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Chuntao Zhu, Fabian Itel, Rona Chandrawati, Xiaojun Han, Brigitte Städler
Multi-compartmentalized microreactors are considered as cell mimics with hierarchical structures inspired by mammalian cells. We report the successful assembly and encapsulation of purified nuclei from RAW 264.7 cells (pNuc) into alginate-based microreactors. We demonstrate the preserved function of nuclei within the microreactors for mRNA production. Further, we load catalase-loaded liposomes (Lcat) into the microreactors to break down hydrogen peroxide (H2O2) into oxygen and water. Assemblies containing both natural pNuc and synthetic Lcat show significantly higher mRNA production in the presence of H2O2 compared to microreactors without Lcat or no H2O2 present, suggesting a beneficial effect of the locally enzymatically produced oxygen for transcription...
September 19, 2018: Biomacromolecules
Sungjun Kim, Junhyung Kim, Gajendiran Mani, Minhyuk Yoon, Mintai P Hwang, Yadong Wang, Byung-Jae Kang, Kyobum Kim
Direct administration of bone morphogenetic protein-2 (BMP-2) for bone regeneration could cause various clinical side effects such as osteoclast activation, inflammation, adipogenesis, and bone cyst formation. In this study, thiolated gelatin/poly(ethylene glycol) diacrylate (PEGDA) interpenetrating (IPN) composite hydrogels were developed for guided skull bone regeneration. To promote bone regeneration, either polycation-based coacervates (Coa) or gelatin microparticles (GMPs) were incorporated within IPN gels as BMP-2 carriers...
September 19, 2018: Biomacromolecules
Shuai Liu, Huiting Jia, Jixiang Yang, Jianping Pan, Huiyun Liang, Liheng Zeng, Hao Zhou, Jiatong Chen, Tianying Guo
Cationic polymers have emerged as appealing non-viral gene vectors for decades, which however, suffer from the paradox between low molecular weight and high transfection efficacy. Low molecular weight cationic polymers (LCPs) are well cell tolerated, but are perplexed by orders-of-magnitude less efficacy compared to their macromolecular counterparts. The deficiency mainly lies in weak DNA binding of polymers and difficulty in endosomal escape of formulated polyplexes. Herein, we demonstrate that through zinc (Zn) coordinated modification of LCPs, the high transfection efficiency and low molecular weight (thus low cytotoxicity) can be achieved simultaneously...
September 19, 2018: Biomacromolecules
Valeria Castelletto, Ian W Hamley, Jani Seitsonen, Janne Ruokolainen, Gemma Harris, Kathrin Bellmann-Sickert, Annette G Beck-Sickinger
The gastric peptide hormone human PYY3-36 is a target for the development of therapeutics, especially for treatment of obesity. The conformation and aggregation behaviour of PEGylated and lipidated derivatives of this peptide is examined using a combination of fluorescence dye assays, circular dichroism (CD) spectroscopy, analytical ultracentrifugation (AUC) measurements, small-angle x-ray scattering (SAXS) and cryogenic-transmission electron microscopy (cryo-TEM). The behaviour of two PYY3-36 derivatives lipidated (with octyl chains) in different positions is compared to that of two derivatives with PEG attached at different residues and to that of the native peptide...
September 19, 2018: Biomacromolecules
Filippo Pierini, Paweł Nakielski, Olga Urbanek, Sylwia Pawłowska, Massimiliano Lanzi, Luciano De Sio, Tomasz Aleksander Kowalewski
Materials for the treatment of cancer have been studied comprehensively over the past few decades. Among the various kinds of biomaterials, polymer-based nanomaterials represent one of the most interesting research directions in nanomedicine, because their controlled synthesis and tailored designs make it possible to obtain nanostructures with biomimetic features and outstanding biocompatibility. Understanding the chemical and physical mechanisms behind the cascading stimuli-responsiveness of "smart" polymers is fundamental for the design of multifunctional nanomaterials to be used as photothermal agents for targeted polytherapy...
September 19, 2018: Biomacromolecules
James D Tang, Steven R Caliari, Kyle J Lampe
Coacervates have enormous potential due to their diverse functional properties supporting a wide number of applications in personal care products, pharmaceuticals, and food processing. Normally, separation of coacervate phases is induced by changes in pH, ionic strength, and/or polyelectrolyte concentration. This study investigates the microphase separation and coacervate complex formation of two natural polyelectrolytes, elastin-like polypeptides (ELPs) and hyaluronic acid (HA), as simple models for biological coacervates...
September 19, 2018: Biomacromolecules
Eva Koziolová, Libor Kostka, Lenka Kotrchová, Vladimír Šubr, Rafal Konefal, Benjamin Nottelet, Tomáš Etrych
We developed a new simplified method for the synthesis of well-defined linear, diblock, or starlike N-(2-hydroxypropyl)methacrylamide (HPMA)-based polymer drug carriers using controlled reversible addition-fragmentation chain transfer polymerization. The prepared monodispersed polymers are after the drug attachment intended for enhanced anticancer therapy. This new approach significantly reduces the number of required synthetic steps and minimizes the consumption of organic solvents during the synthesis. As a result, highly defined linear, diblock, and starlike copolymers designed for pH-triggered drug activation/release in tumor tissue were formed in sufficient amounts for further physicochemical and biological studies...
September 19, 2018: Biomacromolecules
Andrea Belluati, Ioana Craciun, Juan Liu, Cornelia G Palivan
Compartmentalization at the nanoscale is fundamental in nature, where the spatial segregation of biochemical reactions within cells ensures optimal conditions for regulating metabolic pathways. Here, we present a nature-inspired approach to engineer enzymatic cascade reactions taking place between separate vesicular nanocompartments (polymersomes), each containing one enzyme type. We propose, by the selected combination of enzymes, an efficient solution to detoxify the harmful effect of uric acid and prevent the accumulation of the derived H2 O2 , both being associated with various pathological conditions (e...
September 19, 2018: Biomacromolecules
Vinh X Truong, Fanyi Li, John S Forsythe
On-demand photo-uncaging of reactive thiols have been employed in engineering biomaterial scaffolds for regulation of cellular activities. A drawback of the current photo-uncaging chemistry is the utilization of high energy UV light or 2-photon laser light, which may be harmful to cells and cause undesired side reactions within the biological environment. We introduce an effective approach for the caging of thiol using monobromobimane, which can be removed under irradiation of light at λ = 420 nm and in the presence of electrophiles, such as acrylate, propiolate and maleimide, for trapping of the newly release thiol...
September 18, 2018: Biomacromolecules
Xue-Mei Che, Dai-Xu Wei, Guo-Qiang Chen
Poly( R-3-hydroxybutyrate- co- R-3-hydroxyhexanoate) (PHBHHx), a family member of microbial polyhydroxyalkanoates (PHA), is a biodegradable and biocompatible material with some hydrophobicity and reasonable strength for packaging and tissue engineering applications. In this study, superhydrophobic PHBHHx is fabricated via a simple nonsolvent-assisted process. The material can absorb all tested hydrophobic solvents and oil up to 6-fold of the material weights from water, permitting applications for cleaning environmental oil or solvent pollutions with convenience of disposal after the usage due to its biodegradability...
September 18, 2018: Biomacromolecules
Manoj B Parmar, Remant Bahadur K C, Raimar Löbenberg, Hasan Uludag
Small interfering RNA (siRNA) delivered to silence overexpressed genes associated with malignancies is a promising targeted therapy to decrease the uncontrolled growth of malignant cells. To create potent delivery agents for siRNA, here we formulated additive polyplexes of siRNA using linoleic acid-substituted polyethylenimine and additive polymers (hyaluronic acid, polyacrylic acid, dextran sulfate and methyl cellulose), and characterized their physicochemical properties and effectiveness. Incorporating polyanionic polymer along with anionic siRNA in polyplexes was found to decrease the ζ-potential of polyplexes, but enhance the cellular delivery of siRNA...
September 17, 2018: Biomacromolecules
Josefine Morgenstern, Gabriela Gil Alvaradejo, Nicolai Bluthardt, Ana Beloqui, Guillaume Delaittre, Jürgen Hubbuch
Covalent attachment of synthetic polymers to proteins, known as protein-polymer conjugation, is currently one of the main approaches for improving the physicochemical properties of these biomolecules. The most commonly employed polymer is polyethylene glycol (PEG), as evidenced by extensive research and clinical track records for its use in biopharmaceuticals. However, the occurrence of allergic reactions or hypersensitivity and the discovery of PEG antibodies, on the one hand, and the rise of controlled polymerization techniques and novel monomers, on the other hand, have been driving the search for alternative polymers for bioconjugation...
September 17, 2018: Biomacromolecules
Fei Xu, Megan Dodd, Heather Sheardown, Todd Hoare
A reactive electrospinning strategy is used to fabricate viable and proliferative cell-loaded nanofibrous hydrogel scaffolds in a single step using an all-aqueous approach. In situ-gelling and degradable hydrazone-crosslinked poly (oligo ethylene glycol methacrylate)-based hydrogel nanofibrous networks can be produced directly in the presence of cells to support long-term cell viability, adhesion, and proliferation, in contrast to bulk hydrogels of the same composition. Furthermore, the capacity of the gel nanofibers to retain bound water maintains this high cell viability and proliferative capacity following a freeze/thaw cycle without requiring any cryoprotectant additives, ideal properties for ready-to-use functional tissue patches...
September 17, 2018: Biomacromolecules
Hui Yao, Linping Wu, Guo-Qiang Chen
With increasing demand of environmentally friendly materials, development on bio-based polymers such as polyhydroxyalkanoate (PHA) is indispensable. An unsaturated PHA, namely, poly(3-hydroxydodecanoate-co-3-hydroxy-9-decenoate), short as P(3HDD-co-3H9D), provides possibilities for functionalization. Two different strategies are explored for synthesis of PHA-graft-graphene nanocomposites with graphene content ranging from 0.2 to 1.5 vol%. Chemical structures of intermediates and products were confirmed by Fourier transform infrared spectroscopy (FTIR) and nuclear magnetic resonance (NMR)...
September 17, 2018: Biomacromolecules
Naohiko Shimada, Taira Sasaki, Takakuni Kawano, Atsushi Maruyama
Thermoresponsive polymers exhibiting upper critical solution temperature (UCST)-type behavior under physiologically relevant conditions have potential as biomaterials. The phase separation temperature ( Tp ) of the UCST-type polymers can be increased by copolymerization with hydrophobic comonomers. Quantitative index parameters that could be used to rationally tune the Tp are lacking, however. We have reported that ureido copolymers such as poly(allylamine- co-allylurea) (AM-PU) and poly(l-ornithine- co-citrulline) exhibit UCST-type solution behavior under physiologically relevant conditions...
September 14, 2018: Biomacromolecules
Mao Hori, Horacio Cabral, Kazuko Toh, Akihiro Kishimura, Kazunori Kataoka
Polyion complex vesicles (PICsomes) formed from a self-assembly of an oppositely charged pair of block- and homo-polyelectrolytes have shown exceptional features for functional loading of bioactive agents. Nevertheless, the stability of PICsomes is often jeopardized in a physiological environment, and only PICsomes having chemically cross-linked membranes have endured in harsh in vivo conditions, such as in the bloodstream. Herein, we developed versatile PICsomes aimed to last in in vivo settings by stabilizing their membrane through a combination of ionic and hydrogen bonding, which is widely found in natural proteins as a salt bridge, by controlled introduction of guanidinium groups in the polycation fraction toward concurrent polyion complexation and hydrogen bonding...
September 14, 2018: Biomacromolecules
Xun Han, Dylan W Domaille, Benjamin D Fairbanks, Liangcan He, Heidi R Culver, Xinpeng Zhang, Jennifer N Cha, Christopher N Bowman
Due to the ability to generate oligomers of precise sequence, sequential and stepwise solid-phase synthesis has been the dominant method of producing DNA and other oligonucleotide analogues. The requirement for a solid support, however, and the physical restrictions of limited surface area thereon significantly diminish the efficiency and scalability of these syntheses, thus negatively affecting the practical applications of synthetic polynucleotides and other similarly created molecules. By employing the robust photo-initiated thiol-ene click reaction, we developed a new generation of clickable nucleic acids (CNAs) with a polythioether backbone containing repeat units of 6 atoms, matching the spacing of the phosphodiester backbone of natural DNA...
September 13, 2018: Biomacromolecules
Fataneh Karandish, Babak Mamnoon, Li Feng, Manas K Haldar, Lang Xia, Kara N Gange, Seungyong You, Yongki Choi, Kausik Sarkar, Sanku Mallik
Chemotherapeutic agents for treating cancers show considerable side effects, toxicity, and drug resistance. To mitigate the problems, we designed nucleus-targeted, echogenic, stimuli-responsive polymeric vesicles (polymersomes) to transport and subsequently release the encapsulated anticancer drugs within the nuclei of pancreatic cancer cells. We synthesized an alkyne-dexamethasone derivative and conjugated it to N3 -polyethylene glycol (PEG)-polylactic acid (PLA) copolymer employing the Cu2+ catalyzed "Click" reaction...
September 13, 2018: Biomacromolecules
Markus Selin, Sami Nummelin, Jill Deleu, Jarmo Ropponen, Tapani Viitala, Manu Lahtinen, Jari Koivisto, Jouni Hirvonen, Leena Peltonen, Mauri A Kostiainen, Luis M Bimbo
Pharmaceutical nanosuspensions are formed when drug crystals are suspended in aqueous media in the presence of stabilizers. This technology offers a convenient way to enhance the dissolution of poorly water-soluble drug compounds. The stabilizers exert their action through electrostatic or steric interactions, however, the molecular requirements of stabilizing agents have not been studied extensively. Here, four structurally related amphiphilic Janus-dendrimers were synthesized and screened to determine the roles of different macromolecular domains on the stabilization of drug crystals...
September 12, 2018: Biomacromolecules
Bing Xue, Veronika Kozlovskaya, Mohammad Asif Sherwani, Sithira Ratnayaka, Shahriar Habib, Theron Anderson, Marina Manuvakhova, Lidija Klampfer, Nabiha Yusuf, Eugenia Kharlampieva
Conjugation of bioactive targeting molecules to nano- or micrometer-sized drug carriers is a pivotal strategy to improve their therapeutic efficiency. Herein, we developed pH- and redox-sensitive hydrogel particles with a surface-conjugated cancer cell targeting ligand for specific tumor-targeting and controlled release of the anticancer drug doxorubicin. The poly(methacrylic acid) (PMAA) hydrogel cubes of 700 nm and 2 μm with a hepsin-targeting (IPLVVPL) surface peptide are produced through multilayer polymer assembly on sacrificial cubical mesoporous cores...
September 12, 2018: Biomacromolecules
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