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Advanced Materials (Deerfield Beach,... Jun 2024Extensively-used rechargeable lithium-ion batteries (LIBs) face challenges in achieving high safety and long cycle life. To address such challenges, ultrathin solid...
Extensively-used rechargeable lithium-ion batteries (LIBs) face challenges in achieving high safety and long cycle life. To address such challenges, ultrathin solid polymer electrolyte (SPE) is fabricated with reduced phonon scattering by depositing the composites of ionic-liquid (1-ethyl-3-methylimidazolium dicyamide, EMIM:DCA), polyurethane (PU) and lithium salt on the polyethylene separator. The robust and flexible separator matrix not only reduces the electrolyte thickness and improves the mobility of Li, but more importantly provides a relatively regular thermal diffusion channel for SPE and reduces the external phonon scattering. Moreover, the introduction of EMIM:DCA successfully breaks the random intermolecular attraction of the PU polymer chain and significantly decreases phonon scattering to enhance the internal thermal conductivity of the polymer. Thus, the thermal conductivity of the as-obtained SPE increases by approximately six times, and the thermal runaway (TR) of the battery is effectively inhibited. This work demonstrates that optimizing thermal safety of the battery by phonon engineering sheds a new light on the design principle for high-safety Li-ion batteries.
PubMed: 38876140
DOI: 10.1002/adma.202405097 -
Water Research Aug 2024The accumulation of polyurethane plastics (PU-PS) in the environment is on the rise, posing potential risks to the health and function of ecosystems. However, little is...
The accumulation of polyurethane plastics (PU-PS) in the environment is on the rise, posing potential risks to the health and function of ecosystems. However, little is known about the degradation behavior of PU-PS in the environment, especially water environment. To address this knowledge gap, we investigated and isolated a degrading strain of Streptomyces sp. B2 from the surface of polyurethane coatings. Subsequently, a photoreactor was employed to simulate the degradation process of bio-based polyurethane (BPU) and petroleum-based polyurethane (PPU) under three conditions, including single microorganism (SM), single light exposure (SL), and combined light exposure/microorganism action (ML) in aqueous solution. The results indicated that PU-PS mainly relies on biodegradation, with the highest degradation rate observed after 28 d under SM condition (BPU 5.69 %; PPU 5.25 %). SL inhibited microbial growth and degradation, with the least impact on plastic degradation. Microorganisms colonized the plastic surface, secreting relevant hydrolytic enzymes and organic acids into the culture medium, providing a negative charge. The carbon chains were broken and aged through hydrogen peroxide induction or attack by oxygen free radicals. This process promoted the formation of oxidized functional groups such as OH and CO, disrupting the polymer's structure. Consequently, localized fragmentation and erosion of the microstructure occurred, resulting in the generation of secondary microplastic (MPs) particles, weight loss of the original plastic, increased surface roughness, and enhanced hydrophilicity. Additionally, BPU exhibited greater degradability than PPU, as microorganisms could utilize the produced fatty acids, which promoted their reproduction. In contrast, PPU degradation generated a large amount of isocyanate, potentially toxic to cells and inhibiting biodegradation. This study unveils the significant role of microorganisms in plastic degradation and the underlying degradation mechanisms of BPU, providing a novel strategy for polyurethane degradation and valuable information for comprehensive assessment of the behavior and fate of MPs in the environment.
Topics: Polyurethanes; Biodegradation, Environmental; Light; Plastics; Streptomyces
PubMed: 38875861
DOI: 10.1016/j.watres.2024.121856 -
Biomaterials Advances Sep 2024Bioengineering seeks to replicate biological tissues exploiting scaffolds often based on polymeric biomaterials. Digital light processing (DLP) has emerged as a potent...
Bioengineering seeks to replicate biological tissues exploiting scaffolds often based on polymeric biomaterials. Digital light processing (DLP) has emerged as a potent technique to fabricate tissue engineering (TE) scaffolds. However, the scarcity of suitable biomaterials with desired physico-chemical properties along with processing capabilities limits DLP's potential. Herein, we introduce acrylate-endcapped urethane-based polymers (AUPs) for precise physico-chemical tuning while ensuring optimal computer-aided design/computer-aided manufacturing (CAD/CAM) mimicry. Varying the polymer backbone (i.e. poly(ethylene glycol) (PEG) versus poly(propylene glycol) (PPG)) and photo-crosslinkable endcap (i.e. di-acrylate versus hexa-acrylate), we synthesized a series of photo-crosslinkable materials labeled as UPEG2, UPEG6, UPPG2 and UPPG6. Comprehensive material characterization including physico-chemical and biological evaluations, was followed by a DLP processing parametric study for each material. The impact of the number of acrylate groups per polymer (2 to 6) on the physico-chemical properties was pronounced, as reflected by a reduced swelling, lower water contact angles, accelerated crosslinking kinetics, and increased Young's moduli upon increasing the acrylate content. Furthermore, the different polymer backbones also exerted a substantial effect on the properties, including the absence of crystallinity, remarkably reduced swelling behaviors, a slight reduction in Young's modulus, and slower crosslinking kinetics for UPPG vs UPEG. The mechanical characteristics of DLP-printed samples showcased the ability to tailor the materials' stiffness (ranging from 0.4 to 5.3 MPa) by varying endcap chemistry and/or backbone. The in vitro cell assays confirmed biocompatibility of the material as such and the DLP-printed discs. Furthermore, the structural integrity of 3D scaffolds was preserved both in dry and swollen state. By adjusting the backbone chemistry or acrylate content, the post-swelling dimensions could be customized towards the targeted application. This study showcases the potential of these materials offering tailorable properties to serve many biomedical applications such as cartilage TE.
Topics: Acrylates; Polyethylene Glycols; Biocompatible Materials; Urethane; Tissue Engineering; Humans; Tissue Scaffolds; Light; Materials Testing; Polymers; Propylene Glycols; Polyurethanes
PubMed: 38875803
DOI: 10.1016/j.bioadv.2024.213923 -
ACS Applied Materials & Interfaces Jun 2024Hierarchically structural particles (HSPs) are highly regarded as favorable nanomaterials for superhydrophobic coating due to their special multiscale structure and...
Polymerization-Induced Hierarchical Hybrid Particles from Siloxane Emulsification Endowing Polyurethane Composite Coating with Superhydrophobicity, Thermal Insulation, and Fluorescence.
Hierarchically structural particles (HSPs) are highly regarded as favorable nanomaterials for superhydrophobic coating due to their special multiscale structure and surface physicochemical properties. However, most of the superhydrophobic coatings constructed from HSPs are monofunctional, constraining their broader applications. Moreover, traditional methods for constructing HSPs mostly rely on complicated chemical routes and template removal. Herein, we propose an innovative strategy (one-pot method) for producing multifunctional hierarchical hybrid particles (HHPs). Polysilsesquioxane (PSQ), generated from hydrolysis condensation of methyltriethoxylsilane, is used as the sole stabilizer to anchor on the surface of styrene and short fluoroalkyl compound tridecafluorooctyl acrylate comonomers droplets, forming a mesoporous PSQ shell. Subsequently, the comonomers inside of the shell perform restricted polymerization to generate the HHP due to the driving of the mesoporous capillary force. The HHP is then mixed with waterborne polyurethane (WPU) to develop a robust nanocomposite coating (WPU-HHP). Through the deliberate design of the HHP components, the WPU-HHP coating has thermal insulation, photoluminescence properties, and the ability to achieve a wettability transition during abrasion. Our research has achieved the integration of multifunctionality in one waterborne hybrid system, broadening the application areas of nanocomposite coatings.
PubMed: 38875477
DOI: 10.1021/acsami.4c04224 -
Technology and Health Care : Official... May 2024The biological properties of silicone elastomers such as polydimethylsiloxane (PDMS) have widespread use in biomedicine for soft tissue implants, contact lenses, soft...
BACKGROUND
The biological properties of silicone elastomers such as polydimethylsiloxane (PDMS) have widespread use in biomedicine for soft tissue implants, contact lenses, soft robots, and many other small medical devices, due to its exceptional biocompatibility. Additive manufacturing of soft materials still has significant challenges even with major advancements that have occurred in development of these technologies for customized medical devices and tissue engineering.
OBJECTIVE
The aim of this study was to develop a mathematical model of tangential stress in relation to shear stress, shear rate, 3D printing pressure and velocity, for non-Newtonian gels and fluids that are used as materials for 3D printing.
METHOD
This study used FENE (finitely extensible nonlinear elastic model) model, for non-Newtonian gels and fluids to define the dependences between tangential stress, velocity, and pressure, considering viscosity, shear stress and shear rates as governing factors in soft materials friction and adhesion. Experimental samples were fabricated as showcases, by SLA and FDM 3D printing technologies: elastic polymer samples with properties resembling elastic properties of PDMS and thermoplastic polyurethane (TPU) samples. Experimental 3D printing parameters were used in the developed analytical solution to analyse the relationships between governing influential factors (tangential stress, printing pressure, printing speed, shear rate and friction coefficient). Maple software was used for numerical modelling.
RESULTS
Analytical model applied on a printed elastic polymer, at low shear rates, exhibited numerical values of tangential stress of 0.208-0.216 N m - 2 at printing velocities of 0.9 to 1.2 mm s - 1, while the coefficient of friction was as low as 0.09-0.16. These values were in accordance with experimental data in literature. Printing pressure did not significantly influence tangential stress, whereas it was slightly influenced by shear rate changes. Friction coefficient linearly increased with tangential stress.
CONCLUSION
Simple analytical model of friction for elastic polymer in SLA 3D printing showed good correspondence with experimental literature data for low shear rates, thus indicating possibility to use it for prediction of printing parameters towards desired dimensional accuracy of printed objects. Further development of this analytical model should enable other shear rate regimes, as well as additional soft materials and printing parameters.
PubMed: 38875063
DOI: 10.3233/THC-240209 -
Bioactive Materials Oct 2024Previous studies have confirmed that intervertebral disc degeneration (IDD) is closely associated with inflammation-induced reactive oxygen species (ROS) and resultant...
Previous studies have confirmed that intervertebral disc degeneration (IDD) is closely associated with inflammation-induced reactive oxygen species (ROS) and resultant cell mitochondrial membrane potential (MMP) decline. Clearance of ROS in an inflammatory environment is essential for breaking the vicious cycle of MMP decline. Additionally, re-energizing the mitochondria damaged in the inflammatory milieu to restore their function, is equally important. Herein, we proposed an interesting concept of mitochondrion-engine equipped with coolant, which enables first to "cool-down" the inflammatory environment, next to restore the MMP, finally to allow cells to regain normal energy metabolism through materials design. As such, we developed a multi-functional composite composed of a reactive oxygen species (ROS)-responsive sodium alginate/gelatin hydrogel infused into a rigid 3D-printed thermoplastic polyurethane (TPU) scaffold. The TPU scaffold was coated with conductive polypyrrole (PPy) to electrophoretically deposit l-arginine, which could upregulate the Mammalian target of rapamycin () pathway, thus increasing MMP and energy metabolism to stimulate extracellular matrix synthesis for IVD repair. While the ROS-responsive hydrogel acting as the "mito-engine coolant" could scavenge the excessive ROS to create a favorable environment for IVD cells recovery. Demonstrated by and evaluations, the mito-engine system markedly promoted the proliferation and collagen synthesis of nucleus pulposus cells while enhancing the mitochondrial respiration and MMP under oxidative stress. Radiological and histological assessments revealed the efficacy of this system in IVD repair. This unique bioinspired design integrated biomaterial science with mitochondrial biology, presents a promising paradigm for IDD treatment.
PubMed: 38873262
DOI: 10.1016/j.bioactmat.2024.05.044 -
Journal of Colloid and Interface Science Jun 2024Electrically conductive fiberfibre/fabric composites (ECFCs) are competitive candidates for use in wearable electronics. Therefore, it is essential to develop...
Electrically conductive fiberfibre/fabric composites (ECFCs) are competitive candidates for use in wearable electronics. Therefore, it is essential to develop mechanically robust ECFC strain sensors with sensing performance. In this study, MXene assembly and hot-pressing were combined to prepare strong yet breathable ECFCs for strain and temperature sensing. Hydrogen bonding between MXene and polyurethane (PU) and ultrasonication-induced interfacial sintering were responsible for MXene nanosheets assembly on the PU nanofibers. MXene decoration made PU nanofibers electrically conductive, resulting in a conductive network. Hot-pressing improved interface adhesion among the conductive nanofibers. Thus, the mechanical properties of the nanofiber composites, including tensile strength, toughness and fracture energy, were enhanced. The nanofiber composites exhibited surface stability and durability. When the nanofiber composites were used as strain sensors, they showed breathability with a linear resistance response ranging from 1 % to 100 % and cycling stability. In addition, they produced stable sensing signals over 1000 cycles when a notch was present. They could also monitor temperature variations with a negative temperature coefficient (-0.146 %/°C). This study provides an interfacial regulation method for the preparation of multi-functional nanofiber composites with potential applications in flexible and wearable electronics.
PubMed: 38871626
DOI: 10.1016/j.jcis.2024.06.045 -
The Journal of Craniofacial Surgery Jun 2024Surgical simulation has been used extensively for learning microtia reconstruction and has almost exclusively involved framework creation. However, soft tissue...
Surgical simulation has been used extensively for learning microtia reconstruction and has almost exclusively involved framework creation. However, soft tissue reconstruction in microtia is equally challenging and would benefit from a simulation platform. This study aimed to describe the development and preliminary evaluation of a high-fidelity soft tissue microtia simulator. Three-dimensional modeling software, fused deposition 3-dimensional printing, adhesive techniques, silicones, and polyurethane rubbers were utilized to create a right lobular-type microtia simulator that comprises skin, subcutaneous tissue, and cartilage. Two expert microtia surgeons performed a microtia reconstruction on the simulator and evaluated its value and realism using a Likert-type questionnaire. The surgeons utilized a previously developed synthetic framework and successfully performed the critical steps of the soft tissue reconstruction, including marking, incising, dissection, removal of the cartilage remnant, drain insertion, insertion of the framework, closing of the skin, and demonstration of the soft tissue conforming over the framework using suction. A preliminary assessment of the simulator demonstrated that the simulator is anatomically accurate, realistic, and highly valuable as a training tool. A high-fidelity soft tissue microtia simulator was successfully developed and tested. The simulator provides a valuable training platform for learning a critical component of microtia reconstruction.
PubMed: 38869279
DOI: 10.1097/SCS.0000000000010322 -
Materials Horizons Jun 2024Future electronics call for materials with mechanical toughness, flexibility, and stretchability. Moreover, self-healing and recyclability are highly desirable to...
Future electronics call for materials with mechanical toughness, flexibility, and stretchability. Moreover, self-healing and recyclability are highly desirable to mitigate the escalating environmental threat of electronic waste (e-waste). Herein, we report a stretchable, self-healing, and recyclable material based on a mixture of the conductive polymer poly(3,4-ethylenedioxythiophene) doped with polystyrene sulfonate (PEDOT:PSS) with a custom-designed polyurethane (PU) and polyethylene glycol (PEG). This material showed excellent elongation at brake (∼350%), high toughness (∼24.6 MJ m), moderate electrical conductivity (∼10 S cm), and outstanding mechanical and electrical healing efficiencies. In addition, it demonstrated exceptional recyclability with no significant loss in the mechanical and electrical properties after being recycled 20 times. Based on these properties, as a proof of principle for sustainable electronic devices, we demonstrated that electrocardiogram (ECG) electrodes and pressure sensors based on this material could be recycled without significant performance loss. The development of multifunctional electronic materials that are self-healing and fully recyclable is a promising step toward sustainable electronics, offering a potential solution to the e-waste challenge.
PubMed: 38869226
DOI: 10.1039/d4mh00203b -
Journal of Dental Research Jun 2024The water-rich nature of the dentin bonding microenvironment, coupled with the stresses on the bonding interface, contributes to the hydrolytic degradation of the hybrid...
The water-rich nature of the dentin bonding microenvironment, coupled with the stresses on the bonding interface, contributes to the hydrolytic degradation of the hybrid layer, resulting in a decline in bonding durability and, ultimately, restoration failure. Currently, the 3-step etch-and-rinse technique remains the gold standard for dentin bonding, and the bonding mechanism mainly involves a physical interaction with little chemical bonding. In this study, we have developed a siloxane-modified polyurethane monomer (SPU) with acrylate and siloxane modifications that chemically binds to both collagen and hydroxyapatite in dentin. Formulated as a bisphenol A-glycidyl methacrylate alternative, the SPU monomer-based adhesive was designed to improve dentin bonding quality and durability. Attenuated total reflection Fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscope, and hydroxyproline release assays were performed on SPU-treated collagen, hydroxyapatite, and acid-etched dentin slices to dentin. The physicochemical properties of the configured SPU adhesives were profiled for polymerization behavior, water contact angle, and tensile strain and strength. The bonding effectiveness was assessed through micro-tensile strength, nano-leakage tests conducted on the bonded samples before and after thermal cycle aging. Finally, we further conducted in vivo and in vitro experiments to assess the biocompatibility of adhesives. The results showed that the siloxane groups of SPU monomer could covalently bind to dentin collagen and hydroxyapatite. The incorporation of SPU in the adhesive led to a significant increase in adhesive polymerization ( < 0.05) and tensile strain at break up to 134.11%. Furthermore, the SPU adhesive significantly improved dentin bond strength ( < 0.05), reduced interfacial nano-leakage ( < 0.05), and displayed good biocompatibility. In conclusion, the application of SPU, which achieves dual chemical bonding with dentin, can improve the quality of the hybrid layer, buffer the interfacial stresses, enhance the interfacial resistance to hydrolysis, and provide a feasible strategy to extend the service life of adhesive restorations.
PubMed: 38867655
DOI: 10.1177/00220345241253526