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    Cellulose Abetted Assembly and Temporally Decoupled Loading of Cargo into Vesicles Synthesized from Functionally Diverse Lamellar Phase Forming Amphiphiles.
    Biomacromolecules 2018 Feb 21. Epub 2018 Feb 21.
    Department of Bioengineering, University of California, Merced , Merced, California 95343, United States.
    Self-assembled micrometer-scale vesicles composed of lamellar phase forming amphiphiles are useful as chemical microreactors, as minimal artificial cells, as protocell mimics for studies of the origins of life, and as vehicles for the targeted delivery of drugs. Given their varied uses, discovery of a universal mechanism that is simple, rapid, and that produces vesicles from a large variety of amphiphiles with different chemical and physical properties at high yield is extremely desirable. Here we show that cellulose, in the form of cellulose paper, facilitates the assembly of membranous vesicles 5-20 μm in diameter from scientifically and technologically important amphiphiles of diverse chemical structures and functionality such as fatty acids (fatty acid vesicles), amphiphilic diblock copolymers, and amphiphilic triblock copolymers (polymersomes). Read More

    Enhanced Arylamine N-Oxygenase Activity of Polymer-Enzyme Assemblies by Facilitating Electron-Transferring Efficiency.
    Biomacromolecules 2018 Feb 20. Epub 2018 Feb 20.
    A novel N-oxygenase coated core-shell nanoparticle was generated through the co-assembly of poly(4-vinylpyridine) (P4VP) and arylamine N-oxygenase CmlI. The resulting enzyme-hybridized particles, P4VP-CmlI, showed excellent catalytic activities on the oxidation of two arylamine substrates, i.e. Read More

    A Self-Targeting, Dual ROS/pH-Responsive Apoferritin Nanocage for Spatiotemporally Controlled Drug Delivery to Breast Cancer.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    School of Pharmaceutical Sciences, Zhengzhou University , 100 Science Road, Zhengzhou 450001, China.
    In this study, an intelligent pH and ROS dual-responsive drug delivery system based on an apoferritin (AFt) nanocage was prepared. This therapeutic system can specifically self-target 4T1 breast cancer cells by exploiting L-apoferritin receptor SCARA 5, avoiding the nonspecific binding or aggregation of nanoparticles due to the chemical functionalization for targeting. The characteristics of AFt were utilized for the simultaneous delivery of anticancer drug doxorubicin (DOX) and photosensitizer rose bengal (RB). Read More

    Reinforcing mucus barrier properties with low molar mass chitosans.
    Biomacromolecules 2018 Feb 16. Epub 2018 Feb 16.
    The mucus gel covers the wet epithelia that forms the inner lining of the body. It constitutes our first line of defense protecting the body from infections and other deleterious molecules. Failure of the mucus barrier can lead to the inflammation of the mucosa such as in inflammatory bowel diseases. Read More

    Tri-Layer Polymeric Shells containing Magnetite Nanocarrier mediated LCS-1 delivery for Synthetic Lethal Therapy of BLM-defective Colorectal Cancer Cells.
    Biomacromolecules 2018 Feb 16. Epub 2018 Feb 16.
    Synthetic lethality is a molecular targeted therapy for selective killing of cancer cells. We exploited a lethal interaction between Superoxide dismutase1 inhibition and Bloom syndrome gene product (BLM) defect for the treatment of colorectal cancer (CRC) cells (HCT 116) with lung cancer screen-1 (LCS-1) loaded customized nanocarrier. LCS-1 has poor aqueous solubility. Read More

    Neat Protein-Polymer Surfactant Bioconjugates as Universal Solvents.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    Department of Chemistry, Indian Institute of Technology Bombay , Powai, Mumbai 400076, India.
    Solvents, particularly those having low volatility, are of great interest for the biocatalytic synthesis of utility chemicals and fuels. We show novel and universal solvent-like properties of a neat and water-less polymer surfactant-bovine serum albumin (BSA) conjugated material (WL-PSpBSA). This highly viscous, nonvolatile material behaves as a liquid above its solid-liquid transition temperature (∼25-27 °C) and can be used as a solvent for variety of completely dry solutes of different sizes and surface chemistries. Read More

    Rapid-Forming and Self-Healing Agarose-Based Hydrogels for Tissue Adhesives and Potential Wound Dressings.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    Key Laboratory of Colloid and Interface Chemistry & Key Laboratory of Special Aggregated Materials, (Shandong University), Ministry of Education , Jinan 250100, P. R. China.
    To meet the progressive requirements of advanced engineering materials with superior physicochemical performances, self-healing and injectable hydrogels (AD hydrogels) based on agarose with pH-response were prepared through dynamic covalent Schiff-base linkages by simply mixing nontoxic agarose-ethylenediamine conjugate (AG-NH) and dialdehyde-functionalized polyethylene glycol (DF-PEG) solutions. The self-healing and injectable capabilities of the hydrogels without any external stimulus are ascribed to dynamic covalent Schiff-base linkages between the aldehyde groups of DF-PEG and amine groups on AG-NHbackbone. It is demonstrated that the AD hydrogels possess interconnected porous morphologies, rapid gelation time, excellent deformability, and good mechanical strength. Read More

    Guanidinium-functionalized Interpolyelectrolyte Complexes Enable RNAi in Resistant Insect Pests.
    Biomacromolecules 2018 Feb 15. Epub 2018 Feb 15.
    RNAi-based technologies are ideal for pest control as they can provide species specificity and spare non-target organisms. However, in some pests biological barriers prevent use of RNAi, and therefore broad application. In this study we tested the ability of a synthetic cationic polymer, poly-[N-(3-guanidinopropyl)methacrylamide] (pGPMA), that mimics arginine-rich cell penetrating peptides to trigger RNAi in an insensitive animal-Spodoptera frugiperda. Read More

    A Versatile and Robust Approach to Stimuli-Responsive Protein Multilayers with Biologically Enabled Unique Functions.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    Key Laboratory of Polymer Chemistry & Physics of Ministry of Education, Center for Soft Matter Science and Engineering, College of Chemistry and Molecular Engineering, Peking University , Beijing 100871, People's Republic of China.
    Protein-based materials call for innovative processing techniques to integrate their unique biologically enabled functions with other materials of complementary features. Herein, we report the covalent protein layer-by-layer assembly via orthogonal "Tag-Catcher" reactions as a facile and robust approach to make entirely protein-based multilayers on a variety of substrates. Programmed assembly of native telechelic proteins not only endows the materials valuable stimuli-sensitive behaviors, but also unique properties unparalleled by any synthetic counterparts. Read More

    Diels-Alder Click-Cross-Linked Hydrogels with Increased Reactivity Enable 3D Cell Encapsulation.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    Department of Chemical Engineering and Applied Chemistry, Donnelly Centre, University of Toronto , 160 College Street, Toronto, Ontario M5S3E1, Canada.
    Engineered hydrogels have been extensively used to direct cell function in 3D cell culture models, which are more representative of the native cellular microenvironment than conventional 2D cell culture. Previously, hyaluronan-furan and bis-maleimide polyethylene glycol hydrogels were synthesized via Diels-Alder chemistry at acidic pH, which did not allow encapsulation of viable cells. In order to enable gelation at physiological pH, the reaction kinetics were accelerated by replacing the hyaluronan-furan with the more electron-rich hyaluronan-methylfuran. Read More

    pH-Responsive Microencapsulation Systems for the Oral Delivery of Polyanhydride Nanoparticles.
    Biomacromolecules 2018 Feb 21. Epub 2018 Feb 21.
    Department of Chemical and Biological Engineering, Iowa State University , Ames, Iowa 50011, United States.
    Multicompartmental polymer carriers, referred to as Polyanhydride-Releasing Oral MicroParticle Technology (PROMPT), were formed by a pH-triggered antisolvent precipitation technique. Polyanhydride nanoparticles were encapsulated into anionic pH-responsive microparticle gels, allowing for nanoparticle encapsulation in acidic conditions and subsequent release in neutral pH conditions. The effects of varying the nanoparticle composition and feed ratio on the encapsulation efficiency were evaluated. Read More

    Three-dimensional directionality is a pivotal structural feature for the bioactivity of azabisphosphonate-capped Poly(PhosphorHydrazone) nanodrug dendrimers.
    Biomacromolecules 2018 Feb 14. Epub 2018 Feb 14.
    Dendrimers are nanosized, non-linear, hyperbranched polymers whose overall three-dimensional shape is key for their biological activity. Poly(PhosphorHydrazone) (PPH) dendrimers capped with aza-bisphosphonate (ABP) end groups are known to have anti-inflammatory properties enabling the control of inflammatory diseases in different mouse models. Here we screen the anti-inflammatory activity of a series of PPH bearing between 2 and 16 ABP end groups in a mouse model of arthritis, and confront the biological results with atomistic simulations of the dendrimers. Read More

    Peptoid backbone flexibility dictates its interaction with water and surfaces: A molecular dynamics investigation.
    Biomacromolecules 2018 Feb 14. Epub 2018 Feb 14.
    Peptoids are peptide-mimetic biopolymers that are easy-to-synthesize and adaptable for use in drugs, chemical scaffolds, and coatings. However, there is insufficient information about their structural preferences and interactions with the environment in various applications. We conducted a study to understand the fundamental differences between peptides and peptoids using molecular dynamics simulations with semi-empirical (PM6) and empirical (AMBER) potentials, in conjunction with metadynamics enhanced sampling. Read More

    Electrospun Poly(lactic acid)-Based Fibrous Nanocomposite Reinforced by Cellulose Nanocrystals: Impact of Fiber Uniaxial Alignment on Microstructure and Mechanical Properties.
    Biomacromolecules 2018 Feb 22. Epub 2018 Feb 22.
    Key Laboratory of Bio-based Material Science and Technology (Ministry of Education), Northeast Forestry University , Harbin 150040, P R China.
    Uniform poly(lactic acid)/cellulose nanocrystal (PLA/CNC) fibrous mats composed of either random or aligned fibers reinforced with up to 20 wt % CNCs were successfully produced by two different electrospinning processes. Various concentrations of CNCs could be stably dispersed in PLA solution prior to fiber manufacture. The microstructure of produced fibrous mats, regardless of random or aligned orientation, was transformed from smooth to nanoporous surface by changing CNC loading levels. Read More

    Construction of Bioactive and Reinforced Bioresorbable Nanocomposites by Reduced Nano-Graphene Oxide Carbon Dots.
    Biomacromolecules 2018 Feb 19. Epub 2018 Feb 19.
    Department of Fibre and Polymer Technology, KTH Royal Institute of Technology , 100 44 Stockholm, Sweden.
    Bioactive and reinforced poly(ε-caprolactone) (PCL) films were constructed by incorporation of cellulose derived reduced nanographene oxide (r-nGO) carbon nanodots. Two different microwave-assisted reduction routes in superheated water were utilized to obtain r-nGO and r-nGO-CA. For the latter, a green reducing agent caffeic acid (CA), was incorporated in the reduction process. Read More

    Polymer Assembly Encapsulation of Lanthanide Nanoparticles as Contrast Agents for In Vivo Micro-CT.
    Biomacromolecules 2018 Feb 22. Epub 2018 Feb 22.
    Department of Medical Biophysics, ‡Robarts Research Institute, §Department of Chemistry, and ∥Department of Chemical and Biochemical Engineering, The University of Western Ontario , 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
    Despite recent technological advancements in microcomputed tomography (micro-CT) and contrast agent development, preclinical contrast agents are still predominantly iodine-based. Higher contrast can be achieved when using elements with higher atomic numbers, such as lanthanides; lanthanides also have X-ray attenuation properties that are ideal for spectral CT. However, the formulation of lanthanide-based contrast agents at the high concentrations required for vascular imaging presents a significant challenge. Read More

    Synthesis and Properties of Alternating Polypeptoids and Polyampholytes as Protein-Resistant Polymers.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    Key Laboratory of Polymer Ecomaterials and ⊥Laboratory of Polymer Composites Engineering, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , 5625 Renmin Street, Changchun 130022, P. R. China.
    Alternating polypeptoids are particularly appealing because alternating sequence may impart highly ordered structure and special functions, while their simple synthesis still remains a key challenge. We describe that natural amino acid monomers can be polymerized via Ugi reaction in a step-growth fashion as an AA' BB' system, which leads to alternating polypeptoids with molecular weight up to 15 kg/mol. These alternating polypeptoids are thermally responsive and exhibit cloud points (T) between 27 and 37 °C. Read More

    Encoding Stem-Cell-Secreted Extracellular Matrix Protein Capture in Two and Three Dimensions Using Protein Binding Peptides.
    Biomacromolecules 2018 Feb 22. Epub 2018 Feb 22.
    Manufacturing Flagship, Commonwealth Scientific and Industrial Research Organization (CSIRO) , Clayton, Victoria 3169, Australia.
    Capturing cell-secreted extracellular matrix (ECM) proteins through cooperative binding with high specificity and affinity is an important function of native tissue matrices during both tissue homeostasis and repair. However, while synthetic hydrogels, such as those based on poly(ethylene glycol) (PEG), are often proposed as ideal materials to deliver human mesenchymal stem cells (hMSCs) to sites of injury to enable tissue repair, they do not have this capability-a capability that would enable cells to actively remodel their local extracellular microenvironment and potentially provide the required feedback control for more effective tissue genesis. In this work, we detail a methodology that engenders poly(ethylene glycol) (PEG)-based two-dimensional substrates and three-dimensional porous hydrogels with the ability to capture desired extracellular matrix (ECM) proteins with high specificity. Read More

    Single-Step In Situ Assembling Routes for the Shape Control of Polymer Nanoparticles.
    Biomacromolecules 2018 Feb 20. Epub 2018 Feb 20.
    Department of Physical Chemistry and Microreaction Technology, Technical University of Ilmenau , Weimarer Strasse 32, D-98693 Ilmenau, Germany.
    Controlling shapes of polymer nanoparticles via single-step process is a challenge due to their amorphous chemical nature. Precise regulation of interfacial interactions, electrical charging and reaction dynamics during ongoing polymerization process provides an environment where uniform nucleation, growth and in situ assembling can be realized, and hence nanoparticles of complex shapes can be obtained. In this work, it is investigated how in situ assembling of the growing nanoparticles succeeds and specifically in different manners by using cationic, anionic, polyionic, and nonionic surface-active agents in a time-dependent blended form. Read More

    Multifunctional Biomaterial Coating Based on Bio-Inspired Polyphosphate and Lysozyme Supramolecular Nanofilm.
    Biomacromolecules 2018 Feb 19. Epub 2018 Feb 19.
    College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University , Chengdu 610065, China.
    Current implant materials have widespread clinical applications together with some disadvantages, the majority of which are the ease with which infections are induced and difficulty in exhibiting biocompatibility. For the efficient improvement of their properties, the development of interface multifunctional modification in a simple, universal, and environmently benign approach becomes a critical challenge and has acquired the attention of numerous scientists. In this study, a lysozyme-polyphosphate composite coating was fabricated for titanium(Ti)-based biomaterial to obtain a multifunctional surface. Read More

    Design of Carrageenan-Based Heparin-Mimetic Gel Beads as Self-Anticoagulant Hemoperfusion Adsorbents.
    Biomacromolecules 2018 Feb 19. Epub 2018 Feb 19.
    College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University , Chengdu, 610065, People's Republic of China.
    The currently used hemoperfusion adsorbents such as activated carbon and ion-exchange resin show dissatisfactory hemocompatibility, and a large dose of injected heparin leads to the increasing cost and the risk of systematic bleeding. Natural polysaccharide adsorbents commonly have good biocompatibility, but their application is restricted by the poor mechanical strength and low content of functional groups. Herein, we developed an efficient, self-anticoagulant and blood compatible hemoperfusion adsorbent by imitating the structure and functional groups of heparin. Read More

    Structural Comparison of Various Silkworm Silks: An Insight into the Structure-Property Relationship.
    Biomacromolecules 2018 Feb 19. Epub 2018 Feb 19.
    School of Molecular Sciences, Magnetic Resonance Research Center, Arizona State University , Tempe, Arizona 85287-1604, United States.
    Silkworm silk has attracted considerable attention in recent years due to its excellent mechanical properties, biocompatibility, and promising applications in biomedical sector. However, a clear understanding of the molecular structure and the relationship between the excellent mechanical properties and the silk protein sequences are still lacking. This study carries out a thorough comparative structural analysis of silk fibers of four silkworm species (Bombyx mori, Antheraea pernyi, Samia cynthia ricini, and Antheraea assamensis). Read More

    Nonthrombogenic Hydrogel Coatings with Carbene-Cross-Linking Bioadhesives.
    Biomacromolecules 2018 Feb 19. Epub 2018 Feb 19.
    School of Materials Science and Engineering, Nanyang Technological University , 50 Nanyang Avenue, Singapore 639798.
    Bioadhesives are a current unmet clinical need for mending of blood contacting soft tissues without inducing thrombosis. Recent development of carbene precursor bioadhesives with the advantages of on-demand curing, tuneable modulus, and wet adhesion have been synthesized by grafting diazirine onto poly (amidoamine) (PAMAM-G5) dendrimers. Herein, the structure activity relationships of platelet adhesion and activation is evaluated for the first time on the cured PAMAM-g-diazirine bioadhesives. Read More

    Multifunctional Polymeric Micelles with Amplified Fenton Reaction for Tumor Ablation.
    Biomacromolecules 2018 Feb 20. Epub 2018 Feb 20.
    CAS Key Laboratory of Soft Matter Chemistry, Department of Polymer Science and Engineering, University of Science and Technology of China , Hefei 230026, Anhui, China.
    Relative to normal cells, tumor cells lack adequate capability of reactive oxygen scavenging. Thus, tumor cells can be selectively killed by increasing the concentration of reactive oxygen species in tumor tissue. In this report, we construct an integrated multifunctional polymeric nanoparticle which can selectively improve hydrogen peroxide (HO) levels in tumor tissue and convert them into more active hydroxyl radicals by Fenton reaction. Read More

    Swelling and Free-Volume Characteristics of TEMPO-Oxidized Cellulose Nanofibril Films.
    Biomacromolecules 2018 Feb 8. Epub 2018 Feb 8.
    Department of Chemical Engineering, Norwegian University of Science and Technology , 7491 Trondheim, Norway.
    Cellulose nanofibrils (CNFs) are becoming increasingly ubiquitous in diverse technologies requiring sustainable nanoscale species to form or modify films. The objective of the present study is to investigate the swelling behavior and accompanying free volume of self-standing TEMPO-oxidized (TO) CNF films in the presence of water vapor. For this purpose, we have performed time-resolved swelling experiments on films, prepared according to different experimental protocols, at 90% relative humidity (RH) and ambient temperature. Read More

    Self-Standing Nanocellulose Janus-Type Films with Aldehyde and Carboxyl Functionalities.
    Biomacromolecules 2018 Feb 22. Epub 2018 Feb 22.
    Department of Natural and Microbial Products Chemistry, National Research Centre , Dokki, Giza, Egypt 12622.
    Nanocellulose-based self-standing films are becoming a substrate for flexible electronics, diagnostics, and sensors. Strength and surface chemistry are vital variables for these film-based endeavors, the former is one of the assets of nanocellulose. To contribute to the latter, nanocellulose films are tuned with a side-specific functionalization, having an aldehyde and a carboxyl side. Read More

    Amine-Reactive Poly(pentafluorophenyl acrylate) Brush Platforms for Cleaner Protein Purification.
    Biomacromolecules 2018 Feb 15. Epub 2018 Feb 15.
    The National Creative Research Initiative Center for Intelligent Hybrids, School of Chemical and Biological Engineering, Seoul National University , Seoul 08826, Korea.
    Reactive pentafluorophenyl acrylate (PFPA) polymer brushes grafted on silica particles were prepared using surface-initiated reversible addition and fragmentation chain transfer polymerization. The polymer brush was successfully immobilized with antibody, then used for protein separation. The immunoprecipitated proteins showed successful enrichment of target protein, with reduced nonspecific background and less contamination from eluted antibodies. Read More

    In-Situ Quantitative and Multiscale Structural Study of Starch-Based Biomaterials Immersed in Water.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    UR 1268 Biopolymères Interactions Assemblages, INRA , 44300 Nantes, France.
    The behavior upon immersion in water of two types of starchy materials of biomedical relevance, amorphous potato starch and glycerol-plasticized potato starch, is analyzed in depth. Synchrotron X-ray scattering, specifically wide-angle X-ray scattering (WAXS), and magnetic resonance microimaging (MRμI) are used as very precise and nondestructive quantitative methods to monitor water transfers and structure changes in the samples, with refined spatial and kinetics results. The ingress of water in the cylinder-shaped samples can be inferred from both techniques, and from this, a diffusion mechanism is deduced for each sample type. Read More

    CD44-Targeted Facile Enzymatic Activatable Chitosan Nanoparticles for Efficient Antitumor Therapy and Reversal of Multidrug Resistance.
    Biomacromolecules 2018 Feb 14. Epub 2018 Feb 14.
    Beijing Hospital and Beijing Institute of Geriatrics , Ministry of Health, Beijing 100730, People's Republic of China.
    Nanoparticles are attractive platforms for the delivery of various anticancer therapeutics. Nevertheless, their applications are still limited by the relatively low drug loading capacity and the occurrence of multidrug resistance (MDR) against chemotherapeutics. In this study, we report that the integration of d-α-tocopherol succinate (VES) residue with both chitosan and paclitaxel (PTX) led to significant improvement of drug loading capacity and drug loading efficiency through the enhancement of drug/carrier interaction. Read More

    Understanding the Mechanical Properties and Structure Transition of Antheraea pernyi Silk Fiber Induced by Its Contraction.
    Biomacromolecules 2018 Feb 23. Epub 2018 Feb 23.
    State Key Laboratory of Molecular Engineering of Polymers, Laboratory of Advanced Materials and Department of Macromolecular Science, Fudan University , Shanghai 200433, People's Republic of China.
    Like most major ampullate silks of spider, the length of Antheraea pernyi silkworm silk can shrink to a certain degree when the fiber is in contact with water. However, what happens in terms of molecule chain level and how it correlates to the mechanical properties of the silk during its contraction is not yet fully understood. Here, we investigate the water-induced mechanical property changes as well as the structure transition of two kinds of A. Read More

    Series of In Situ Photoinduced Polymer Graftings for Sensitive Detection of Protein Biomarkers via Cascade Amplification of Liquid Crystal Signals.
    Biomacromolecules 2018 Feb 14. Epub 2018 Feb 14.
    Key Laboratory of Carbon Fiber and Functional Polymers (Beijing University of Chemical Technology) , Ministry of Education, Beijing, 100029 China.
    Developing of new polymeric materials for the sensitive and rapid detection of trace protein biomarkers has attracted increasing attention in biomedical fields. Herein, series of in situ photoinduced polymer graftings were developed for sensitive detection of protein biomarkers by using featured cascade amplification of liquid crystal (LC) signals. The limit-of-detection (LOD) for native bovine serum albumin (BSA) molecules is around 10 μg/mL in a LC biosensor before signal amplification. Read More

    Dissolution of Cellulosic Fibers: Impact of Crystallinity and Fiber Diameter.
    Biomacromolecules 2018 Feb 2;19(2):640-651. Epub 2018 Feb 2.
    Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York (SUNY) , Buffalo, New York 14260-4200, United States.
    With the aim of informing the selection of biomass pretreatment options and to assist in interpreting experimental results from different biomass/solvent combinations, this study addresses the impact of crystallinity and size on the kinetics of semicrystalline cellulose fiber swelling and dissolution. To this end, a newly developed phenomenological model is utilized that accounts for the role of decrystallization and disentanglement as two rate-determinant steps in the cellulose dissolution process. Although fibers with lower crystallinity swell more and faster, the degree of crystallinity does not affect the dissolution rate. Read More

    Thermal Stabilization of Biologics with Photoresponsive Hydrogels.
    Biomacromolecules 2018 Feb 9. Epub 2018 Feb 9.
    Macromolecular Engineering Laboratory, Department of Mechanical and Process Engineering, ETH Zürich , 8092 Zürich, Switzerland.
    Modern medicine, biological research, and clinical diagnostics depend on the reliable supply and storage of complex biomolecules. However, biomolecules are inherently susceptible to thermal stress and the global distribution of value-added biologics, including vaccines, biotherapeutics, and Research Use Only (RUO) proteins, requires an integrated cold chain from point of manufacture to point of use. To mitigate reliance on the cold chain, formulations have been engineered to protect biologics from thermal stress, including materials-based strategies that impart thermal stability via direct encapsulation of the molecule. Read More

    Visible Light-Induced Hydrogelation of an Alginate Derivative and Application to Stereolithographic Bioprinting Using a Visible Light Projector and Acid Red.
    Biomacromolecules 2018 Feb 2;19(2):672-679. Epub 2018 Feb 2.
    Shitennoji Senior High School , 1-11-73 Shitennoji, Tennoji, Osaka 543-0051, Japan.
    Visible light-induced hydrogelation is attractive for various biomedical applications. In this study, hydrogels of alginate with phenolic hydroxyl groups (Alg-Ph) were obtained by irradiating a solution containing the polymer, ruthenium II trisbipyridyl chloride ([Ru(bpy)]) and sodium persulfate (SPS), with visible light. The hydrogelation kinetics and the mechanical properties of the resultant hydrogels were tunable by controlling the intensity of the light and the concentrations of [Ru(bpy)]and SPS. Read More

    Large and Small Assembly: Combining Functional Macromolecules with Small Peptides to Control the Morphology of Skeletal Muscle Progenitor Cells.
    Biomacromolecules 2018 Feb 13. Epub 2018 Feb 13.
    Biofab3D, St. Vincent's Hospital , Fitzroy 3065, Australia.
    The material properties of natural tissues, such as skeletal muscle, are highly sophisticated and are synthetically challenging to mimic. Using natural biomacromolecules to functionalize self-assembled peptide (SAP) hydrogels has the potential to increase the utility of these materials by more closely reproducing the natural cellular environment. Here, to demonstrate that a conserved co-assembly pathway can retain distinct function, the biocompatible peptide derivative Fmoc-FRGDF was co-assembled with either a sulfated polysaccharide, fucoidan, or the provisional matrix proteoglycan, versican. Read More

    Broad-Spectrum Antibacterial Activity of Proteolytically Stable Self-Assembled αγ-Hybrid Peptide Gels.
    Biomacromolecules 2018 Feb 14. Epub 2018 Feb 14.
    Department of Chemistry, Indian Institute of Technology Ropar , Rupnagar 140001, Punjab, India.
    Bacterial infections pose a serious threat to mankind, and there is immense interest in the design and development of self-assembled peptide gels using ultrashort peptides for antibacterial applications. The peptide gels containing natural amino acids suffer from poor stability against proteolytic enzymes. Therefore, there is a need to design and develop peptide gels with improved stability against proteolytic enzymes. Read More

    Charged Metallopolymer-Grafted Silica Nanoparticles for Antimicrobial Applications.
    Biomacromolecules 2018 Feb 31;19(2):417-425. Epub 2018 Jan 31.
    Department of Pathology, Microbiology and Immunology, University of South Carolina, School of Medicine , Columbia, South Carolina 29209, United States.
    Inappropriate and frequent use of antibiotics has led to the development of antibiotic-resistant bacteria, which cause infectious diseases that are difficult to treat. With the rising threat of antibiotic resistance, the need to develop effective new antimicrobial agents is prominent. We report antimicrobial metallopolymer nanoparticles, which were prepared by surface-initiated reversible addition-fragmentation chain transfer polymerization of a cobaltocenium-containing methacrylate monomer from silica nanoparticles. Read More

    Structural Analysis of Polysaccharide Networks by Transmission Electron Microscopy: Comparison with Small-Angle X-ray Scattering.
    Biomacromolecules 2018 Feb 9. Epub 2018 Feb 9.
    Institute of Fundamental Sciences, Massey University , Palmerston North, New Zealand.
    Polysaccharide gels assembled from the anionic biopolymers pectin and carrageenan have been studied using transmission electron microscopy (TEM). Gels were formed in several different ways: for pectin, hydrogen bonding was used to form junction zones between strands, whereas for carrageenan systems, several different ion types were used to form ionotropic networks. Using this approach, several distinct network architectures were realized. Read More

    Photothermal Effect-Triggered Drug Release from Hydrogen Bonding-Enhanced Polymeric Micelles.
    Biomacromolecules 2018 Feb 12. Epub 2018 Feb 12.
    Key Laboratory of Polymer Ecomaterials, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , Changchun 130022, China.
    Incorporation of noncovalent interactions into hydrophobic cores of polymeric micelles provides the micelles with enhanced physical stability and drug loading efficiency, however, it also creates obstacles for drug release due to the strong interactions between carriers and drugs. Herein, a series of amphiphilic block copolymers based on poly(ethylene glycol)-b-poly(l-lysine) (mPEG-b-PLL) with similar chemical structures, while different hydrogen bonding donors (urethane, urea, and thiourea groups) are synthesized, and their capacities for codelivery of anticancer drug (e.g. Read More

    Macromolecular pHPMA-Based Nanoparticles with Cholesterol for Solid Tumor Targeting: Behavior in HSA Protein Environment.
    Biomacromolecules 2018 Feb 30;19(2):470-480. Epub 2018 Jan 30.
    Technische Universität München , Physik-Department, Physik weicher Materie, James-Franck-Str. 1, 85748 Garching, Germany.
    Nanoparticles (NPs) that form by self-assembly of amphiphilic poly(N-(2-hydroxypropyl)-methacrylamide) (pHPMA) copolymers bearing cholesterol side groups are potential drug carriers for solid tumor treatment. Here, we investigate their behavior in solutions of human serum albumin (HSA) in phosphate buffered saline. Mixed solutions of NPs, from polymer conjugates with or without the anticancer drug doxorubicin (Dox) bound to them, and HSA at concentrations up to the physiological value are characterized by synchrotron small-angle X-ray scattering and isothermal titration calorimetry. Read More

    Multivalent Polyaspartamide Cross-Linker for Engineering Cell-Responsive Hydrogels with Degradation Behavior and Tunable Physical Properties.
    Biomacromolecules 2018 Feb 30;19(2):691-700. Epub 2018 Jan 30.
    Department of Chemistry, School of Natural Science and ‡School of Materials Science and Engineering, Ulsan National Institute of Science and Technology , Ulsan 44919, South Korea.
    Hydrogels possess favorable physical properties ideally suited for various biotechnology applications. To tailor to specific needs, a number of modification strategies have been employed to tune their properties. Herein, a multifunctional polymeric cross-linker based on polyaspartamide is developed, which allows for the facile adjustment of the type and number of reactive functional groups to fit different reaction schemes and control the physical properties of the hydrogels. Read More

    Cyclodextrin-Functionalized Fiber Yarns Spun from Deep Eutectic Cellulose Solutions for Nonspecific Hormone Capture in Aqueous Matrices.
    Biomacromolecules 2018 Feb 2;19(2):652-661. Epub 2018 Feb 2.
    VTT Technical Research Centre of Finland Ltd , Biologinkuja 7, FI-02044 Espoo, Finland.
    A wood based yarn platform for capturing pharmaceutical molecules from water was developed. Cellulose fiber yarns were modified with cyclodextrins, and the capture of 17α-ethinyl estradiol (EE2), a synthetic estrogen hormone used as contraceptive, from water was tested. The yarns were prepared by spinning a deep eutectic solution (DES) of cellulose in choline chloride-urea. Read More

    Weak Hydrogen Bonds Lead to Self-Healable and Bioadhesive Hybrid Polymeric Hydrogels with Mineralization-Active Functions.
    Biomacromolecules 2018 Feb 5. Epub 2018 Feb 5.
    School of Materials Science and Engineering, South China University of Technology , Guangzhou 510640, People's Republic of China.
    Hydrogels with self-healing features that can spontaneously repair themselves upon mechanical damage are increasingly attractive for biomedical applications. Many attempts have been made to develop unique hydrogels possessing this property, as well as stimuli-responsiveness and biocompatibility; however, the hydrogel fabrication strategies often involve specific design of functional monomers that are able to optimally provide reversible physical or chemical interactions. Here, we report that weak hydrogen bonds, provided by oligo(ethylene glycol) methacrylate (OEGMA) and methacrylic acid (MAA), a monomer combination that is commonly used to prepare chemically cross-linking hydrogels, can generate self-healable hydrogels with mechanically resilient and adhesive properties through a facile one-step free radical copolymerization. Read More

    Biosynthesis and Characterization of Polyhydroxyalkanoates with Controlled Composition and Microstructure.
    Biomacromolecules 2018 Feb 9. Epub 2018 Feb 9.
    School of Chemical Engineering and Analytical Science, The Mill, The University of Manchester , Manchester M13 9PL, U.K.
    Volatile fatty acids (VFA) C2:0 to C6:0 were used as the sole carbon source for poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) production with controllable composition and microstructure in Haloferax mediterranei. Feeding carbon-even VFA gave >90 mol % poly(3-hydroxybutyrate) (3HB) PHBV, while carbon-odd VFA generated >87 mol % poly(3-hydroxyvalerate) (3HV) PHBV. Bespoke random, block, and blend copolymers with 0-100 mol % 3HV were synthesized using C4:0/C5:0 mixtures. Read More

    Matrix Metalloproteinase-9-Responsive Nanogels for Proximal Surface Conversion and Activated Cellular Uptake.
    Biomacromolecules 2018 Feb 8. Epub 2018 Feb 8.
    Department of Chemistry, ‡Molecular and Cellular Biology Program, §Center for Bioactive Delivery at the Institute for Applied Life Sciences, University of Massachusetts , Amherst, Massachusetts 01003, United States.
    Here, we have exploited the heightened extracellular concentration of matrix metalloproteinase-9 (MMP-9) to induce surface-conversional properties of nanogels with the aim of tumor-specific enhanced cellular uptake. A modular polymeric nanogel platform was designed and synthesized for facile formulation and validation of MMP-9-mediated dePEGylation and generation of polyamine-type surface characteristics through peptide N-termini. Nanogels containing MMP-9-cleavable motifs and different poly(ethylene glycol) corona lengths (350 and 750 g/mol) were prepared, and enzymatic surface conversional properties were validated by MALDI characterization of cleaved byproducts, fluorescamine assay amine quantification, and zeta potential. Read More

    In Vivo Coating of Bacterial Magnetic Nanoparticles by Magnetosome Expression of Spider Silk-Inspired Peptides.
    Biomacromolecules 2018 Feb 5. Epub 2018 Feb 5.
    Department of Molecular Structural Biology, Max Planck Institute of Biochemistry , D-82152 Martinsried, Germany.
    Magnetosomes are natural magnetic nanoparticles with exceptional properties that are synthesized in magnetotactic bacteria by a highly regulated biomineralization process. Their usability in many applications could be further improved by encapsulation in biocompatible polymers. In this study, we explored the production of spider silk-inspired peptides on magnetosomes of the alphaproteobacterium Magnetospirillum gryphiswaldense. Read More

    Zero-Order Release of Gossypol Improves Its Antifertility Effect and Reduces Its Side Effects Simultaneously.
    Biomacromolecules 2018 Jan 22. Epub 2018 Jan 22.
    State Key Laboratory of Medicinal Chemical Biology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) , Tianjin 300071, China.
    Gossypol was considered a promising male contraceptive but finally failed due to two side effects: hypokalemia and the irreversibility of its contraceptive effect. Here we demonstrate that sustained zero-order release could be a solution for these problems. The in vitro release of gossypol from gossypol/PEG layer-by-layer films follows a perfect zero-order kinetics. Read More

    Hierarchically Self-Assembled Supramolecular Host-Guest Delivery System for Drug Resistant Cancer Therapy.
    Biomacromolecules 2018 Feb 1. Epub 2018 Feb 1.
    Fujian Provincial Key Laboratory of Innovative Drug Target Research and State Key Laboratory of Cellular Stress Biology, School of Pharmaceutical Sciences, Xiamen University , Xiamen 361102, China.
    In this report, a new star-like copolymer β-CD-g-(PNIPAAm-b-POEGA), consisting of a β-CD core, grafted with temperature-responsive poly(N-isopropylacrylamide) (PNIPAAm) and biocompatible poly(oligo(ethylene glycol) acrylate) (POEGA) in a block copolymer of the arms, was used to deliver chemotherapeutics to drug resistant cancer cells and tumors. The first step of the self-assembly process involves the encapsulation of chemotherapeutics through host-guest inclusion complexation between the β-cyclodextrin cavity and the anticancer drug. Next, the chain interaction of the PNIPAAm segment at elevated temperature drives the drug-loaded β-CD-g-(PNIPAAm-b-POEGA)/PTX inclusion complex to hierarchically self-assemble into nanosized supramolecular assemblies at 37 °C, whereas the presence of poly(ethylene glycol) (PEG) chains in the distal end of the star-like copolymer arms impart enhanced stability to the self-assembled structure. Read More

    Cyclam-Modified PEI for Combined VEGF siRNA Silencing and CXCR4 Inhibition To Treat Metastatic Breast Cancer.
    Biomacromolecules 2018 Feb 19;19(2):392-401. Epub 2018 Jan 19.
    State Key Laboratory of Natural Medicines, Department of Pharmaceutics, China Pharmaceutical University , Nanjing, 210009, China.
    Chemokine receptor CXCR4 plays an important role in cancer cell invasion and metastasis. Recent findings suggest that anti-VEGF therapies upregulate CXCR4 expression, which contributes to resistance to antiangiogenic therapies. Here, we report the development of novel derivatives of polyethylenimine (PEI) that effectively inhibit CXCR4 while delivering anti-VEGF siRNA. Read More

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