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    Stereoselective Stabilization of Polymeric Vitamin E Conjugate Micelles.
    Biomacromolecules 2017 Nov 17. Epub 2017 Nov 17.
    Vitamin E (α-tocopherol) (TPGS) micelle is a robust nanocarrier in delivering hydrophobic active pharmaceutical ingredients, but is suffering from poor stability that is essential in terms of pharmaceutical and biomedical applications. Taking advantage of the chirality of vitamin E, this work reports the stereoselective stabilization of polymer-vitamin E conjugate micelles. Vitamin E was covalently linked to multivalent methoxy poly(ethylene glycol)-co-poly(glutamic acid), generating amphiphilic conjugates that could self-assemble into micelles. Read More

    Physalis Mottle Virus-Like Particles as Nanocarriers for Imaging Reagents and Drugs.
    Biomacromolecules 2017 Nov 16. Epub 2017 Nov 16.
    Department of Chemistry, North Carolina State University , Raleigh, North Carolina 27695, United States.
    Platform technologies based on plant virus nanoparticles (VNPs) and virus-like particles (VLPs) are attracting the attention of researchers and clinicians because the particles are biocompatible, biodegradable, noninfectious in mammals, and can readily be chemically and genetically engineered to carry imaging agents and drugs. When the Physalis mottle virus (PhMV) coat protein is expressed in Escherichia coli, the resulting VLPs are nearly identical to the viruses formed in vivo. Here, we isolated PhMV-derived VLPs from ClearColi cells and carried out external and internal surface modification with fluorophores using reactive lysine-N-hydroxysuccinimide ester and cysteine-maleimide chemistries, respectively. Read More

    Injectable Thermo-Sensitive Polypeptide-based CDDP-Complexed Hydrogel for Improving Localized Antitumor Efficacy.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    In this study, a type of novel thermo-sensitive polypeptide-based hydrogel with tunable gelation behavior through changing the content of carboxyl groups was developed for the purpose of improving the cisplatin (CDDP) release behavior and enhancing the localized antitumor efficiency. The introduction of carboxyl groups in methoxy-poly(ethylene glycol)-b-(poly(γ-ethyl-L-glutamate-co-L-glutamic acid) (mPEG-b-P(ELG-co-LG)) not only led to adjustable mechanical properties of the hydrogel, but also significantly reduced the burst release of the drug through the complexation between the carboxyl groups of polypeptide and CDDP. Furthermore, both the good biocompatibility and biodegradable properties of mPEG-b-P(ELG-co-LG) hydrogel were observed in vivo. Read More

    Lipogels for Encapsulation of Hydrophilic Proteins and Hydrophobic Small Molecules.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    Lipid-polymer hybrid materials have the potential to exhibit enhanced stability and loading capabilities in comparison to parent liposome or polymer materials. However, complexities lie in formulating and characterizing such complex nanomaterials. Here we describe a lipid-coated polymer gel (lipogel) formulated using a one-pot methodology, where self-assembling liposomes template a UV-curable polymer gel core. Read More

    Plasmonically Enhanced Galactoxyloglucan Endowed Gold Nanoparticles Exposed Tumor Targeting Biodistribution Envisaged in a Surface-Enhanced Raman Scattering Platform.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    Biopolymer capped gold nanoparticles (AuNPs) were perceived for tracing biodistribution in a solid tumor mice through surface-enhanced Raman scattering (SERS) fingerprinting. In this strategy, a robust and ecofriendly green chemistry approach was adopted to construct galactoxyloglucan (PST001) endowed AuNPs (PST-GNPs) with cancer-cell-selective toxic nature and excellent biocompatibility. Plasmonically enhanced light scattering properties facilitated PST-GNPs to be a superior SERS substrate with high Raman signal enhancement. Read More

    A Water-Soluble Galactose-Decorated Cationic Photodynamic Therapy Agent Based on BODIPY to Selectively Eliminate Biofilm.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    A multitude of serious chronic infections involved in bacterial biofilms that are difficult to eradicate. Here, a water-soluble galactose functionalized cationic 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene (BODIPY)-based photodynamic therapy agent was synthesized for selectively eliminating the bacterial biofilm. These conjugates can capture bacteria to form aggregations through electrostatic interaction and then generate a large number of reactive oxygen species (ROS) under visible light irradiation to kill the bacteria without the emergence of bacterial resistance. Read More

    Systemic mRNA Delivery to the Lungs by Functional Polyester-based Carriers.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    Messenger RNA (mRNA) has recently come into focus as an emerging therapeutic class with great potential for protein replacement therapy, cancer immunotherapy, regenerative medicine, vaccines, and gene editing. However, the lack of effective and safe delivery methods impedes the broad application of mRNA-based therapeutics. Here, we report a robust approach to develop efficient polymeric delivery carriers for mRNA. Read More

    Estimating The Strength of Single Chitin Nanofibrils via Sonication-Induced Fragmentation.
    Biomacromolecules 2017 Nov 14. Epub 2017 Nov 14.
    We report the mechanical strength of native chitin nanofibrils. Highly crystalline α-chitin nanofibrils were purified from filaments produced by a microalgae Phaeocystis globosa, and two types of β-chitin nanofibrils were purified from pens of a squid Loligo bleekeri and tubes of a tubeworm Lamellibrachia satsuma, with relatively low and high crystallinity, respectively. These chitin nanofibrils were fully dispersed in water. Read More

    Direct UV-Triggered Thiol-ene Cross-Linking of Electrospun Polyester Fibers from Unsaturated Poly(macrolactone)s and Their Drug Loading by Solvent Swelling.
    Biomacromolecules 2017 Nov 14. Epub 2017 Nov 14.
    Department of Pharmaceutical and Medicinal Chemistry, Royal College of Surgeons in Ireland , 123 St. Stephens Green, Dublin 2, Ireland.
    Electrospinning is considered a relatively simple and versatile technique to form high porosity porous scaffolds with micron to nanoscale fibers for biomedical applications. Here, electrospinning of unsaturated aliphatic polyglobalide (PGl) into well-defined fibers with an average diameter of 9 μm is demonstrated. Addition of a dithiol cross-linker and a photoinitiator to the polymer solution enabled the UV-triggered intracross-linking of the fibers during the spinning process. Read More

    Molar Masses and Molar Mass Distributions of Chitin and Acid-Hydrolyzed Chitin.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Never-dried and dried crab shell chitin and squid pen chitin samples were acid-hydrolyzed in 1M HCl at 85 °C for up to 2 h. The crystallinities, crystal sizes, and degrees of N-acetylation of the acid-hydrolyzed chitin samples are almost unchanged the same before and after acid hydrolysis. The original and acid-hydrolyzed chitin samples were dissolved in 8% (w/w) lithium chloride/N,N,-dimethylacetamide and the solutions were subjected to size-exclusion chromatography with multi-angle laser-light scattering analysis to determine their molar masses and molar mass distributions. Read More

    Synthesis and in vitro evaluation of monodisperse amino-functional polyester dendrimers with rapid degradability and antibacterial properties.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Amine functional polymers, especially cationically charged, are interesting biomacromolecules for several reasons including easy cell membrane entrance, their ability to escape endosomes through the proton sponge effect, spontaneous complexation and delivery of drugs and siRNA and simple functionalization in aqueous solutions. Dendrimers, a subclass of precision polymers, are monodisperse and exhibit a large and exact number of peripheral end groups in relation to their size and have shown promise in drug delivery, biomedical imaging and as anti-viral agents. In this work, hydroxyl functional dendrimers of generation 1 to 5 based on 2,2-bis(methylol)propionic acid (bis-MPA) were modified to bear 6 to 96 peripheral amino groups through esterification reactions with beta-alanine. Read More

    Carbon papers and aerogels based on graphene layers and chitosan: direct preparation from high surface area graphite.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    In this work, carbon papers and aerogels based on graphene layers and chitosan were prepared. They were obtained by mixing chitosan (CS) and a high surface area nanosized graphite (HSAG) in water in the presence of acetic acid. HSAG/CS water dispersions were stable for months. Read More

    Poly(ω-methoxyalkyl acrylate)s: A nonthrombogenic polymer family with tunable protein adsorption.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    A series of polyacrylates with different n-alkyl side chain lengths (one to six, and twelve carbons) and a ω-methoxy terminal group [poly(ω-methoxyalkyl acrylate): PMCxA] were prepared to study their nonthrombogenicity using human platelet adhesion, micro bicinchoninic acid (micro BCA) protein assay, and enzyme-linked immunosorbent assay (ELISA) tests. In all cases, human platelet adhesion was suppressed on the PMCxA coated substrates, and the number of human platelets adhered to the PMC3A [poly(3-methoxypropyl acrylate)] coated surface was comparable to that of commercialized nonthrombogenic coating agent poly(2-methoxyethyl acrylate) (PMEA, equal to PMC2A). The amount of protein adsorbed onto the PMCxA was investigated by micro BCA using bovine serum albumin (BSA) and human fibrinogen (hFbn), revealing that PMC3A exhibited significantly high resistance to non-specific BSA adsorption. Read More

    Facile Low-temperature Synthesis of Cellulose Nanocrystals Carrying Buckminsterfullerene and Its Radical Scavenging Property in Vitro.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Buckminsterfullerene (C60), known for its strong radical scavenging properties, has been studied extensively for its biomedical applications. Its clinical use would be promoted by novel functionalisation of C60 with the aid of drug delivery carriers based on nanoparticle technologies. Cellulose nanocrystals (CNCs), have been recently exploited as a promising nanoplatform for drug delivery, owing to their intriguing attributes such as nanoscale dimensions, low toxicity, broad chemical-modifying capacity, and biocompatibility. Read More

    Formulation and composition effects in phase transitions of emulsions co-stabilized by cellulose nanofibrils and an ionic surfactant.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Cellulose nanofibrils (CNF) offer great prospects as a natural stabilizer of colloidal dispersions and complex fluids for application in food, pharma, and cosmetics. In this study, an ionic surfactant (sodium dodecyl sulfate, SDS) was used as emulsifier of oil-in-water and water-in-oil emulsions that were further co-stabilized by addition of CNF. The adsorption properties of SDS in both, CNF dispersions and emulsions, as well as the influence of composition (CNF and SDS concentration) and formulation (ionic strength, oil and CNF types) on the phase behavior were elucidated and described in the framework of Windsor systems. Read More

    Cell Migration and Bone Formation from Mesenchymal Stem Cell Spheroids in Alginate Hydrogels are Regulated by Adhesive Ligand Density.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    The adhesion and migration of cells entrapped in engineered materials is regulated by available adhesive ligands. Although mesenchymal stem cell (MSC) spheroids injected into damaged tissues promote repair, their transplantation in biomaterials which regulate cell migration from the aggregate may further enhance their therapeutic potential. Alginate hydrogels were modified with Arginine-Glycine-Aspartic acid (RGD) at increasing concentrations, and osteogenically induced human MSC spheroids were entrapped to assess cell migration, survival, and differentiation. Read More

    Template assisted enzymatic synthesis of oligopeptides from a polylactide chain.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Peptides are often attached to polymer materials, as bioactive components, for the control of interactions between the material and its surrounding proteins and cells. However, synthesizing peptides and attaching them to polymers can be challenging and laborious. Herein, we describe the grafting of oligopeptides to an aliphatic polyester, using a one-step chemo-enzymatic synthesis with papain as the biocatalyst. Read More

    Uptake of Long Protein-Polyelectrolyte Nanotubes by Dendritic Cells.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Institute of Condensed Matter and Nanosciences, Université catholique de Louvain , Croix du Sud 1 L7.04.02, B1348. Louvain-la-Neuve, Belgium.
    Anisotropic nanostructures, such as nanotubes, incorporating bioactive molecules present interesting features for application as drug delivery carriers. Here, we present the synthesis of layer-by-layer (LbL) nanotubes including protein (ovalbumin) layers and go from simple to more complex synergetic combinations of synthetic and natural polyelectrolytes, leading to structures with tunable properties. The rigidity in organic and aqueous media, the stability in buffer solution and the uptake of different LbL tubes by dendritic cells (DCs) are analyzed to contrast size and chemistry. Read More

    Effect of Ionic Functional Groups on the Oxidation State and Interfacial Binding Property of Catechol-Based Adhesive.
    Biomacromolecules 2017 Nov 10. Epub 2017 Nov 10.
    Adhesive hydrogels were prepared by copolymerizing dopamine methacrylamide (DMA) with either acrylic acid (AAc) or N-(3-aminopropyl)methacrylamide hydrochloride (APMH). The effect of incorporating the anionic and cationic side chains on the oxidation state of catechol was characterized using the FOX assay to track the production of hydrogen peroxide (H2O2) byproduct generated during the autoxidation of catechol while the interfacial binding property of the adhesive was determined by performing Johnson-Kendall-Roberts (JKR) contact mechanics tests tested over a wide range of pH values (pH 3-9). The ionic species contributed to interfacial binding to surfaces with the opposite charge, with measured work of adhesion values that were comparable to or in some cases higher than those of catechol. Read More

    Nonswelling thiol-yne crosslinked hydrogel materials as cytocompatible soft tissue scaffolds.
    Biomacromolecules 2017 Nov 10. Epub 2017 Nov 10.
    A key drawback of hydrogel materials for tissue engineering applications is their characteristic swelling response, which leads to a diminished mechanical performance. However, if a solution can be found to overcome such limitation, there is a wider application for these materials. Herein, we describe a simple and effective way to control the swelling and degradation rate of nucleophilic thiol-yne poly(ethylene glycol) (PEG) hydrogel networks using two straightforward routes: 1) using multi-arm alkyne and thiol terminated PEG precursors or 2) introducing a thermoresponsive unit into the PEG network while maintaining their robust mechanical properties. Read More

    Brush-like cationic polymers with low charge density for gene delivery.
    Biomacromolecules 2017 Nov 10. Epub 2017 Nov 10.
    Using a combined synthesis approach comprising reversible addition fragmentation transfer (RAFT) polymerization and ring opening reaction (ROR), a series of poly glycidyl methacrylate (polyGMA) polymers were designed and synthesized for gene delivery. These polymers characterised by low cationic charge respective to established gene delivery vectors such as PEI were studied to further elucidate the key structure activity parameters which mediate efficient and biocompatible gene delivery. Compared to PEI these brush-like polymers facilitated markedly improved safety and gene delivery efficiency. Read More

    Molecular Weight and Charge Density Effects of Guanidinylated Biodegradable Polycarbonates on Antimicrobial Activity and Selectivity.
    Biomacromolecules 2017 Nov 10. Epub 2017 Nov 10.
    Six guanidine functionalized aliphatic biodegradable polycarbonates with varying molecular weights and charge densities were synthesized via post-synthesis modification of alkyne containing polycarbonates using Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) click chemistry. The concept of passive diluting group was to modify the cationic charge density of the polycarbonate without changing its hydrophilicity. Within the molecular weight range from 8,000 g mol-1 to 30,000 g mol-1, these guanidine polycarbonates exhibited broad-spectrum biocidal activity with low toxicity to red blood cells (RBCs). Read More

    Squid Suckerin Biomimetic Peptides Form Amyloid-like Crystals with Robust Mechanical Properties.
    Biomacromolecules 2017 Nov 7. Epub 2017 Nov 7.
    We present the self-assembly of fibers formed from a peptide sequence (A1H1) derived from suckerins proteins of squid sucker ring teeth (SRT). SRT are protein-only biopolymers with an unconventional set of physico-chemical and mechanical properties, including high elastic modulus coupled with thermoplastic behaviour. We have identified a conserved peptide building block from suckerins that possess the ability to assemble into materials with similar mechanical properties as the native SRT. Read More

    Durable Anti-Superbug Polymers: Covalent Bonding of Ionic Liquid onto the Polymer Chains.
    Biomacromolecules 2017 Nov 16. Epub 2017 Nov 16.
    Shanghai Institute of Applied Physics, Chinese Academy of Sciences , No.2019, Jialuo Road, Jiading District, Shanghai 201800, People's Republic of China.
    Here, we fabricated the ionic liquid (IL) grafted poly(vinylidene fluoride) (PVDF) (PVDF-g-IL) via electron-beam irradiation to fight common bacteria and multidrug-resistant "superbugs". Two types of ILs, 1-vinyl-3-butylimmidazolium chloride (IL (Cl)) and 1-vinyl-3-ethylimidazolium tetrafluoroborate (IL (BF4)), were used. It was found that the PVDF-g-IL exhibited superior antibacterial performance, with almost the same mechanical and thermal performance as unmodified PVDF. Read More

    Design of Glycopolymers Carrying Sialyl Oligosaccharides for Controlling the Interaction with the Influenza Virus.
    Biomacromolecules 2017 Nov 14. Epub 2017 Nov 14.
    Department of Engineering, Graduate School of Chemical Engineering, Kyushu University , 744 Motooka Nishi-ku, Fukuoka 819-0395, Japan.
    We designed glycopolymers carrying sialyl oligosaccharides by "post-click" chemistry and evaluated the interaction with the influenza virus. The glycopolymer structures were synthesized in a well-controlled manner by reversible addition-fragmentation chain transfer polymerization and the Huisgen reaction. Acrylamide-type monomers were copolymerized to give hydrophilicity to the polymer backbones, and the hydrophilicity enabled the successful introduction of the oligosaccharides into the polymer backbones. Read More

    Nano into Micro Formulations of Tobramycin for the Treatment of Pseudomonas aeruginosa Infections in Cystic Fibrosis.
    Biomacromolecules 2017 Nov 16. Epub 2017 Nov 16.
    Dipartimento di Scienze e Tecnologie Biologiche Chimiche e Farmaceutiche (STEBICEF), Università di Palermo , Via Archirafi 32, 90123 Palermo, Italy.
    Here, nano into micro formulations (NiMs) of tobramycin for the treatment of Pseudomonas aeruginosa airway infections in cystic fibrosis (CF) are described. NiMs were produced by spray drying a solution containing polymers or sugars and a nanometric polyanion-tobramcyin complex (PTC), able to achieve a prolonged antibiotic release. NiMs properties were compared to TOBIPodhaler(Novartis), the only one commercially available dry powder inhalatory formulation based on porous microparticles. Read More

    Rheology as a Mechanoscopic Method to Monitor Mineralization in Hydrogels.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    Department of Materials Science and Engineering and ‡Department of Mechanical Engineering, Massachusetts Institute of Technology , Cambridge, Massachusetts 02139, United States.
    Biominerals have been widely studied due to their unique mechanical properties, afforded by their inorganic-organic composite structure and well-controlled growth in macromolecular environments. However, a lack of suitable characterization techniques for inorganic minerals in organic-rich media has prevented a full understanding of biomineralization. Here, we applied rheometry to study mineral nucleation and growth dynamics by measuring viscoelastic material properties of a hydrogel system during mineralization. Read More

    Cofibrillization of Pathogenic and Functional Amyloid Proteins with Gold Nanoparticles against Amyloidogenesis.
    Biomacromolecules 2017 Nov 14. Epub 2017 Nov 14.
    ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, Monash Institute of Pharmaceutical Sciences, Monash University , 381 Royal Parade, Parkville, Victoria 3052, Australia.
    Biomimetic nanocomposites and scaffolds hold the key to a wide range of biomedical applications. Here we show, for the first time, a facile scheme of cofibrillizing pathogenic and functional amyloid fibrils via gold nanoparticles (AuNPs) and their applications against amyloidogenesis. This scheme was realized by β-sheet stacking between human islet amyloid polypeptide (IAPP) and the β-lactoglobulin "corona" of the AuNPs, as revealed by transmission electron microscopy, 3D atomic force microscopy, circular dichroism spectroscopy, and molecular dynamics simulations. Read More

    Poly(methyl 6-acryloyl-β-d-glucosaminoside) as a Cationic Glycomimetic of Chitosan.
    Biomacromolecules 2017 Nov 1. Epub 2017 Nov 1.
    Department of Bioengineering, University of California, Los Angeles , 410 Westwood Plaza, Room 5121, Engineering V, P.O. Box 951600, Los Angeles, California 90095-1600, United States.
    Chitosan, a cationic polysaccharide derived from one of the most abundant natural polymers, chitin, has been investigated extensively for its antimicrobial properties. However, it suffers from the inherent drawbacks of natural products such as batch-to-batch variability, limited supply, contamination, and potential adverse reaction. Additionally, its solubility depends on the degree of deacetylation and pH, as it is only soluble under acidic conditions. Read More

    Importance of Evaluating Dynamic Encapsulation Stability of Amphiphilic Assemblies in Serum.
    Biomacromolecules 2017 Nov 14. Epub 2017 Nov 14.
    Department of Chemistry, ‡Center for Bioactive Delivery, Institute for Applied Life Sciences, and §Molecular and Cellular Biology Program, University of Massachusetts , Amherst, Massachusetts 01003, United States.
    In targeted drug delivery systems, it is desirable that the delivery of hydrophobic drugs to a cell or tissue is achieved with little to no side effects. To ensure that the drugs do not leak during circulation, encapsulation stability of the drug carrier in serum is critical. In this paper, we report on a modified FRET-based method to evaluate encapsulation stability of amphiphilic assemblies and cross-linked polymer assemblies in serum. Read More

    Controlling Enzymatic Polymerization from Surfaces with Switchable Bioaffinity.
    Biomacromolecules 2017 Nov 15. Epub 2017 Nov 15.
    Laboratory for Surface Science and Technology, Department of Materials, ETH Zürich , Vladimir-Prelog-Weg 5, CH-8093 Zürich, Switzerland.
    The affinity of surfaces toward proteins is found to be a key parameter to govern the synthesis of polymer brushes by surface-initiated biocatalytic atom transfer radical polymerization (SI-bioATRP). While the "ATRPase" hemoglobin (Hb) stimulates only a relatively slow growth of protein repellent brushes, the synthesis of thermoresponsive grafts can be regulated by switching the polymer's attraction toward proteins across its lower critical solution temperature (LCST). Poly(N-isopropylacrylamide) (PNIPAM) brushes are synthesized in discrete steps of thickness at temperatures above LCST, while the biocatalyst layer is refreshed at T < LCST. Read More

    Transformation of Coiled α-Helices into Cross-β-Sheets Superstructure.
    Biomacromolecules 2017 Nov 10. Epub 2017 Nov 10.
    Center for Materials Sciences, Philipps University of Marburg , 35032 Marburg, Germany.
    The fibrous silk produced by bees, wasps, ants, or hornets is known to form a four-strand α-helical coiled coil superstructure. We have succeeded in showing the formation of this coiled coil structure not only in natural fibers, but also in artificial films made of regenerated silk of the hornet Vespa simillima xanthoptera using wide- and small-angle X-ray scatterings and polarized Fourier transform infrared spectroscopy. On the basis of time-resolved simultaneous synchrotron X-ray scattering observations for in situ monitoring of the structural changes in regenerated silk material during tensile deformation, we have shown that the application of tensile force under appropriate conditions induces a transition from the coiled α-helices to a cross-β-sheet superstructure. Read More

    How Bound and Free Fatty Acids in Cellulose Films Impact Nonspecific Protein Adsorption.
    Biomacromolecules 2017 Nov 8. Epub 2017 Nov 8.
    Wood Technology and Wood Chemistry, Georg-August-University of Goettingen , Büsgenweg 4, 37077 Göttingen, Germany.
    The effect of fatty acids and fatty acid esters to impair nonspecific protein adsorption on cellulose thin films is investigated. Thin films are prepared by blending trimethylsilyl cellulose solutions with either cellulose stearoyl ester or stearic acid at various ratios. After film formation by spin coating, the trimethylsilyl cellulose fraction of the films is converted to cellulose by exposure to HCl vapors. Read More

    Starch Aerogels: A Member of the Family of Thermal Superinsulating Materials.
    Biomacromolecules 2017 Nov 8. Epub 2017 Nov 8.
    MINES ParisTech, PSL Research University, Centre for Material Forming (CEMEF), UMR CNRS 7635, CS 10207, 06904 Sophia Antipolis, France.
    Starch aerogels were prepared via dissolution in water (thermomechanical treatment), retrogradation, solvent exchange, and drying with supercritical CO2. Amylose content in starches was varied from 0 to 100%. The aerogels' bulk density, morphology, specific surface area, thermal conductivity, and mechanical properties under compression were investigated. Read More

    Immobilization of β-Cyclodextrin-Conjugated Lactoferrin onto Polymer Monolith for Enrichment of Ga in Metabolic Residues of Ga-Based Anticancer Drugs.
    Biomacromolecules 2017 Nov 7. Epub 2017 Nov 7.
    College of Chemistry, Jilin University , Changchun 130012, China.
    Biological-material-functionalized porous monoliths were prepared with lactoferrin and β-cyclodextrin via a click reaction. With the monolith as an extraction medium, a method combined with ICP-MS was developed for the determination of total gallium originating from metabolic residues of orally bioavailable gallium complexes with tris(8-quinolinolato)gallium (GaQ3) as a representative. The method exhibited favorable adsorption behaviors for gallium with high selectivity, low detection limit (2 ng L(-1)), and an enrichment factor of 29-fold with the sample throughput of 30 min(-1). Read More

    Characterization and Elimination of Undesirable Protein Residues in Plant Cell Wall Materials for Enhancing Lignin Analysis by Solution-State Nuclear Magnetic Resonance Spectroscopy.
    Biomacromolecules 2017 Nov 8. Epub 2017 Nov 8.
    Department of Biochemistry, University of Wisconsin-Madison , Madison, Wisconsin 53706, United States.
    Protein polymers exist in every plant cell wall preparation, and they interfere with lignin characterization and quantification. Here, we report the structural characterization of the residual protein peaks in 2D NMR spectra in corn cob and kenaf samples and note that aromatic amino acids are ubiquitous and evident in spectra from various other plants and tissues. The aromatic correlations from amino acid residues were identified and assigned as phenylalanine and tyrosine. Read More

    Simple One-Pot Synthesis of Fully Biobased Unsaturated Polyester Resins Based on Itaconic Acid.
    Biomacromolecules 2017 Nov 8. Epub 2017 Nov 8.
    Innovation Center of Faculty of Technology and Metallurgy, University of Belgrade , 4 Karnegijeva Street, 11000 Belgrade, Serbia.
    For the preparation of fully biobased unsaturated polyester resins (UPRs), the replacement of styrene with alternate nonpetroleum-based monomers turned out to be one of the most challenging tasks. Its complexity lies in the fact that reactive diluents (RD) have to have low viscosity and volatility, good compatibility with prepolymer, and capability to homopolymerize and copolymerize with its unsaturations. In this context, we directed our efforts to develop fully biobased UPRs using the dialkyl itaconates as an alternative to styrene. Read More

    Self-Assembled Polypeptide Nanogels with Enzymatically Transformable Surface as a Small Interfering RNA Delivery Platform.
    Biomacromolecules 2017 Nov 13. Epub 2017 Nov 13.
    Department of Polymer Chemistry, Graduate School of Engineering, Kyoto University , Katsura, Nishikyo-ku, Kyoto 615-8510, Japan.
    Nanometer-size gel particles, or nanogels, have potential for delivering therapeutic macromolecules. A cationic surface promotes cellular internalization of nanogels, but undesired electrostatic interactions, such as with blood components, cause instability and toxicities. Poly(ethylene glycol) coating has been used to shield charges, but this decreases delivery efficiency. Read More

    Glycosylated Reversible Addition-Fragmentation Chain Transfer Polymers with Varying Polyethylene Glycol Linkers Produce Different Short Interfering RNA Uptake, Gene Silencing, and Toxicity Profiles.
    Biomacromolecules 2017 Nov 9. Epub 2017 Nov 9.
    CSIRO Manufacturing , Private Bag 10, Clayton South, Victoria 3169, Australia.
    Achieving efficient and targeted delivery of short interfering (siRNA) is an important research challenge to overcome to render highly promising siRNA therapies clinically successful. Challenges exist in designing synthetic carriers for these RNAi constructs that provide protection against serum degradation, extended blood retention times, effective cellular uptake through a variety of uptake mechanisms, endosomal escape, and efficient cargo release. These challenges have resulted in a significant body of research and led to many important findings about the chemical composition and structural layout of the delivery vector for optimal gene silencing. Read More

    Preparation and Characterization of Hypoglycemic Nanoparticles for Oral Insulin Delivery.
    Biomacromolecules 2017 Nov 7. Epub 2017 Nov 7.
    School of Life Science, South China Normal University , Guangzhou 510631, China.
    Polymeric nanoparticles have been widely investigated as insulin delivery systems for oral administration. However, the toxic nature of many artificial polymers hampers their effective application, creating a demand for the further exploration of alternative natural polymers. In addition, ethnobotanical research has reported that over 800 plant species have a hypoglycemic function, some of which are polymers. Read More

    Independently Tuning the Biochemical and Mechanical Properties of 3D Hyaluronan-Based Hydrogels with Oxime and Diels-Alder Chemistry to Culture Breast Cancer Spheroids.
    Biomacromolecules 2017 Oct 31. Epub 2017 Oct 31.
    Department of Chemical Engineering and Applied Chemistry, University of Toronto , 200 College Street, Toronto, Ontario M5S 3E5, Canada.
    For native breast cancer cell growth to be mimicked in vitro as spheroids, a well-defined matrix that mimics the tumor microenvironment is required. Finding a biomimetic material for 3D cell culture other than Matrigel has challenged the field. Because hyaluronan is naturally abundant in the tumor microenvironment and can be chemically modified, we synthesized a hyaluronan (HA) hydrogel with independently tunable mechanical and chemical properties for 3D culture of breast cancer cells. Read More

    A Bottom-Up Synthesis of Vinyl-Cellulose Nanosheets and Their Nanocomposite Hydrogels with Enhanced Strength.
    Biomacromolecules 2017 Nov 3. Epub 2017 Nov 3.
    Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology , Tokyo 152-8550, Japan.
    Extracted nanocellulose from natural resources commonly requires modification before it is used as an effective nanofiller. In the present study, through an enzymatic polymerization of α-d-glucose 1-phosphate from the primer 2-(glucosyloxy)ethyl methacrylate (GEMA), a novel type of two-dimensional methacrylate-containing cellulose nanosheets (CNS) with a thickness of about 6 nm, named as GEMA-CNS, was directly synthesized under a mild condition by a "bottom-up" method. The structure and morphology of GEMA-CNS were characterized by (1)H-nuclear magnetic resonance (NMR), matrix-assisted laser desorption/ionization time-of-flight mass spectra (MALDI-TOF MS), Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), and atomic force microscopy (AFM). Read More

    Boric Acid Induced Transient Cross-Links in Lactose-Modified Chitosan (Chitlac).
    Biomacromolecules 2017 Nov 8. Epub 2017 Nov 8.
    Department of Life Sciences, University of Trieste , Via Licio Giorgieri 5, I-34127 Trieste, Italy.
    The present paper explores the effect of boric acid on Chitlac, a lactose-modified chitosan which had previously shown interesting biological and physical-chemical features. The herewith-reported experimental evidences demonstrated that boric acid binds to Chitlac, producing conformational and association effects on the chitosan derivative. The thermodynamics of boric acid binding to Chitlac was explored by means of (11)B NMR, circular dichroism (CD), and UV-vis spectroscopy, while macromolecular effects were investigated by means of viscometry and dynamic light scattering (DLS). Read More

    Porous Poly(ε-caprolactone)-Poly(l-lactic acid) Semi-Interpenetrating Networks as Superior, Defect-Specific Scaffolds with Potential for Cranial Bone Defect Repair.
    Biomacromolecules 2017 Oct 26. Epub 2017 Oct 26.
    Department of Biomedical Engineering and ‡Department of Material Science and Engineering, Texas A&M University , College Station, Texas 77843, United States.
    The treatment of irregular cranial bone defects is currently limited due to the graft resorption that can occur when an ill-fitting interface exists between an autograft and the surrounding tissue. A tissue engineering scaffold able to achieve defect-specific geometries could improve healing. This work reports a macroporous, shape memory polymer (SMP) scaffold composed of a semi-interpenetrating network (semi-IPN) of thermoplastic poly(l-lactic acid) (PLLA) within cross-linked poly(ε-caprolactone) diacrylate (PCL-DA) that is capable of conformal fit within a defect. Read More

    Enhancing Photochemical Internalization of DOX through a Porphyrin-based Amphiphilic Block Copolymer.
    Biomacromolecules 2017 Oct 31. Epub 2017 Oct 31.
    State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University , Shanghai 201620, China.
    Drug resistance is a primary obstacle that seriously reduces the therapy efficiency of most chemotherapeutic agents. To address this issue, the photochemical internalization (PCI) was employed to help the anticancer drug escape from lysosome and improve their translocation to the nucleus. A pH-sensitive porphyrin-based amphiphilic block copolymer (PEG113-b-PCL54-a-porphyrin) was synthesized, which was acted not only as a carrier for the delivery of DOX but also as a photosensitizer for PCI. Read More

    Star Polymers Reduce Islet Amyloid Polypeptide Toxicity via Accelerated Amyloid Aggregation.
    Biomacromolecules 2017 Oct 31. Epub 2017 Oct 31.
    ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, Monash Institute of Pharmaceutical Sciences, Monash University , 381 Royal Parade, Parkville, Victoria 3052, Australia.
    Protein aggregation into amyloid fibrils is a ubiquitous phenomenon across the spectrum of neurodegenerative disorders and type 2 diabetes. A common strategy against amyloidogenesis is to minimize the populations of toxic oligomers and protofibrils by inhibiting protein aggregation with small molecules or nanoparticles. However, melanin synthesis in nature is realized by accelerated protein fibrillation to circumvent accumulation of toxic intermediates. Read More

    Doxorubicin-Loaded Unimolecular Micelle-Stabilized Gold Nanoparticles as a Theranostic Nanoplatform for Tumor-Targeted Chemotherapy and Computed Tomography Imaging.
    Biomacromolecules 2017 Oct 26. Epub 2017 Oct 26.
    School of Chemistry and Chemical Engineering, South China University of Technology , Guangzhou 510640, P. R. China.
    Current research is mainly trending toward addressing the development of multifunctional nanocarriers that could precisely reach disease sites, release drugs in a controlled-manner, and act as an imaging agent for both diagnosis and targeted therapy. In this study, a pH-sensitive theranostic nanoplatform as a promising dual-functional nanovector for tumor therapy and computed tomography (CT) imaging was developed. The 21-arm star-like triblock polymer of β-cyclodextrin-{poly(ε-caprolactone)-poly(2-aminoethyl methacrylate)-poly[poly(ethylene glycol) methyl ether methacrylate]}21 [β-CD-(PCL-PAEMA-PPEGMA)21] with stable unimolecular micelles formed in aqueous solution was first synthesized by combined ROP with ARGET ATRP techniques and then was used as a template for fabricating gold nanoparticles (AuNPs) with uniform sizes and excellent colloidal stability in situ followed by the encapsulation of doxorubicin (DOX) with maximum entrapment efficiency up to 60% to generate the final product β-CD-(PCL-PAEMA-PPEGMA)21/AuNPs/DOX. Read More

    Spectroelectrochemical Reverse Engineering DemonstratesThat Melanin's Redox and Radical Scavenging Activities Are Linked.
    Biomacromolecules 2017 Nov 1. Epub 2017 Nov 1.
    Institute for Bioscience and Biotechnology Research, University of Maryland , 4291 Fieldhouse Drive, 5112 Plant Sciences Building, College Park, Maryland 20742, United States.
    Melanins are ubiquitous in nature but their biological activities and functions have been difficult to discern. Conventional approaches to determine material function start by resolving structure and then characterize relevant properties. These approaches have been less successful for melanins because of their complex structure and insolubility, and because their relevant properties are not readily characterized by conventional methods. Read More

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