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1.
Int J Mol Sci ; 25(15)2024 Aug 01.
Article in English | MEDLINE | ID: mdl-39125977

ABSTRACT

This study aimed to synthesize a novel elastomeric ligature with dimethylaminohexadecyl methacrylate (DMAHDM) grafted, providing a new strategy for improving the issue of enamel demineralization during fixed orthodontics. DMAHDM was incorporated into elastomeric ligatures at different mass fractions using ultraviolet photochemical grafting. The antibacterial properties were evaluated and the optimal DMAHDM amount was determined based on cytotoxicity assays. Moreover, tests were conducted to evaluate the in vivo changes in the mechanical properties of the elastomeric ligatures. To assess the actual in vivo effectiveness in preventing enamel demineralization, a rat demineralization model was established, with analyses focusing on changes in surface microstructure, elemental composition, and nanomechanical properties. Elastomeric ligatures with 2% DMAHDM showed excellent biocompatibility and the best antibacterial properties, reducing lactic acid production by 65.3% and biofilm bacteria by 50.0% within 24 h, without significant mechanical property differences from the control group (p > 0.05). Most importantly, they effectively prevented enamel demineralization in vivo, enhancing elastic modulus by 73.2% and hardness by 204.8%. Elastomeric ligatures incorporating DMAHDM have shown great potential for application in preventing enamel demineralization, providing a new strategy to solve this issue during fixed orthodontics.


Subject(s)
Dental Enamel , Elastomers , Tooth Demineralization , Tooth Demineralization/prevention & control , Animals , Elastomers/chemistry , Rats , Dental Enamel/drug effects , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Methacrylates/chemistry , Methacrylates/pharmacology , Orthodontic Appliances , Biofilms/drug effects , Male
2.
Int J Biol Macromol ; 275(Pt 1): 133621, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38960248

ABSTRACT

Plant fiber-reinforced polylactic acid (PLA) composites are extensively utilized in eco-friendly packaging, sports equipment, and various other applications due to their environmental benefits and cost-effectiveness. However, PLA suffers from brittleness and poor toughness, which restricts its use in scenarios demanding high toughness. To expand the application range of plant fiber-reinforced PLA-based composites and enhance their poor toughness, this study employed a two-step process involving wheat straw fiber (WF) to improve the interfacial compatibility between WF and PLA. Additionally, four elastomeric materials-poly (butylene adipate-co-terephthalate) (PBAT), poly (butylene succinate) (PBS), polycaprolactone (PCL), and polyhydroxyalkanoate (PHA)-were incorporated to achieve a mutual reactive interface enhancement and elastomeric toughening. The results demonstrated that Fe3+/TsWF/PLA/PBS exhibited a tensile strength, elongation at break, and impact strength of 34.01 MPa, 14.23 %, and 16.2 kJ/m2, respectively. These values represented a 2.4 %, 86.7 %, and 119 % increase compared to the unmodified composites. Scanning electron microscopy analysis revealed no fiber exposure in the cross-section, indicating excellent interfacial compatibility. Furthermore, X-ray diffraction and differential scanning calorimetry tests confirmed improvements in the crystalline properties of the composites. This work introduces a novel approach for preparing fiber-reinforced PLA-based composites with exceptional toughness and strength.


Subject(s)
Elastomers , Polyesters , Tensile Strength , Polyesters/chemistry , Elastomers/chemistry , Polymers/chemistry , Triticum/chemistry , Materials Testing , Butylene Glycols/chemistry
3.
Biomacromolecules ; 25(8): 5019-5027, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-38982931

ABSTRACT

Dielectric elastomers generate muscle-like electroactive actuation, which is applicable in soft machines, medical devices, etc. However, the actuation strain and energy density of most dielectric elastomers, in the absence of prestretch, have long been limited to ∼20% and ∼10 kJ m-3, respectively. Here, we report a dielectric elastomer with ZrO2 nanoparticles confined in nanodomains, which achieves an actuation strain >100% and an energy density of ∼150 kJ m-3 without prestretch. We decorate the surface of each nanoparticle with a layer of a diblock oligomer, poly(acrylic acid-b-styrene). The surface-decorated nanoparticles coassemble with a triblock copolymer elastomer, poly(styrene-b-(2-ethylhexyl acrylate)-b-styrene) during cosolvent casting. Consequently, the nanoparticles are confined in the polystyrene nanodomains, which results in a dielectric elastomer nanocomposite with a low modulus, high breakdown strength, and intense strain-hardening behavior. During the actuation, the nanocomposite avoids the snap-through instability that most elastomers would suffer and achieves a superior actuation performance.


Subject(s)
Elastomers , Polystyrenes , Zirconium , Elastomers/chemistry , Zirconium/chemistry , Polystyrenes/chemistry , Nanocomposites/chemistry , Nanoparticles/chemistry , Artificial Organs , Acrylic Resins/chemistry
4.
Int J Mol Sci ; 25(13)2024 Jun 26.
Article in English | MEDLINE | ID: mdl-39000090

ABSTRACT

The acidic byproducts of bacteria in plaque around orthodontic brackets contribute to white spot lesion (WSL) formation. Nitric oxide (NO) has antibacterial properties, hindering biofilm formation and inhibiting the growth of oral microbes. Materials that mimic NO release could prevent oral bacteria-related pathologies. This study aims to integrate S-nitroso-acetylpenicillamine (SNAP), a promising NO donor, into orthodontic elastomeric ligatures, apply an additional polymer coating, and evaluate the NO-release kinetics and antimicrobial activity against Streptococus mutans. SNAP was added to clear elastomeric chains (8 loops, 23 mm long) at three concentrations (50, 75, 100 mg/mL, and a control). Chains were then coated, via electrospinning, with additional polymer (Elastollan®) to aid in extending the NO release. NO flux was measured daily for 30 days. Samples with 75 mg/mL SNAP + Elastollan® were tested against S. mutans for inhibition of biofilm formation on and around the chain. SNAP was successfully integrated into ligatures at each concentration. Only the 75 mg/mL SNAP chains maintained their elasticity. After polymer coating, samples exhibited a significant burst of NO on the first day, exceeding the machine's reading capacity, which gradually decreased over 29 days. Ligatures also inhibited S. mutans growth and biofilm formation. Future research will assess their mechanical properties and cytotoxicity. This study presents a novel strategy to address white spot lesion (WSL) formation and bacterial-related pathologies by utilizing nitric oxide-releasing materials. Manufactured chains with antimicrobial properties provide a promising solution for orthodontic challenges, showing significant potential for academic-industrial collaboration and commercial viability.


Subject(s)
Biofilms , Elastomers , Nitric Oxide , Streptococcus mutans , Streptococcus mutans/drug effects , Streptococcus mutans/growth & development , Elastomers/chemistry , Nitric Oxide/chemistry , Nitric Oxide/metabolism , Biofilms/drug effects , S-Nitroso-N-Acetylpenicillamine/pharmacology , S-Nitroso-N-Acetylpenicillamine/chemistry , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/chemical synthesis , Orthodontic Brackets/microbiology , Microbial Sensitivity Tests , Anti-Infective Agents/pharmacology , Anti-Infective Agents/chemistry , Anti-Infective Agents/chemical synthesis , Nitric Oxide Donors/pharmacology , Nitric Oxide Donors/chemistry , Nitric Oxide Donors/chemical synthesis , Humans
5.
Drug Discov Ther ; 18(3): 188-193, 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38880603

ABSTRACT

Wheelchair cushions are recommended to be used with wheelchair and can protect the buttocks from pain and injury by relieving interface pressure for wheelchair users. However, further investigations are required for proper use in response to the development of new types of wheelchair cushions. The objective of this study was to evaluate physical characteristics of wheelchair cushions by comparing pressure redistributing effects of four types of cushions. The participants were 16 healthy adults who consented to participate in this study. A pressure mapping system (CONFORMat, Nitta Corp.) was used for the measurements. Pressure at ischium was measured immediately after the stabilization of the sitting posture and 10 minutes after. The pressure at ischium significantly decreased with any wheelchair cushions (P < 0.01). A significant negative correlation between body mass index and pressure at ischium was observed without a wheelchair cushion (r = - 0.70), however, the correlation disappeared upon use of a wheelchair cushion. The pressure at ischium increased over time with cushions of urethane, air, and urethane-air hybrid while that with the 3D thermoplastic elastomer cushion did not, and the change in the pressure was statistically less than that in other cushions (P < 0.01). Use of wheelchair cushions was effective in redistribution of the pressure at ischium, and the overtime change in the pressure depends on the type of used cushions.


Subject(s)
Elastomers , Equipment Design , Ischium , Pressure , Wheelchairs , Humans , Adult , Elastomers/chemistry , Male , Female , Urethane/chemistry , Young Adult , Body Mass Index , Pressure Ulcer/prevention & control
6.
Sensors (Basel) ; 24(12)2024 Jun 11.
Article in English | MEDLINE | ID: mdl-38931570

ABSTRACT

Conventional passive ankle foot orthoses (AFOs) have not seen substantial advances or functional improvements for decades, failing to meet the demands of many stakeholders, especially the pediatric population with neurological disorders. Our objective is to develop the first comfortable and unobtrusive powered AFO for children with cerebral palsy (CP), the DE-AFO. CP is the most diagnosed neuromotor disorder in the pediatric population. The standard of care for ankle control dysfunction associated with CP, however, is an unmechanized, bulky, and uncomfortable L-shaped conventional AFO. These passive orthoses constrain the ankle's motion and often cause muscle disuse atrophy, skin damage, and adverse neural adaptations. While powered orthoses could enhance natural ankle motion, their reliance on bulky, noisy, and rigid actuators like DC motors limits their acceptability. Our innovation, the DE-AFO, emerged from insights gathered during customer discovery interviews with 185 stakeholders within the AFO ecosystem as part of the NSF I-Corps program. The DE-AFO is a biomimetic robot that employs artificial muscles made from an electro-active polymer called dielectric elastomers (DEs) to assist ankle movements in the sagittal planes. It incorporates a gait phase detection controller to synchronize the artificial muscles with natural gait cycles, mimicking the function of natural ankle muscles. This device is the first of its kind to utilize lightweight, compact, soft, and silent artificial muscles that contract longitudinally, addressing traditional actuated AFOs' limitations by enhancing the orthosis's natural feel, comfort, and acceptability. In this paper, we outline our design approach and describe the three main components of the DE-AFO: the artificial muscle technology, the finite state machine (the gait phase detection system), and its mechanical structure. To verify the feasibility of our design, we theoretically calculated if DE-AFO can provide the necessary ankle moment assistance for children with CP-aligning with moments observed in typically developing children. To this end, we calculated the ankle moment deficit in a child with CP when compared with the normative moment of seven typically developing children. Our results demonstrated that the DE-AFO can provide meaningful ankle moment assistance, providing up to 69% and 100% of the required assistive force during the pre-swing phase and swing period of gait, respectively.


Subject(s)
Ankle , Cerebral Palsy , Foot Orthoses , Robotics , Cerebral Palsy/physiopathology , Cerebral Palsy/rehabilitation , Humans , Child , Robotics/methods , Ankle/physiopathology , Ankle/physiology , Elastomers/chemistry , Gait/physiology , Equipment Design , Biomechanical Phenomena
7.
BMC Oral Health ; 24(1): 713, 2024 Jun 20.
Article in English | MEDLINE | ID: mdl-38902666

ABSTRACT

BACKGROUND: Low mechanical properties are the main limitation of glass ionomer cements (GICs). The incorporation of elastomeric micelles is expected to enhance the strength of GICs without detrimentally affecting their physical properties and biocompatibility. This study compared the chemical and mechanical properties, as well as the cytotoxicity, of elastomeric micelles-containing glass ionomer cement (DeltaFil, DT) with commonly used materials, including EQUIA Forte Fil (EF), Fuji IX GP Extra (F9), and Ketac Molar (KT). METHOD: Powder particles of GICs were examined with SEM-EDX. Setting kinetics were assessed using ATR-FTIR. Biaxial flexural strength/modulus and Vickers surface microhardness were measured after immersion in water for 24 h and 4 weeks. The release of F, Al, Sr, and P in water over 8 weeks was analyzed using a fluoride-specific electrode and ICP-OES. The toxicity of the material extract on mouse fibroblasts was also evaluated. RESULTS: High fluoride levels in the powder were detected with EF and F9. DT demonstrated an initial delay followed by a faster acid reaction compared to other cements, suggesting an improved snap set. DT also exhibited superior flexural strength than other materials at both 24 h and 4 weeks but lower surface microhardness (p < 0.05). EF and F9 showed higher release of F, Al, and P than DT and KT. There was no statistically significant difference in fibroblast viability among the tested materials (p > 0.05). CONCLUSIONS: Elastomeric micelles-containing glass ionomer cement (DT) exhibited satisfactory mechanical properties and cytocompatibility compared with other materials. DT could, therefore, potentially be considered an alternative high-strength GIC for load-bearing restorations.


Subject(s)
Elastomers , Fibroblasts , Flexural Strength , Glass Ionomer Cements , Hardness , Materials Testing , Micelles , Glass Ionomer Cements/toxicity , Glass Ionomer Cements/chemistry , Animals , Mice , Fibroblasts/drug effects , Elastomers/chemistry , Elastomers/toxicity , Aluminum/chemistry , Fluorides/chemistry , Strontium/chemistry , Polycarboxylate Cement/chemistry , Polycarboxylate Cement/toxicity , Cell Survival/drug effects , Microscopy, Electron, Scanning , Surface Properties , Pliability , Kinetics , Spectroscopy, Fourier Transform Infrared , Stress, Mechanical , Time Factors , Biocompatible Materials/chemistry
8.
Mater Horiz ; 11(16): 3911-3920, 2024 08 12.
Article in English | MEDLINE | ID: mdl-38836844

ABSTRACT

Expanding the detection information of wearable smart devices in applications has practical implications for their use in daily life and healthcare. Damage and breakage caused by mechanical injuries and continuous use are unavoidable for polymer matrices so self-healing properties are expected to be conferred on flexible sensors to extend their life and durability. In addition, a good linearity of relative resistance change vs. strain (gauge factor, GF) facilitates the streamlined conversion of electrical signals to 3D information of human motion, whereas existing works on sensors neglect the quantitative analysis of signals. This letter reports a self-healable flexible electronic sensor based on hydrogen bonding and electrostatic interaction between maleic acid-grafted natural rubber (MNR), polyaniline (PANI), and phytic acid (PA). MNR is the flexible matrix and the template for aniline (ANI) polymerization, and PA acts as the dopant and crosslinking agent. The MNR-PANI-PA sensor shows easy self-healing at room temperature, enhanced mechanical behaviour (∼2.5 MPa, 1000% strain), and excellent linearity (GF of 13.8 over 250% strain and GF of 32.0 over 250-100% strain). Due to the highly linear relationship between ΔR/R and bending angle, the electrical signals of human limb movement can output relevant information on bending angle and frequency. By constructing a sensing array, changes in the position and magnitude of applied pressure could also be detected in real-time. Based on these advantages, the MNR-PANI-PA composite sensor is expected to have potential applications in health monitoring, body motion detection, and electronic skins.


Subject(s)
Aniline Compounds , Elastomers , Movement , Wearable Electronic Devices , Humans , Elastomers/chemistry , Movement/physiology , Electric Conductivity , Pressure , Phytic Acid/chemistry , Rubber/chemistry , Maleates/chemistry
9.
J Mech Behav Biomed Mater ; 155: 106566, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38729087

ABSTRACT

The objective of this study is to develop a reliable tribological model to enable a more thorough investigation of the frictional behavior of fascia tissues connected to non-specific lower back pain. Several models were designed and evaluated based on their coefficient of friction, using a low-frequency, low-load reciprocating motion. The study found that two technical elastomers, layered on PDMS to simulate the fascia and underlying muscle, are suitable substitutes for biological tissue in the model. The influence of tribopair geometry was also examined, and the results showed that greater conformity of contact leads to a lower COF, regardless of the material combination used. Finally, the friction properties of HA of various molecular weights and concentrations were tested.


Subject(s)
Fascia , Friction , Materials Testing , Fascia/physiology , Dimethylpolysiloxanes/chemistry , Biomechanical Phenomena , Models, Biological , Elastomers/chemistry
10.
Int J Biol Macromol ; 268(Pt 2): 131946, 2024 May.
Article in English | MEDLINE | ID: mdl-38692545

ABSTRACT

The development of flexible wearable multifunctional electronics has gained great attention in the field of human motion monitoring. However, developing mechanically tough, highly stretchable, and recyclable composite conductive materials for application in multifunctional sensors remained great challenges. In this work, a mechanically tough, highly stretchable, and recyclable composite conductive elastomer with the dynamic physical-chemical dual-crosslinking network was fabricated by the combination of multiple hydrogen bonds and dynamic ester bonds. To prepare the proposed composite elastomers, the polyaniline-modified carboxylate cellulose nanocrystals (C-CNC@PANI) were used as both conductive filler to yield high conductivity of 15.08 mS/m, and mechanical reinforcement to construct the dynamic dual-crosslinking network with epoxidized natural rubber latex to realize the high mechanical strength (8.65 MPa) and toughness (29.57 MJ/m3). Meanwhile, the construction of dynamic dual-crosslinking network endowed the elastomer with satisfactory recyclability. Based on these features, the composite conductive elastomers were used as strain sensors, and electrode material for assembling flexible and recyclable self-powered sensors for monitoring human motions. Importantly, the composite conductive elastomers maintained reliable sensing and energy harvesting performance even after multiple recycling process. This study provides a new strategy for the preparation of recyclable, mechanically tough composite conductive materials for wearable sensors.


Subject(s)
Cellulose , Elastomers , Electric Conductivity , Rubber , Wearable Electronic Devices , Elastomers/chemistry , Cellulose/chemistry , Rubber/chemistry , Humans , Nanocomposites/chemistry , Nanoparticles/chemistry , Mechanical Phenomena , Aniline Compounds/chemistry
11.
ACS Appl Mater Interfaces ; 16(19): 25404-25414, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38692284

ABSTRACT

Liquid crystal elastomers (LCEs), as a classical two-way shape-memory material, are good candidates for developing artificial muscles that mimic the contraction, expansion, or rotational behavior of natural muscles. However, biomimicry is currently focused more on the actuation functions of natural muscles dominated by muscle fibers, whereas the tactile sensing functions that are dominated by neuronal receptors and synapses have not been well captured. Very few studies have reported the sensing concept for LCEs, but the signals were still donated by macroscopic actuation, that is, variations in angle or length. Herein, we develop a conductive porous LCE (CPLCE) using a solvent (dimethyl sulfoxide (DMSO))-templated photo-cross-linking strategy, followed by carbon nanotube (CNT) incorporation. The CPLCE has excellent reversible contraction/elongation behavior in a manner similar to the actuation functions of skeletal muscles. Moreover, the CPLCE shows excellent pressure-sensing performance by providing real-time electrical signals and is capable of microtouch sensing, which is very similar to natural tactile sensing. Furthermore, macroscopic actuation and tactile sensation can be integrated into a single system. Proof-of-concept studies reveal that the CPLCE-based artificial muscle is sensitive to external touch while maintaining its excellent actuation performance. The CPLCE with tactile sensation beyond reversible actuation is expected to benefit the development of versatile artificial muscles and intelligent robots.


Subject(s)
Elastomers , Liquid Crystals , Nanotubes, Carbon , Liquid Crystals/chemistry , Elastomers/chemistry , Nanotubes, Carbon/chemistry , Porosity , Solvents/chemistry , Touch/physiology , Artificial Organs , Muscle, Skeletal/physiology , Muscle, Skeletal/chemistry , Humans
12.
ACS Nano ; 18(22): 14558-14568, 2024 Jun 04.
Article in English | MEDLINE | ID: mdl-38761154

ABSTRACT

To propel electronic skin (e-skin) to the next level by integrating artificial intelligence features with advanced sensory capabilities, it is imperative to develop stretchable memory device technology. A stretchable memory device for e-skin must offer, in particular, long-term data storage while ensuring the security of personal information under any type of deformation. However, despite the significance of these needs, technology related to stretchable memory devices remains in its infancy. Here, we report an intrinsically stretchable floating gate (FG) polymer memory transistor. The device features a dual-stimuli (optical and electrical) writing system to prevent easy erasure of recorded data. An FG comprising an intermixture of Ag nanoparticles and elastomer and with proper energy-band alignment between the semiconductor and dielectric facilitated sustainable memory performance, while achieving a high memory on/off ratio (>105) and a long retention time (106 s) with the ability to withstand 50% uniaxial or 30% biaxial strain. In addition, our memory transistor exhibited high mechanical durability over multiple stretching cycles (1000 times), along with excellent environmental stability with respect to factors such as temperature, moisture, air, and delamination. Finally, we fabricated a 7 × 7 active-matrix memory transistor array for personalized storage of e-skin data and successfully demonstrated its functionality.


Subject(s)
Transistors, Electronic , Wearable Electronic Devices , Information Storage and Retrieval , Silver/chemistry , Humans , Elastomers/chemistry , Computer Storage Devices , Metal Nanoparticles/chemistry , Equipment Design
13.
ACS Appl Bio Mater ; 7(6): 3777-3785, 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38754861

ABSTRACT

Oral devices, such as foil-type devices, show great potential for the delivery of poorly permeable macromolecules by enabling unidirectional release of the loaded pharmaceutical composition in close proximity to the epithelium in the small intestine or colon. However, one of the primary concerns associated with the use of foil-type devices so far has been the utilization of nonbiodegradable elastomers in the fabrication of the devices. Therefore, research into biodegradable substitute materials with similar characteristics enables drug delivery in a sustainable and environmentally friendly manner. In this study, a biodegradable elastomer, polyoctanediol citrate (POC), was synthesized via a one-pot reaction, with subsequent purification and microscale pattern replication via casting. The microstructure geometry was designed to enable fabrication of foil-type devices with the selected elastomer, which has a high intrinsic surface free energy. The final elastomer was demonstrated to have an elastic modulus ranging up to 2.2 ± 0.1 MPa, with strain at failure up to 110.1 ± 1.5%. Devices were loaded with acetaminophen and enterically coated, demonstrating 100% release at 2.5 h, following dissolution for 1 h in 0.1 M hydrochloric acid and 1.5 h in pH 6.8 phosphate-buffered saline. The elastomer demonstrated promising properties based on mechanical testing, surface free energy evaluation, and degradation studies.


Subject(s)
Biocompatible Materials , Elastomers , Materials Testing , Particle Size , Elastomers/chemistry , Biocompatible Materials/chemistry , Biocompatible Materials/chemical synthesis , Drug Delivery Systems , Humans , Acetaminophen/chemistry , Acetaminophen/administration & dosage , Administration, Oral , Citrates/chemistry , Macromolecular Substances/chemistry , Macromolecular Substances/chemical synthesis , Polymers/chemistry
14.
Biomaterials ; 309: 122598, 2024 Sep.
Article in English | MEDLINE | ID: mdl-38696943

ABSTRACT

Current vascular grafts, primarily Gore-Tex® and Dacron®, don't integrate with the host and have low patency in small-diameter vessels (<6 mm). Biomaterials that possess appropriate viscoelasticity, compliance, and high biocompatibility are essential for their application in small blood vessels. We have developed metal ion crosslinked poly(propanediol-co-(hydroxyphenyl methylene)amino-propanediol sebacate) (M-PAS), a biodegradable elastomer with a wide range of mechanical properties. We call these materials metallo-elastomers. An initial test on Zn-, Fe-, and Cu-PAS grafts reveals that Cu-PAS is the most suitable because of its excellent elastic recoil and well-balanced polymer degradation/tissue regeneration rate. Here we report host remodeling of Cu-PAS vascular grafts in rats over one year. 76 % of the grafts remain patent and >90 % of the synthetic polymer is degraded by 12 months. Extensive cell infiltration leads to a positive host remodeling. The remodeled grafts feature a fully endothelialized lumen. Circumferentially organized smooth muscle cells, elastin fibers, and widespread mature collagen give the neoarteries mechanical properties similar to native arteries. Proteomic analysis further reveals the presence of important vascular proteins in the neoarteries. Evidence suggests that Cu-PAS is a promising material for engineering small blood vessels.


Subject(s)
Blood Vessel Prosthesis , Carotid Arteries , Elastomers , Animals , Elastomers/chemistry , Rats , Male , Biocompatible Materials/chemistry , Rats, Sprague-Dawley , Polymers/chemistry , Materials Testing
15.
Macromol Rapid Commun ; 45(13): e2400022, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38704741

ABSTRACT

The preparation of self-healing polyurethane elastomers (PUEs) incorporating dynamic bonds is of considerable practical significance. However, developing a PUE with outstanding mechanical properties and high self-healing efficiency poses a significant challenge. Herein, this work has successfully developed a series of self-healing PUEs with various outstanding properties through rational molecular design. These PUEs incorporate m-xylylene diisocyanate and reversible dimethylglyoxime as hard segment, along with polytetramethylene ether glycol as soft segment. A significant amount of dynamic oxime-carbamate and hydrogen bonds are formed in hard segment. The microphase separated structure of the PUEs enables them to be colorless with a transparency of >90%. Owing to the chemical composition and multiple dynamic interactions, the PUEs are endowed with ultra-high tensile strength of 34.5 MPa, satisfactory toughness of 53.9 MJ m-3, and great elastic recovery both at low and high strains. The movement of polymer molecular chains and the dynamic reversible interactions render a self-healing efficiency of 101% at 70 °C. In addition, this self-healing polyurethane could still maintain high mechanical properties after recycling. This study provides a design strategy for the preparation of a comprehensive polyurethane with superior overall performance, which holds wide application prospects in the fields of flexible displays and solar cells.


Subject(s)
Carbamates , Elastomers , Hydrogen Bonding , Oximes , Polyurethanes , Tensile Strength , Polyurethanes/chemistry , Oximes/chemistry , Elastomers/chemistry , Carbamates/chemistry , Molecular Structure , Elasticity
16.
Adv Mater ; 36(32): e2400241, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38780175

ABSTRACT

Biological organisms exhibit phenomenal adaptation through morphology-shifting mechanisms including self-amputation, regeneration, and collective behavior. For example, reptiles, crustaceans, and insects amputate their own appendages in response to threats. Temporary fusion between individuals enables collective behaviors, such as in ants that temporarily fuse to build bridges. The concept of morphological editing often involves the addition and subtraction of mass and can be linked to modular robotics, wherein synthetic body morphology may be revised by rearranging parts. This work describes a reversible cohesive interface made of thermoplastic elastomer that allows for strong attachment and easy detachment of distributed soft robot modules without direct human handling. The reversible joint boasts a modulus similar to materials commonly used in soft robotics, and can thus be distributed throughout soft robot bodies without introducing mechanical incongruities. To demonstrate utility, the reversible joint is implemented in two embodiments: a soft quadruped robot that self-amputates a limb when stuck, and a cluster of three soft-crawling robots that fuse to cross a land gap. This work points toward future robots capable of radical shape-shifting via changes in mass through autotomy and interfusion, as well as highlights the crucial role that interfacial stiffness change plays in autotomizable biological and artificial systems.


Subject(s)
Elastomers , Robotics , Elastomers/chemistry , Animals
17.
ACS Appl Mater Interfaces ; 16(15): 19480-19495, 2024 Apr 17.
Article in English | MEDLINE | ID: mdl-38581369

ABSTRACT

Light-driven soft actuators based on photoresponsive materials can be used to mimic biological motion, such as hand movements, without involving rigid or bulky electromechanical actuations. However, to our knowledge, no robust photoresponsive material with desireable mechanical and biological properties and relatively simple manufacture exists for robotics and biomedical applications. Herein, we report a new visible-light-responsive thermoplastic elastomer synthesized by introducing photoswitchable moieties (i.e., azobenzene derivatives) into the main chain of poly(ε-caprolactone) based polyurethane urea (PAzo). A PAzo elastomer exhibits controllable light-driven stiffness softening due to its unique nanophase structure in response to light, while possessing excellent hyperelasticity (stretchability of 575.2%, elastic modulus of 17.6 MPa, and strength of 44.0 MPa). A bilayer actuator consisting of PAzo and polyimide films is developed, demonstrating tunable bending modes by varying incident light intensities. Actuation mechanism via photothermal and photochemical coupling effects of a soft-hard nanophase is demonstrated through both experimental and theoretical analyses. We demonstrate an exemplar application of visible-light-controlled soft "fingers" playing a piano on a smartphone. The robustness of the PAzo elastomer and its scalability, in addition to its excellent biocompatibility, opens the door to the development of reproducible light-driven wearable/implantable actuators and lightweight soft robots for clinical applications.


Subject(s)
Elastomers , Robotics , Elastomers/chemistry , Polyurethanes , Urea
18.
Biomed Mater ; 19(3)2024 Apr 30.
Article in English | MEDLINE | ID: mdl-38636492

ABSTRACT

Three-dimensional (3D) printing has emerged as a transformative technology for tissue engineering, enabling the production of structures that closely emulate the intricate architecture and mechanical properties of native biological tissues. However, the fabrication of complex microstructures with high accuracy using biocompatible, degradable thermoplastic elastomers poses significant technical obstacles. This is primarily due to the inherent soft-matter nature of such materials, which complicates real-time control of micro-squeezing, resulting in low fidelity or even failure. In this study, we employ Poly (L-lactide-co-ϵ-caprolactone) (PLCL) as a model material and introduce a novel framework for high-precision 3D printing based on the material plasticization process. This approach significantly enhances the dynamic responsiveness of the start-stop transition during printing, thereby reducing harmful errors by up to 93%. Leveraging this enhanced material, we have efficiently fabricated arrays of multi-branched vascular scaffolds that exhibit exceptional morphological fidelity and possess elastic moduli that faithfully approximate the physiological modulus spectrum of native blood vessels, ranging from 2.5 to 45 MPa. The methodology we propose for the compatibilization and modification of elastomeric materials addresses the challenge of real-time precision control, representing a significant advancement in the domain of melt polymer 3D printing. This innovation holds considerable promise for the creation of detailed multi-branch vascular scaffolds and other sophisticated organotypic structures critical to advancing tissue engineering and regenerative medicine.


Subject(s)
Biocompatible Materials , Elastomers , Polyesters , Printing, Three-Dimensional , Tissue Engineering , Tissue Scaffolds , Elastomers/chemistry , Tissue Scaffolds/chemistry , Tissue Engineering/methods , Polyesters/chemistry , Biocompatible Materials/chemistry , Elastic Modulus , Materials Testing , Humans , Stress, Mechanical , Blood Vessels , Blood Vessel Prosthesis
19.
Adv Mater ; 36(27): e2400763, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38641927

ABSTRACT

Muscles featuring high frequency and high stroke linear actuation are essential for animals to achieve superior maneuverability, agility, and environmental adaptability. Artificial muscles are yet to match their biological counterparts, due to inferior actuation speed, magnitude, mode, or adaptability. Inspired by the hierarchical structure of natural muscles, artificial muscles are created that are powerful, responsive, robust, and adaptable. The artificial muscles consist of knots braided from 3D printed liquid crystal elastomer fibers and thin heating threads. The unique hierarchical, braided knot structure offers amplified linear stroke, force rate, and damage-tolerance, as verified by both numerical simulations and experiments. In particular, the square knotted artificial muscle shows reliable cycles of actuation at 1Hz in 3000m depth underwater. Potential application is demonstrated by propelling a model boat. Looking ahead, the knotted artificial muscles can empower novel biomedical devices and soft robots to explore various environments, from inside human body to the mysterious deep sea.


Subject(s)
Biomimetic Materials , Water , Biomimetic Materials/chemistry , Water/chemistry , Muscles , Printing, Three-Dimensional , Robotics , Artificial Organs , Animals , Elastomers/chemistry , Biomimetics/methods , Liquid Crystals/chemistry , Humans
20.
Macromol Rapid Commun ; 45(13): e2300709, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38577749

ABSTRACT

Photoresponsive liquid-crystalline elastomers (LCEs) are promising candidates for light-controlled soft actuators. Photoinduced stress/strain originates from the changes in mechanical properties after light irradiation. However, the correlation between the photoinduced mechanical performance and in-use conditions such as stress/strain states and polymer network properties (such as effective crosslink density and dangling chain density) remains unexplored for practical applications. Here, isometric photo-induced stress or isotonic strain is investigated at different operating strains or stresses, respectively, on LCEs with polymer network variations, produced by different amounts of solvent during polymerization. As the solvent volume increases, the moduli and photoinduced stresses decrease. However, the photo-induced strain, fracture strain, fracture stress, and viscosity increase. The optical response performance initially increases with the operating strain/stress, peaks at a higher actuation strain/stress, and then, decreases depending on the polymer network. The maximum work densities, which also depend on the operating stress, are in the range of ≈200-300 kJm-3. These findings, highlighting the significant variations in the mechanical performance with the operating stress/strain ranges and amount of solvent used in the synthesis, are critical for designing LCE-based mechanical devices.


Subject(s)
Elastomers , Liquid Crystals , Polymers , Elastomers/chemistry , Liquid Crystals/chemistry , Polymers/chemistry , Photochemical Processes , Light , Polymerization , Viscosity , Stress, Mechanical
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