo isomerization, but the cis-isomers are less stable compared to the liquid state.
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30.
  • Rouhi, Mona, et al. (författare)
  • Role of Comonomers in the Recognition of Anionic Biomolecules in Water : Hydrogen-Bonded Imprinted Polymeric Receptor
  • 2021
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 3:10, s. 4904-4912
  • Tidskriftsartikel (refereegranskat)abstract
    • The field of anion recognition in aqueous media is dominated by multiple positive charges and/or metal ions containing synthetic receptors. Here, we report the synthesis of a highly water-compatible oxyanion-imprinted neutral receptor by cross-linking the polymerizable diary! urea host monomer and phenyl phosphonic acid (PPA) complex in the presence of a large number of comonomers containing hydroxyl or methyl ester groups. We have demonstrated that the affinity of the imprinted receptor for anions is easily tuned by decorating the hydrophilic and hydrophobic end groups around the binding pocket of the imprinted receptor. The binding characteristics of the synthesized artificial binders were evaluated in aqueous and nonaqueous environments. We have demonstrated practical applicability of the PPA-imprinted receptor by packing in the solid-phase extraction cartridge which was used to separate the ubiquitous pesticide glyphosate from water. Also, the developed receptor can selectively bind to phosphorylated tyrosine amino acids and phosphorylated tyrosine octapeptides in aqueous buffered media than to other phosphorylated and nonphosphorylated analogues. The approach utilized here to use an inexpensive dummy template can be utilized for the synthesis of imprinted receptors for anions with phosphate motifs.
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31.
  • Scalon, Lucas, et al. (författare)
  • Assessing the Donor-Acceptor Nature and the Electrochemical Stability of a Fluorene-Diketopyrrolopyrrole-Thiophene-Based Copolymer
  • 2021
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 3:8, s. 4223-4233
  • Tidskriftsartikel (refereegranskat)abstract
    • Organic dyes have been studied for applications in large-area, flexible, cheap, and efficient organic electronic devices. Among them, diketopyrrolopyrrole (DPP) has gained attention thanks to its planar structure, photochemical and thermal stability, and easy processability. Also, the electron-withdrawing nature of DPP makes its application attractive in the synthesis of donor-acceptor (D-A) copolymers, with appealing features such as the tunable energy levels and photophysical and electrochemical properties. Inspired by these exciting characteristics, a copolymer was developed based on DPP, thiophene, and fluorene (PFDPP2T). Photophysical and electrochemical studies using both experimental and theoretical approaches were performed aiming to understand the properties of this material, such as, for instance, the D-A characteristic and the outstanding electrochemical stability upon oxidation that enables more than 400 cycles of p-doping. The outcomes unveil fundamental aspects of this class of copolymers, reinforcing their suitability for photo-electrochemical and optoelectronic applications.
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32.
  • Singha, Shuvra, et al. (författare)
  • Plant Cuticle-Inspired Polyesters as Promising Green and Sustainable Polymer Materials
  • 2021
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 3:8, s. 4088-4100
  • Tidskriftsartikel (refereegranskat)abstract
    • The plant cuticle is a hydrophobic barrier membrane found mainly on leaf surfaces and fruit skin. This work presents the structural and barrier properties of cuticle-inspired poly(hydroxyhexadecanoate) (PHHA), an omega-hydroxy fatty acid-derived biopolyester. PHHA was copolymerized and cross-linked with glycerol by melt polycondensation, and films were fabricated by compression molding. The study showed the effect of the addition of a trifunctional comonomer on the thermal, mechanical, and barrier properties. The neat PHHA, owing to its higher crystallinity, demonstrated the best water vapor barrier properties, but formed brittle films. The glycerol-copolymerized films, on the other hand, were flexible and displayed a good balance between barrier and mechanical properties. The water vapor transmission rate was overall similar to that of PLA, and limonene (a hydrophobic food component) uptake and diffusivity were lower than that of low-density polyethylene, the commonly used polymer for packaging. In addition, the polyester had UV-blocking properties. The way the films were made yielded a rough surface, mimicking the outer rough wax layer in plant cuticles with high water repellence. Hence, these cutin-inspired polyesters are promising for, e.g., water barrier (packaging/device) applications, provided means of efficient/sustainable production/isolation of the monomer is developed.
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33.
  • Suriyanarayanan, Subramanian, et al. (författare)
  • On-Surface Synthesis of Porosity-Controlled Molecularly Imprinted Polymeric Receptors for the Biotinyl Moiety
  • 2024
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 6:2, s. 1470-1482
  • Tidskriftsartikel (refereegranskat)abstract
    • Controlled on-surface synthesis of polymer films using amide-based, environmentally friendly, nonionic deep eutectic solvents (ni-DESs) has been developed to regulate the porous features of the films. An appropriate combination of acetamide (A), urea (U), and their methyl derivatives (N-methylacetamide (NMA) and N-methylurea (NMU)) was used to prepare ni-DES. Polymer films were electrosynthesized using 4-aminobenzoic acid (4-ABA) and pyrrole as monomers in ni-DESs. We presumed that the flickering-cluster-like complexes and the extended H-bond networks in ni-DESs enhance the porosity of the polymer films, thus improving permeability features, as reflected in sensor performance. Electrosynthesized polymer films, imprinted with biotin templates (MIPs), have been tested as receptors for biotinylated targets. Molecular dynamics simulations of the prepolymerization mixture revealed the formed complexes between 4-ABA and biotin comprising high-frequency H-bonds. X-ray photoelectron spectroscopy (XPS) and reflection absorption infrared spectroscopy (RAIRS) studies revealed the structural integrity in the polymer films irrespective of the medium. Scanning electron microscopy (SEM) and electrochemical impedance spectroscopy (EIS) measurements showed a highly corrugated and porous nature for MIPA-U and MIPNMU-U when prepared in A-U and NMU-U ni-DESs. Atomic force microscope (AFM) studies support these observations, displaying an enhancement in the surface roughness from 1.44 nm (MIPaqueous) to 23.6 nm (MIPNMU-U). QCM analysis demonstrated a remarkable improvement in sensitivity of MIPA-U (17.99 +/- 0.72 Hz/mM) and MIPNMU-U (18.40 +/- 0.81 Hz/mM) films toward the biotin methyl ester (BtOMe, biotin derivative) than the MIPaqueous film. The chemosensor devised with the above MIP recognition films selectively recognized BtOMe (LOD = 12.5 ng/mL) and biotinylated biomolecules, as shown by the stability constant K-s values (MIPA-U = 1442 and MIPNMU-U = 1502 M-1). The porous network generated in the polymer films by the flickering-cluster-like complexes present in the ni-DES facilitates the analyte diffusion and recognition. We propose this ni-DES as an economically advantageous and environmentally friendly alternative to conventional ionic liquids and organic solvents in polymer synthesis and to influence polymer morphology for developing hierarchical materials.
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34.
  • Svenningsson, Leo, 1990, et al. (författare)
  • Polarized Raman Spectroscopy Strategy for Molecular Orientation of Polymeric Fibers with Raman Tensors Deviating from the Molecular Frame
  • 2020
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 2:11, s. 4809-4813
  • Tidskriftsartikel (refereegranskat)abstract
    • Polarized light is frequently used to identify molecular anisotropy in polymers, biological systems, and other materials. The influence of the Raman tensor by polarized light reveals not only the chemical structure but also information on the morphology of polymers. The orientation distribution of molecules in polymers has previously been determined for systems with the principal axis components of the Raman tensor parallel to the molecular frame. In many cases, the Raman tensor principal axis is not parallel to the molecular chain axis. Therefore, the orientation of the Raman tensor, relative to the molecular chain axis, is crucial if accurate information about the molecular orientation distribution is sought for. This work presents a strategy for separating the Raman tensor orientation angles from the molecular orientation angles for polymeric samples with fiber symmetry. Composite polymeric materials often experience signal overlap in the X-ray scattering wide-angle region, where the anisotropy is often resolved. While X-ray scattering investigates intermolecular distances, Raman spectroscopy resolves chemical information, and anisotropy, by the influence of Raman scattering. The quantitative principles presented here may aid in the evaluation of anisotropy in such composite materials.
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35.
  • Sångeland, Christofer, et al. (författare)
  • Stable Cycling of Sodium Metal All-Solid-State Batteries with Polycarbonate-Based Polymer Electrolytes
  • 2019
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 1:4, s. 825-832
  • Tidskriftsartikel (refereegranskat)abstract
    • Solid polymer electrolytes based on high-molecular-weight poly(trimethylene carbonate) (PTMC) in combination with NaFSI salt were investigated for application in sodium batteries. The polycarbonate host material proved to be able to dissolve large amounts of salt, at least up to a carbonate:Na+ ratio of 1:1. Combined DSC, conductivity, and FTIR data indicated the formation of a percolating network of salt clusters along with the transition to a percolation-type ion transport mechanism at the highest salt concentrations. While the highest total ionic conductivities were seen at the highest salt concentrations (up to a remarkable 5 x 10(-5) S cm(-1) at 25 degrees C at a 1:1 carbonate:Na+ ratio), the most stable battery performance was seen at a more moderate salt loading of 5:1 carbonate:Na+, reaching >80 cycles at a stable capacity of similar to 90 mAh g(-1) at 60 degrees C in a sodium metal/Prussian blue cell. The results highlight the importance of the choice of salt and salt concentration on electrolyte performance as well as demonstrate the potential of utilizing polycarbonate-based electrolytes in sodium-based energy storage systems.
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36.
  • Wang, Bei, et al. (författare)
  • Sandwiched Polyethylene Shrink Film Masking with Tunable Resolution and Shape for Liquid Alloy Patterning
  • 2019
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 1:2, s. 145-151
  • Tidskriftsartikel (refereegranskat)abstract
    • Among numerous patterning techniques, masked liquid alloy printing is one of the most promising techniques for scalable fabrication of liquid-alloy-based stretchable electronics. Like any other mask-based process, its resolution is often constrained by the quality of the mask, and the fabrication cost increases drastically with increased resolution. In this work, by introducing a sandwiched thermal shrink polymer film masking technique and a corresponding intermediate release agent, fine liquid alloy patterns were demonstrated by using a mechanical cutting plotter together with a common oven. The final resolution and shape of the mask could be tuned based on the anisotropy of the shrink polymer film and other operational parameters of the technique. After shrinkage, the width of the patterned liquid alloy lines and space in-between could be tuned to less than one third of the original cut pattern, to about 35 and 60 mu m, respectively, according to requirements. To better predict the final structure, several parameters were investigated experimentally and numerically. Finally, a liquid alloy strain sensor and three-dimensional conformal masking were demonstrated, showing the potential of the developed technique.
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37.
  • Xiao, Linhong, et al. (författare)
  • Recent Advances in Polymer-Based Photothermal Materials for Biological Applications
  • 2020
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 2:10, s. 4273-4288
  • Forskningsöversikt (refereegranskat)abstract
    • The photothermal effect, which is a phenomenon of converting light energy into thermal energy using photothermal conversion materials, has recently attracted significant attention in biological applications because of the minimal invasiveness to healthy tissues, high specificity, and easy operation. Polymer-based photothermal materials have emerged as a promising category of photothermal agents in biological applications because they show superiorities in tailorable molecular structures, high photothermal conversion efficiencies, and excellent biocompatibility. In this Review, we summarize the recent progresses achieved in polymer-based photothermal materials for biological applications. To have a better understanding of the working mechanism and the design of polymer-based photothermal materials, this Review starts with the fundamental description of photothermal conversion mechanism of polymer-based photothermal materials. According to their structures and compositions, the polymer-based photothermal materials can be classified into three types: conjugated polymers, polymer-modified carbon nanomaterials, and polymer-modified metals and metal compounds. Then we present the recent advances of the polymer-based photothermal materials in a diversity of biological areas such as photothermal therapy and photothermal sterilization. In the last section, we summarize the critical existing issues in polymer-based photothermal materials for biological applications and propose some perspectives that are related to the design and synthesis of polymer-based photothermal materials for biological applications.
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38.
  • Xu, Huan, et al. (författare)
  • Nanostructured Phase Morphology of a Biobased Copolymer for Tough and UV-Resistant Polylactide
  • 2021
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 3:4, s. 1973-1982
  • Tidskriftsartikel (refereegranskat)abstract
    • Despite technological feasibility and industrial scalability in toughening polylactide (PLA) by direct blending, avoiding the sacrifice of mechanical strength or full renewability remains a challenge. Here, low-molecular-weight poly(ethylene 2,5-furandicarboxylate)-block-polylactide (PEF-b-PLA) was synthesized to yield a fully biobased copolymer with expected partial miscibility with PLA. The ability of PEF-b-PLA to toughen PLA at 10 wt % (PLA10) and 20 wt % (PLA20) loadings was then evaluated. To understand the achieved properties, the formation of a nanostructured dispersion phase due to favorable interfacial adhesion arising from the miscibility of the PLA block with the PLA matrix was investigated. The morphological features, together with comparable strength inherited from the PEF blocks, afforded an unusual combination of toughness and strength for the PLA blends. Compared to the poor tensile toughness of a pure PLA film (1.77 MJ/m(3)), a striking increase of 839 and 912% was achieved for PLA10 and PLA20, respectively. More importantly, both pure PLA and the blends were characterized by comparable yield strength (similar to 30 MPa). This was accompanied by excellent UV-shielding imparted by the functional groups on the PEF blocks, which would improve the prospects of realizing PLA-based functional packing materials. The proposed design of copolymers, with good industrial feasibility, should be useful to guide the toughening approaches for PLA and probably other degradable polyester blends by profound morphology control.
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39.
  • Xu, Yunsheng, et al. (författare)
  • Recyclable and Flexible Polyester Thermosets Derived from Microwave-Processed Lignin
  • 2020
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 2:5, s. 1917-1924
  • Tidskriftsartikel (refereegranskat)abstract
    • Commercial Kraft lignin was successfully valorized into recyclable and flexible polyester thermosets. Kraft lignin was first processed into more well-defined lignin fractions via liquid-solid extraction in green solvents (methanol and ethanol) or microwave-processed in ethanol at different temperatures (80 and 160 degrees C). The lignin fractions were then cross-linked in one pot with PEG and citric acid into polyester thermosets. In comparison to the thermoset synthesized from the original Kraft lignin, the thermosets synthesized from all the ethanol-extracted fractions were more homogenous and flexible as reflected by a sharper alpha-transition and over 100% increase in elongation at break. Furthermore, recycling of two of the prepared thermosets was evaluated (i.e., the thermoset prepared from the original lignin and the one prepared from microwave-processed lignin). Both materials could be rapidly recycled back into liquid resins under microwave hydrolysis and recured into thermosets under the original curing conditions. However, good quality films and comparable mechanical properties were only obtained after recuring the recycled resin originally synthesized from the microwave-processed lignin. Microwave processing compared to liquid-solid extraction paved the way for higher yields of narrow dispersity lignin fractions and matching final properties, providing an attractive approach to recyclable flexible lignin thermosets.
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40.
  • Xue, Xiaoting, et al. (författare)
  • Amplification of Molecular Recognition Signal on Imprinted Polymers Using Hybridization Chain Reaction
  • 2023
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 5:1, s. 680-689
  • Tidskriftsartikel (refereegranskat)abstract
    • Hybridization chain reaction (HCR)-based amplification strategies have shown excellent prospects of application in detection thanks to its non-enzymatic and isothermal features. For protein biomarker detection, most bioanalytical assays are dependent on antibodies or aptamers to provide specific recognition to allow single strand DNA (ssDNA) to initiate specific HCR to realize effective signal amplification. Molecularly imprinted polymers (MIPs) are excellent alternative molecular recognition materials because of low cost and high stability. In this work, we developed a non-enzymatic, HCR-amplified protein detection/quantification using MIP as a recognition element for hemoglobin (Hb). The MIP was prepared by Pickering emulsion polymerization using mesoporous silica nanoparticles as a stabilizer, producing surface-accessible binding sites for Hb. To demonstrate specific detection of proteins, Hb captured by the MIP beads was reacted with a ssDNA to add the initiator sequence of the HCR to the captured protein in situ. After addition of two hairpin DNA molecules that were labeled with fluorophores and quenchers, the HCR reaction took place and led to the opening of the hairpins and formation of nicked dsDNA, with concomitant emission of fluorescence. A linear relationship between fluorescence intensity and the logarithm protein concentration in the range of 0.01–1 mg/mL was obtained. The limit of Hb detection was as low as 0.006 mg/mL. In addition, the non-enzymatic, isothermal fluorescent detection exhibited high selectivity, satisfactory recovery, and good repeatability. This work opens possibilities of using MIP and nucleic acid amplification to achieve low-cost, simple, and reliable detection and quantification of protein biomarkers.
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41.
  • Yandi, Wetra, et al. (författare)
  • Polyampholytic Poly(AEMA-co-SPMA) Thin Films and Their Potential for Antifouling Applications
  • 2021
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 3:11, s. 5361-5372
  • Tidskriftsartikel (refereegranskat)abstract
    • Polyampholytic poly(2-aminoethyl methacrylate-co-sulfopropyl methacrylate) (p(AEMA-co-SPMA)) thin films were prepared by self-initiated photopolymerization and photografting (SIPGP) and are demonstrated to be a potential alternative to films prepared from zwitterionic poly(sulfobetaine methacrylate) (pSBMA) for antifouling applications. SIPGP allows polymerization from aqueous solutions containing only monomers, implying that p(AEMA-co-SPMA) thin films can be prepared simply and inexpensively without the risk of introducing potentially toxic substances necessary in many controlled polymerization reactions. For the polymers, wettabilities were studied by contact angle goniometry, the compositions of the films were determined by infrared and X-ray photoelectron spectroscopies, and streaming current measurements were used to assess their net charge. The antibiofouling properties were compared via adsorption of fibrinogen and bovine serum albumin, settlement of algal zoospores, and the growth of sporelings of the marine alga Ulva lactuca. The fouling of the p(AEMA-co-SPMA) copolymer was in several respects similar to that of the zwitterionic pSBMA and suggests that it is potentially suitable for applications under high-salinity conditions, such as marine or physiological environments.
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42.
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43.
  • Yuan, Yusheng, et al. (författare)
  • Mechanochemical Preparation and Self-Assembly of Protein : Dye Hybrids for White Luminescence
  • 2021
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 3:10, s. 4825-4836
  • Tidskriftsartikel (refereegranskat)abstract
    • Protein nanofibrils (PNFs) functionalized with multiple dyes are prepared by a combination of mechanochemistry and liquid-phase self-assembly. The three employed dyes are Fluorescent Brightener 378 (F378), 2-butyl-6-(butylamino)-1H-benzo[de]isoquinoline-1,3(2H)-dione (Fluorol 555), and Nile red (NR). F378 acts as the donor with Fluorol 555 as the acceptor. F555 in turn acts as the donor and NR as the acceptor. This enables a FRET cascade that enables conversion of UV light to white light. The efficiency of FRET can be influenced by the details of the self-assembly process. If proteins milled with different dyes are mixed prior to self-assembly, nanofibrils are formed containing all three dyes, thus favoring FRET processes. By tuning the ratio of the three luminescent dyes, PNF dispersions are obtained that display bright white light emission. Moreover, the PNF dispersions can be converted into white luminescent films and gels where the PNFs may help to organize dye molecules. Additionally, the PNF materials can be employed as coatings on commercial LEDs, enabling emission of white light.
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44.
  • Zhang, Qicheng, et al. (författare)
  • Molecularly Imprinted Polymers for Targeting Lipopolysaccharides and Photothermal Inactivation of Pseudomonas aeruginosa
  • 2023
  • Ingår i: ACS Applied Polymer Materials. - 2637-6105. ; 5:4, s. 3055-3064
  • Tidskriftsartikel (refereegranskat)abstract
    • Although photothermal therapy is of significance in therapeutic strategies for fighting bacterial infection, the precise target of photothermal agents to bacterial sites is still a challenge. In this work, lipopolysaccharide (LPS) imprinted photothermal molecularly imprinted polymers (PMIP) were prepared for the efficient capture and elimination of Pseudomonas aeruginosa. The LPS derived from Pseudomonas aeruginosa was selected as a template due to its cis-diol structure, which can provide active sites to direct the boronate affinity-mediated synthesis of molecularly imprinted polymers. Polydopamine with good biocompatibility and photothermal effect was used as an imprinting matrix to achieve good photothermal function and imprinting efficiency. The combination of bacteria-imprinting with photothermal ability allowed PMIP to deactivate target bacteria with enhanced precision and efficiency. Taken together, our study offers a promising strategy to design synthetic materials for targeting and treating pathogens for various infectious diseases and expands the application of molecular imprinting technology in the field of antimicrobials.
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45.
  • Zhou, Qilong, et al. (författare)
  • Versatile Ionic Gel Driven by Dual Hydrogen Bond Networks : Toward Advanced Lubrication And Self-Healing
  • 2021
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 3:11, s. 5932-5941
  • Tidskriftsartikel (refereegranskat)abstract
    • From one to more, the same raw materials giving rise to multifarious products is one of the goals of researchers to pursue industrial efficiency. Herein, we designed a formula (controlling the content of the matrix) to prepare two functional ionic gels, integrating the excellent lubrication, thermal conductivity, and self-healing ability to meet different industrial demands of the lubrication and biomedical fields. Deep eutectic solvents (DESs) of urea/choline chloride (UCC) and glycerol/choline chloride (GCC) were locked in polyacrylamide (PAM) ionic gel formed by acrylamide (AM) and a photoinitiator by freer-adical polymerization. The unique dual hydrogen bond network in the ionic gel causes the material to exhibit a low wear rate, which can effectively reduce the wear of metal contact. With the addition of PAM, the ionic gel has excellent mechanical strength and good recovery performance. Unexpectedly, this dense hydrogen bond network enhances thermal conductivity by optimizing phonon and electron transfer. The versatile ionic gel has a good application prospect as a substitute for industrial lubricants and medical device materials.
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46.
  • Zozoulenko, Igor, et al. (författare)
  • Polarons, Bipolarons, And Absorption Spectroscopy of PEDOT
  • 2019
  • Ingår i: ACS APPLIED POLYMER MATERIALS. - : American Chemical Society (ACS). - 2637-6105. ; 1:1, s. 83-94
  • Tidskriftsartikel (refereegranskat)abstract
    • Electronic structure and optical absorption spectra of poly(3,4-ethyl-enedioxythiophene) (PEDOT) for different oxidation levels were studied using density functional theory (DFT) and time-dependent DFT. It is shown, that the DFT-based predictions for the polaronic and bipolaronic states and the nature of corresponding optical transitions are qualitatively different from the widely used traditional picture based on semi-empirical pre-DFT approaches that still dominate the current literature. On the basis of the results of our calculations, the experimental Vis/NIR absorbance spectroscopy and the electron paramagnetic resonance spectroscopy are re-examined, and a new interpretation of the measured spectra and the spin signal, which is qualitatively different from the traditional interpretation, is provided. The findings and conclusions concerning the nature of polaronic and bipolaronic states, band structure and absorption spectra presented for PEDOT, are generic for a wide class of conducting polymers (such as polythiophenes and their derivatives) that have a similar structure of monomer units.
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47.
  • Özeren, Hüsamettin Deniz, et al. (författare)
  • Ranking Plasticizers for Polymers with Atomistic Simulations; PVT, Mechanical Properties and the Role of Hydrogen Bonding in Thermoplastic Starch
  • 2020
  • Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 2:5, s. 2016-2026
  • Tidskriftsartikel (refereegranskat)abstract
    • Virgin biopolymers are often brittle and, therefore, need the addition of plasticizers to obtain the required mechanical properties for practical applications, e.g. in bags and disposable kitchen items. In this article, based on a combined experimental and modelling approach, it is shown that it is possible to rank molecules with respect to their plasticization efficiency (depression in glass transition temperature with PVT data and reduced stiffness and strength) using molecular dynamics simulations. Starch was used as the polymeric matrix material due to its promising potential as a sustainable, eco-friendly, biobased replacement for fossil-based plastics. Three polyols (glycerol, sorbitol and xylitol), two ethanolamines and glucose were investigated. The results indicate that molecular simulations can be used to find the optimal plasticizer among a set of candidates, or to design/identify better plasticizers in a complex polymer system. Glycerol was the most efficient of the six plasticizers, explained by it forming the least amount of hydrogen bonds, having the shortest hydrogen bond lifetimes and low molecular rigidity. Hence, not only was it possible to rank plasticizers, the ranking results could also be explained by the simulations.
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