Scholarly Works, Macromolecules Innovation Institute (MII)

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3D printing vending machine
(United States Patent and Trademark Office, 2016-08-16)
A vending machine for creating a three-dimensional object having an enclosure having an exterior and interior. The interior receives and houses at least one three-dimensional printer. An interface for accepting an instruction associated with an object to be printed and transmitting the instruction to the printer. A storage section for storing a printed object that provides access to the printed part but limits or prohibits access to the interior.
Ammonium Bisphosphonate Polymeric Magnetic Nanocomplexes for Platinum Anticancer Drug Delivery and Imaging with Potential Hyperthermia and Temperature-Dependent Drug Release
Zhang, Rui; Fellows, Benjamin; Pothayee, Nikorn; Hu, Nan; Pothayee, Nipon; Jo, Ami; Bohórquez, Ana C.; Rinaldi, Carlos; Mefford, Olin Thompson; Davis, Richey M.; Riffle, Judy S. (Hindawi, 2018-08-05)
Novel magnetite-ammonium bisphosphonate graft ionic copolymer nanocomplexes (MGICs) have been developed for potential drug delivery, magnetic resonance imaging, and hyperthermia applications. The complexes displayed relatively uniform sizes with narrow size distributions upon self-assembly in aqueous media, and their sizes were stable under simulated physiological conditions for at least 7 days. The anticancer drugs, cisplatin and carboplatin, were loaded into the complexes, and sustained release of both drugs was observed. The transverse NMR relaxivities (s) of the complexes were 244 s−1 (mM Fe)−1 which is fast compared to either the commercial T2-weighted MRI agent Feridex IV® or our previously reported magnetite-block ionomer complexes. Phantom MRI images of the complexes demonstrated excellent negative contrast effects of such complexes. Thus, the bisphosphonate-bearing MGICs could be promising candidates for dual drug delivery and magnetic resonance imaging. Moreover, the bisphosphonate MGICs generate heat under an alternating magnetic field of 30 kA·m−1 at 206 kHz. The temperature of the MGIC dispersion in deionized water increased from 37 to 41°C after exposure to the magnetic field for 10 minutes, corresponding to a specific absorption rate of 77.0 W·g−1. This suggests their potential as hyperthermia treatment agents as well as the possibility of temperature-dependent drug release, making MGICs more versatile in potential drug delivery applications.
Bioactive Cellulose Nanocrystal-Poly(epsilon-Caprolactone) Nanocomposites for Bone Tissue Engineering Applications
Hong, Jung Ki; Cooke, Shelley L.; Whittington, Abby R.; Roman, Maren (2021-02-25)
3D-printed bone scaffolds hold great promise for the individualized treatment of critical-size bone defects. Among the resorbable polymers available for use as 3D-printable scaffold materials, poly(epsilon-caprolactone) (PCL) has many benefits. However, its relatively low stiffness and lack of bioactivity limit its use in load-bearing bone scaffolds. This study tests the hypothesis that surface-oxidized cellulose nanocrystals (SO-CNCs), decorated with carboxyl groups, can act as multi-functional scaffold additives that (1) improve the mechanical properties of PCL and (2) induce biomineral formation upon PCL resorption. To this end, an in vitro biomineralization study was performed to assess the ability of SO-CNCs to induce the formation of calcium phosphate minerals. In addition, PCL nanocomposites containing different amounts of SO-CNCs (1, 2, 3, 5, and 10 wt%) were prepared using melt compounding extrusion and characterized in terms of Young's modulus, ultimate tensile strength, crystallinity, thermal transitions, and water contact angle. Neither sulfuric acid-hydrolyzed CNCs (SH-CNCs) nor SO-CNCs were toxic to MC3T3 preosteoblasts during a 24 h exposure at concentrations ranging from 0.25 to 3.0 mg/mL. SO-CNCs were more effective at inducing mineral formation than SH-CNCs in simulated body fluid (1x). An SO-CNC content of 10 wt% in the PCL matrix caused a more than 2-fold increase in Young's modulus (stiffness) and a more than 60% increase in ultimate tensile strength. The matrix glass transition and melting temperatures were not affected by the SO-CNCs but the crystallization temperature increased by about 5.5 degrees C upon addition of 10 wt% SO-CNCs, the matrix crystallinity decreased from about 43 to about 40%, and the water contact angle decreased from 87 to 82.6 degrees. The abilities of SO-CNCs to induce calcium phosphate mineral formation and increase the Young's modulus of PCL render them attractive for applications as multi-functional nanoscale additives in PCL-based bone scaffolds.
Biodegradable Poly(Lactic Acid) Nanocomposites for Fused Deposition Modeling 3D Printing
Bardot, Madison; Schulz, Michael D. (MDPI, 2020-12-21)
3D printing by fused deposition modelling (FDM) enables rapid prototyping and fabrication of parts with complex geometries. Unfortunately, most materials suitable for FDM 3D printing are non-degradable, petroleum-based polymers. The current ecological crisis caused by plastic waste has produced great interest in biodegradable materials for many applications, including 3D printing. Poly(lactic acid) (PLA), in particular, has been extensively investigated for FDM applications. However, most biodegradable polymers, including PLA, have insufficient mechanical properties for many applications. One approach to overcoming this challenge is to introduce additives that enhance the mechanical properties of PLA while maintaining FDM 3D printability. This review focuses on PLA-based nanocomposites with cellulose, metal-based nanoparticles, continuous fibers, carbon-based nanoparticles, or other additives. These additives impact both the physical properties and printability of the resulting nanocomposites. We also detail the optimal conditions for using these materials in FDM 3D printing. These approaches demonstrate the promise of developing nanocomposites that are both biodegradable and mechanically robust.
Bulk and interfacial interactions between hydroxypropyl-cellulose and bile salts: Impact on the digestion of emulsified lipids
Zornjak, Jennifer; Liu, Jianzhao; Esker, Alan R.; Lin, Tiantian; Fernández-Fraguas, Cristina (2020-09)
Hydroxypropyl-cellulose (HPC) is a surface-active, non-digestible polysaccharide, commonly used in food emulsions as thickener and/or emulsifier. Due to these dual characteristics, HPC is a potential ingredient to modulate lipid digestion. Since bile salts (BS) are key players during lipid digestion, the aim of this work was to investigate the impact that interactions of HPC with BS has on the digestion of emulsified lipids. We studied the effect of two BS species differing in bile-acid moiety, sodium-taurocholate (NaTC) and sodium-taurodeoxycholate (NaTDC). A Quartz-Crystal-Microbalance (QCM-D) was used to evaluate HPC-BS interfacial interactions during the sequential and simultaneous adsorption of both components at a hydrophobic surface, while microDifferential-Scanning-Calorimetry was used to examine bulk interactions. In vitro lipid digestion was studied by using a pH-stat method. Results showed that, under fed-state conditions, NaTDC micelles were more effective at displacing a pre-adsorbed HPC layer from the surface than NaTC monomers. Nevertheless, HPC was resistant to complete displacement by both BS. Additionally, HPC was more susceptible to interact with NaTDC in the bulk, compared to NaTC, which made the adsorption more competitive for NaTDC. The reduced amount of free NaTDC in solution could explain the delayed lipolysis shown by HPC-stabilized emulsions when NaTDC was used to simulate duodenal conditions. These findings show that the delay of lipid digestion by HPC is due to the combined effect of HPC-BS interfacial and bulk interactions, with BS-binding in solution mostly contributing to this effect, and the BS molecular and micellar structure playing essential roles on both situations.
Capillary forces on a small particle at a liquid-vapor interface: Theory and simulation
Tang, Yanfei; Cheng, Shengfeng (American Physical Society, 2018-09-24)
Continuous flow synthesis of a pharmaceutical intermediate: a computational fluid dynamics approach
Armstrong, Cameron T.; Pritchard, Cailean Q.; Cook, Daniel W.; Ibrahim, Mariam; Desai, Bimbisar K.; Whitham, Patrick J.; Marquardt, Brian J.; Chen, Yizheng; Zoueu, Jeremie T.; Bortner, Michael J.; Roper, Thomas D. (2019-03-01)
Continuous flow chemistry has the potential to greatly improve efficiency in the synthesis of active pharmaceutical ingredients (APIs); however, the optimization of these processes can be complicated by a large number of variables affecting reaction success. In this work, a screening design of experiments was used to compare computational fluid dynamics (CFD) simulations with experimental results. CFD simulations and experimental results both identified the reactor residence time and reactor temperature as the most significant factors affecting product yield for this reaction within the studied design space. A point-to-point comparison of the results showed absolute differences in product yield as low as 2.4% yield at low residence times and up to 19.1% yield at high residence times with strong correlation between predicted and experimental percent yields. CFD was found to underestimate the product yields at low residence times and overestimate at higher residence times. The correlation in predicted product yield and the agreement in identifying significant factors in reaction performance reveals the utility of CFD as a valuable tool in the design of continuous flow tube reactors with significantly reduced experimentation.
Control of Stratification in Drying Particle Suspensions via Temperature Gradients
Tang, Yanfei; Grest, Gary S.; Cheng, Shengfeng (2019-03-26)
A potential strategy for controlling stratification in a drying suspension of bidisperse particles is studied using molecular dynamics simulations. When the suspension is maintained at a constant temperature during fast drying, it can exhibit "small-on-top" stratification with an accumulation (depletion) of smaller (larger) particles in the top region of the drying film, consistent with the prediction of current theories based on diffusiophoresis. However, when only the region near the substrate is thermalized at a constant temperature, a negative temperature gradient develops in the suspension because of evaporative cooling at the liquid-vapor interface. Since the associated thermophoresis is stronger for larger nanoparticles, a higher fraction of larger nanoparticles migrate to the top of the drying film at fast evaporation rates. As a result, stratification is converted to "large-on-top". Very strong small-on-top stratification can be produced with a positive thermal gradient in the drying suspension. Here, we explore a way to produce a positive thermal gradient by thermalizing the vapor at a temperature higher than that of the solvent. Possible experimental approaches to realize various thermal gradients in a suspension undergoing solvent evaporation and thus to produce different stratification states in the drying film are suggested.
A critical review of the current knowledge regarding the biological impact of nanocellulose
Endes, Carola; Camarero-Espinosa, Sandra; Mueller, Silvana; Foster, Earl Johan; Petri-Fink, Alke; Rothen-Rutishauser, Barbara; Weder, Christoph; Clift, Martin James David (2016-12-01)
Several forms of nanocellulose, notably cellulose nanocrystals and nanofibrillated cellulose, exhibit attractive property matrices and are potentially useful for a large number of industrial applications. These include the paper and cardboard industry, use as reinforcing filler in polymer composites, basis for low-density foams, additive in adhesives and paints, as well as a wide variety of food, hygiene, cosmetic, and medical products. Although the commercial exploitation of nanocellulose has already commenced, little is known as to the potential biological impact of nanocellulose, particularly in its raw form. This review provides a comprehensive and critical review of the current state of knowledge of nanocellulose in this format. Overall, the data seems to suggest that when investigated under realistic doses and exposure scenarios, nanocellulose has a limited associated toxic potential, albeit certain forms of nanocellulose can be associated with more hazardous biological behavior due to their specific physical characteristics.
Development of Recyclable and High-Performance In Situ Hybrid TLCP/Glass Fiber Composites
Chen, Tianran; Kazerooni, Dana; Ju, Lin; Okonski, David A.; Baird, Donald G. (MDPI, 2020-08-24)
By combining the concepts of in situ thermotropic liquid crystalline polymer (TLCP) composites and conventional fiber composites, a recyclable and high-performance in situ hybrid polypropylene-based composite was successfully developed. The recycled hybrid composite was prepared by injection molding and grinding processes. Rheological and thermal analyses were utilized to optimize the processing temperature of the injection molding process to reduce the melt viscosity and minimize the degradation of polypropylene. The ideal temperature for blending the hybrid composite was found to be 305 °C. The influence of mechanical recycling on the different combinations of TLCP and glass fiber composites was analyzed. When the weight fraction ratio of TLCP to glass fiber was 2 to 1, the hybrid composite exhibited better processability, improved tensile performance, lower mechanical anisotropy, and greater recyclability compared to the polypropylene reinforced by either glass fiber or TLCP alone.
Double helical conformation and extreme rigidity in a rodlike polyelectrolyte
Wang, Ying; He, Yadong; Yu, Zhou; Gao, Jianwei; ten Brinck, Stephanie; Slebodnick, Carla; Fahs, Gregory B.; Zanelotti, Curt J.; Hegde, Maruti; Moore, Robert Bowen; Ensing, Bernd; Dingemans, Theo J.; Qiao, Rui; Madsen, Louis A. (Nature Publishing Group, 2019-02-18)
The ubiquitous biomacromolecule DNA has an axial rigidity persistence length of ~50 nm, driven by its elegant double helical structure. While double and multiple helix structures appear widely in nature, only rarely are these found in synthetic non-chiral macromolecules. Here we report a double helical conformation in the densely charged aromatic polyamide poly(2,2′-disulfonyl-4,4′-benzidine terephthalamide) or PBDT. This double helix macromolecule represents one of the most rigid simple molecular structures known, exhibiting an extremely high axial persistence length (~1 micrometer). We present X-ray diffraction, NMR spectroscopy, and molecular dynamics (MD) simulations that reveal and confirm the double helical conformation. The discovery of this extreme rigidity in combination with high charge density gives insight into the self-assembly of molecular ionic composites with high mechanical modulus (~ 1 GPa) yet with liquid-like ion motions inside, and provides fodder for formation of other 1D-reinforced composites. © 2019, The Author(s).
The effect of residual lignin on the rheological properties of cellulose nanofibril suspensions
Iglesias, Maria C.; Shivyari, Niloofar; Norris, Ann; Martin-Sampedro, Raquel; Eugenio, M. E.; Lahtinen, Panu; Auad, Maria L.; Elder, Thomas; Jiang, Zhihua; Frazier, Charles E.; Peresin, Maria S. (2020-10-10)
Although the removal of lignin and hemicelluloses from cellulose pulp to produce fully bleached cellulose nanofibrils (B-CNF) is the most common practice, the presence of residual lignin and hemicelluloses in raw materials for the production of lignin containing cellulose nanofibrils (LCNFs) holds several advantages. In this work, we investigated the effect of residual lignin inEucalyptus globuluscellulose fibers on the properties of the resulting LCNFs. The stability of the colloidal suspensions was assessed by zeta-potential values and charge density analyses. Morphology of the CNFs was studied using scanning electron microscopy and atomic force microscopy. Fibril diameter and diameter distributions for CNFs with different levels of residual lignin showed a decrease on fiber diameter as the lignin content increases. Differences in the chemical composition of the CNFs was evidenced as indicated in the Fourier-transform infrared spectroscopy spectra, particularly in fingerprint region. Thermal behavior of the CNFs was not altered by the presence of lignin, as indicated by thermogravimetric analysis. Finally, the rheological behavior of the samples was evaluated observing a gel-like behavior as well as an increase of the viscosity in LCNFs with higher lignin contents.
Elucidating the Potential Biological Impact of Cellulose Nanocrystals
Camarero-Espinosa, Sandra; Endes, Carola; Mueller, Silvana; Petri-Fink, Alke; Rothen-Rutishauser, Barbara; Weder, Christoph; Clift, Martin James David; Foster, Earl Johan (MDPI, 2016-07-08)
Cellulose nanocrystals exhibit an interesting combination of mechanical properties and physical characteristics, which make them potentially useful for a wide range of consumer applications. However, as the usage of these bio-based nanofibers increases, a greater understanding of human exposure addressing their potential health issues should be gained. The aim of this perspective is to highlight how knowledge obtained from studying the biological impact of other nanomaterials can provide a basis for future research strategies to deduce the possible human health risks posed by cellulose nanocrystals.
Exceptional capacitive deionization rate and capacity by block copolymer–based porous carbon fibers
Liu, Tianyu; Serrano, Joel; Elliott, John; Yang, Xiaozhou; Cathcart, William; Wang, Zixuan; He, Zhen; Liu, Guoliang (American Association for the Advancement of Science, 2020-04-17)
Capacitive deionization (CDI) is energetically favorable for desalinating low-salinity water. The bottlenecks of current carbon-based CDI materials are their limited desalination capacities and time-consuming cycles, caused by insufficient ion-accessible surfaces and retarded electron/ion transport. Here, we demonstrate porous carbon fibers (PCFs) derived from microphase-separated poly(methyl methacrylate)-block-polyacrylonitrile (PMMA-b-PAN) as an effective CDI material. PCF has abundant and uniform mesopores that are interconnected with micropores. This hierarchical porous structure renders PCF a large ion-accessible surface area and a high desalination capacity. In addition, the continuous carbon fibers and interconnected porous network enable fast electron/ion transport, and hence a high desalination rate. PCF shows desalination capacity of 30 mgNaCl g⁻¹ PCF and maximal time-average desalination rate of 38.0 mgNaCl g⁻¹ PCF min⁻¹, which are about 3 and 40 times, respectively, those of typical porous carbons. Our work underlines the promise of block copolymer–based PCF for mutually high-capacity and high-rate CDI.
Fabrication and characterization of PLGA nanoparticles encapsulating large CRISPR–Cas9 plasmid
Jo, Ami; Ringel-Scaia, Veronica M.; McDaniel, Dylan K.; Thomas, Cassidy A.; Zhang, Rui; Riffle, Judy S.; Allen, Irving C.; Davis, Richey M. (2020-01-20)
Background The clustered regularly interspaced short palindromic repeats (CRISPR) and Cas9 protein system is a revolutionary tool for gene therapy. Despite promising reports of the utility of CRISPR–Cas9 for in vivo gene editing, a principal problem in implementing this new process is delivery of high molecular weight DNA into cells. Results Using poly(lactic-co-glycolic acid) (PLGA), a nanoparticle carrier was designed to deliver a model CRISPR–Cas9 plasmid into primary bone marrow derived macrophages. The engineered PLGA-based carriers were approximately 160 nm and fluorescently labeled by encapsulation of the fluorophore 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene). An amine-end capped PLGA encapsulated 1.6 wt% DNA, with an encapsulation efficiency of 80%. Release studies revealed that most of the DNA was released within the first 24 h and corresponded to ~ 2–3 plasmid copies released per nanoparticle. In vitro experiments conducted with murine bone marrow derived macrophages demonstrated that after 24 h of treatment with the PLGA-encapsulated CRISPR plasmids, the majority of cells were positive for TIPS pentacene and the protein Cas9 was detectable within the cells. Conclusions In this work, plasmids for the CRISPR–Cas9 system were encapsulated in nanoparticles comprised of PLGA and were shown to induce expression of bacterial Cas9 in murine bone marrow derived macrophages in vitro. These results suggest that this nanoparticle-based plasmid delivery method can be effective for future in vivo applications of the CRISPR–Cas9 system.
Folic Acid-Conjugated Cellulose Nanocrystals Show High Folate-Receptor Binding Affinity and Uptake by KB and Breast Cancer Cells
Bittleman, Katelyn Rose; Dong, Shuping; Roman, Maren; Lee, Yong Woo (American Chemical Society, 2018-10-24)
The study evaluates cellulose nanocrystals (CNCs) as nanocarriers for targeted, intracellular delivery of molecular agents. CNCs were labeled with fluorescein-5′-isothiocyanate as an imaging agent and conjugated to folic acid (FA) as a targeting ligand. The CNC conjugates were characterized by UV–vis spectroscopy, ζ-potential analysis, dynamic light scattering, and atomic force microscopy. Cellular binding/uptake of the FA-conjugated CNCs by KB and MDA-MB-468 cells was quantified with cellular uptake assays. Internalization of the particles was confirmed by confocal microscopy. Uptake mechanisms were determined by inhibition studies with chlorpromazine and genistein. Binding affinity was qualitatively assessed with a free folate inhibition assay. Both KB and MDA-MB-468 cells exhibited significant and folate-receptor specific binding/uptake of FA-conjugated CNCs. Clathrin-mediated endocytosis was a significant uptake mechanism in both cell types, whereas caveolae-mediated endocytosis only played a significant role in MDA-MB-468 cells. Uptake inhibition of FA-conjugated CNCs by KB cells required high concentrations (>1 mM) of free FA. The observed FR-specific internalization of FA-conjugated CNCs by FR-positive cancer cells and tumors and their remarkable high affinity for the FR demonstrate the great potential of CNCs as novel nanocarriers for imaging agents and chemotherapeutics in the early detection and treatment of cancer.
Functionalized Cellulose Nanocrystal Nanocomposite Membranes with Controlled Interfacial Transport for Improved Reverse Osmosis Performance
Smith, Ethan D.; Hendren, Keith D.; Haag, James; Foster, Earl Johan; Martin, Stephen M. (MDPI, 2019-01-20)
Thin-film nanocomposite membranes (TFNs) are a recent class of materials that use nanoparticles to provide improvements over traditional thin-film composite (TFC) reverse osmosis membranes by addressing various design challenges, e.g., low flux for brackish water sources, biofouling, etc. In this study, TFNs were produced using as-received cellulose nanocrystals (CNCs) and 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanocrystals (TOCNs) as nanoparticle additives. Cellulose nanocrystals are broadly interesting due to their high aspect ratios, low cost, sustainability, and potential for surface modification. Two methods of membrane fabrication were used in order to study the effects of nanoparticle dispersion on membrane flux and salt rejection: a vacuum filtration method and a monomer dispersion method. In both cases, various quantities of CNCs and TOCNs were incorporated into a polyamide TFC membrane via in-situ interfacial polymerization. The flux and rejection performance of the resulting membranes was evaluated, and the membranes were characterized via attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), transmission electron microscopy (TEM), and atomic force microscopy (AFM). The vacuum filtration method resulted in inconsistent TFN formation with poor nanocrystal dispersion in the polymer. In contrast, the dispersion method resulted in more consistent TFN formation with improvements in both water flux and salt rejection observed. The best improvement was obtained via the monomer dispersion method at 0.5 wt% TOCN loading resulting in a 260% increase in water flux and an increase in salt rejection to 98.98 ± 0.41% compared to 97.53 ± 0.31% for the plain polyamide membrane. The increased flux is attributed to the formation of nanochannels at the interface between the high aspect ratio nanocrystals and the polyamide matrix. These nanochannels serve as rapid transport pathways through the membrane, and can be used to tune selectivity via control of particle/polymer interactions.
Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting
Frost, Brody A.; Sutliff, Bradley P.; Thayer, Patrick; Bortner, Michael J.; Foster, Earl Johan (2019-10-18)
Bioprinting has advanced drastically in the last decade, leading to many new biomedical applications for tissue engineering and regenerative medicine. However, there are still a myriad of challenges to overcome, with vast amounts of research going into bioprinter technology, biomaterials, cell sources, vascularization, innervation, maturation, and complex 4D functionalization. Currently, stereolithographic bioprinting is the primary technique for polymer resin bioinks. However, it lacks the ability to print multiple cell types and multiple materials, control directionality of materials, and place fillers, cells, and other biological components in specific locations among the scaffolds. This study sought to create bioinks from a typical polymer resin, poly(ethylene glycol) diacrylate (PEGDA), for use in extrusion bioprinting to fabricate gradient scaffolds for complex tissue engineering applications. Bioinks were created by adding cellulose nanocrystals (CNCs) into the PEGDA resin at ratios from 95/5 to 60/40 w/w PEGDA/CNCs, in order to reach the viscosities needed for extrusion printing. The bioinks were cast, as well as printed into single-material and multiple-material (gradient) scaffolds using a CELLINK BIOX printer, and crosslinked using lithium phenyl-2,4,6-trimethylbenzoylphosphinate as the photoinitiator. Thermal and mechanical characterizations were performed on the bioinks and scaffolds using thermogravimetric analysis, rheology, and dynamic mechanical analysis. The 95/5 w/w composition lacked the required viscosity to print, while the 60/40 w/w composition displayed extreme brittleness after crosslinking, making both CNC compositions non-ideal. Therefore, only the bioink compositions of 90/10, 80/20, and 70/30 w/w were used to produce gradient scaffolds. The gradient scaffolds were printed successfully and embodied unique mechanical properties, utilizing the benefits of each composition to increase mechanical properties of the scaffold as a whole. The bioinks and gradient scaffolds successfully demonstrated tunability of their mechanical properties by varying CNC content within the bioink composition and the compositions used in the gradient scaffolds. Although stereolithographic bioprinting currently dominates the printing of PEGDA resins, extrusion bioprinting will allow for controlled directionality, cell placement, and increased complexity of materials and cell types, improving the reliability and functionality of the scaffolds for tissue engineering applications.
Homogeneous nanodiscs of native membranes formed by stilbene-maleic-acid copolymers
Esmaili, Mansoore; Brown, Chanelle J.; Shaykhutdinov, Rustem; Acevedo-Morantes, Claudia; Wang, Yong Liang; Wille, Holger; Gandour, Richard D.; Turner, S. Richard; Overduin, Michael (2020-08-28)
Methylstilbene-alt-maleic acid copolymers spontaneously convert biological membranes into bilayer discs with similar to 20 nm diameters. This readily functionalizable class of copolymers has the compositional homogeneity, hydrophobicity, dynamics, and charge that may help to achieve optimal structural resolution, membrane dissolution, stability, and broad utility.
Imidazole-containing triblock copolymers with a synergy of ether and imidazolium sites
Jangu, Chainika; Wang, Jing-Han Helen; Wang, Dong; Fahs, Gregory B.; Heflin, James R.; Moore, Robert Bowen; Colby, Ralph H.; Long, Timothy E. (The Royal Society of Chemistry, 2015-03-06)
Reversible addition-fragmentation chain transfer (RAFT) polymerization enabled the synthesis of well-defined A-BC-A triblock copolymers containing a synergy of pendant ether and imidazolium sites. The soft central BC block comprises low Tg di(ethylene glycol) methyl ether methacrylate (DEGMEMA) and 1-(4-vinylbenzyl) methyl imidazolium units. External polystyrene blocks provide mechanical reinforcement within a nanoscale morphology. Dynamic mechanical analysis (DMA) of the A-BC-A triblock copolymers exhibited a plateau region, which suggested the formation of a microphase-separated morphology. Atomic force microscopy (AFM) and small angle X-ray scattering (SAXS) collectively probed the morphology of the A-BC-A triblock copolymers, revealing long-range order at the nanoscale dimensions. Dielectric relaxation spectroscopy (DRS) examined the ion-transport properties of ionomeric A-BC-A triblock copolymers and random copolymers with different compositions. The role of morphology was demonstrated with block copolymer nanoscale structures providing superior ionic conductivity and mechanical performance compared to random copolymers. Under a 4 V direct current (DC) applied voltage, electromechanical transducers derived from these triblock copolymer membranes with added ionic liquid showed superior actuation performance compared to a benchmark Nafion[registered sign] membrane, suggesting potential for ionic polymer device applications. This was attributed to optimum modulus, improved ionic conductivity, and microphase-separated morphology of triblock copolymers.

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