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Collette, Elisabeth Anne. "Synthesis and Characterization of Amphiphilic Polymers." University of Akron / OhioLINK, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=akron1386959114.
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Njikang, Gabriel. "Interfacial Properties of Amphiphilic Dendritic Polymers." Thesis, University of Waterloo, 2006. http://hdl.handle.net/10012/1232.
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The self-assembly behavior of arborescent polystyrene-graft-poly(ethylene oxide) copolymers (PS-g-PEO) at the air-water interface and the solubilization/release properties of arborescent polystyrene-graft-poly(2-vinylpyridine) (PS-g-P2VP) copolymers were investigated. These amphiphilic dendritic molecules are covalently bonded unimolecular micelles incorporating a highly branched hydrophobic polystyrene core surrounded by a hydrophilic poly(ethylene oxide) or poly(2-vinylpyridine) shell. Molecules of PS-g-PEO copolymers spontaneously formed supramolecular assemblies at the air-water interface. The type of superstructures formed was found to depend upon copolymer composition, while the level of association was more directly related to the branching density of the polymers. At low surface pressures the PEO segments apparently remained adsorbed on the water subphase, but desorbed into water at very high surface pressures, in the condensed monolayer state. Controlled degradation of the PEO chains with UV light greatly enhanced molecular association, resulting in the formation of either large clusters or long ribbon-like superstructures. The PS-g-P2VP copolymers were found to efficiently solubilize and release hydrophobic small molecules in aqueous media. The partition coefficient and solubilization capacity of the copolymers for hydrophobic polyaromatic hydrocarbons increased with the polystyrene content of the copolymers, while the rate of solubilization decreased with increasing branching functionality of the copolymers. The release profiles for two model drugs displayed an initial burst in release followed by gradual approach to equilibrium. The diffusion coefficients of the drugs in the micelles increased with the branching functionality and the generation number of the micelles, presumably due to increased electrostatic repulsions of the protonated vinylpyridine units.
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Capuano, G. "AMPHIPHILIC, BIODEGRADABLE ANDBIOCOMPATIBLE POLYMERS FOR INDUSTRIALAPPLICATIONS." Doctoral thesis, Università degli Studi di Milano, 2017. http://hdl.handle.net/2434/477898.
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The aim of this PhD work was to establish the synthetic procedures for new families of biocompatible and biodegradable and/or bioeliminable biomaterials that can be differently processed to obtain nanoparticles, core-shell nanofibres and hydrogel slabs or conduits, respectively. Depending on composition, size and morphology, these biomaterials may be intended for applications as drug delivery systems and/or tissue regeneration.
Specifically, the research project has been developed along two main lines:
• Synthesis of poly(lactic-glycolic acid)-g-poly(1-vinylpyrrolidin-2-one) (PLGA-g-PVP) copolymers whose architecture consisted of a long PLGA backbone with oligomeric PVP pendants. These were obtained by the radical polymerisation of 1-vinylpyrrolidin-2-one in molten PLGA 50:50, acting as chain transfer agent. The procedure was a single pot - single step one. Copolymers were characterized by FTIR, 1H- and 13C-NMR and thermal analyses. They were saponified giving, besides PLGA degradation products, also un-degraded PVP. This was isolated and analysed by size exclusion chromatography, to evaluate the molecular weights of grafted PVP chains. MALDI-TOF analysis allowed identifying the chemical structure of PVP terminals and unambiguously establishing that PVP chains had been grafted onto PLGA backbone
PLGA-g-PVP with different PVP content were formulated as drug nanocarriers by different procedures. Doxorubicin-loaded nanoparticles were prepared by the solvent diffusion method and fully characterised. In vitro drug release kinetics were studied and in vitro biological activity evaluated on several antitumoral cell lines.
PLGA-g-PVP were also used as coatings of lipid nanocapsules for the delivery of curcumin and artemisinin as antimalarials. Drug loaded-lipid micro-dispersions were first prepared by oil in water emulsion. The lipid drops were converted into nanometric ones by high pressure homogenization and finally surface coated by adding a DMSO/acetone PLGA-g-PVP solution. Growth inhibition assay were conducted on plasmodium falciparum (3D7) cultures. Haemoltic assays were conducted on healthy red blood cells.
PLGA-g-PVP- and PLGA-based scaffolds consisting of nanofibrous mats were produced by electrospinning. Starting materials were electrospun and their morphology was evaluated by scanning electron microscopy and wettability by contact angle measurements. Coaxial electrospinning of two materials, in which PLGA formed the core and PLGA-g-PVP the shell of fibres, were also conducted and compared with those obtained by mixed solutions of staritng materials. Chemical composition was evaluated by TGA, morphology by scanning electron microscopy and wettability by contact angle measurements. Nanofabric scaffold produced will be evaluated for drug release and tissue engineering applications.
• Synthesis of a new classes of poly(saccharide)-poly(aminoamine)s 3D-network intended as scaffolds for the regeneration of liver.
In particular, hyaluronic acid-polyamidoamine and hyaluronic acid-gelatin- polyamidoamine hydrogels were synthesised by amidation reaction between the carboxylic acid group of hyaluronic acid and amine groups of gelatin and or an NH2-functionalized PAA, promoted by 4-(4,6-dimethoxy-1,3,5-triazin-2-yl)-4-methylmorpholinium chloride (DMTMM) as coupling agent. Chemical-physical characterization were carried out on hydrogels. In order to promote hepatic cell proliferation serotonin was bonded to both hydrogels, adding it to the initial recipe, exploiting the above reaction between carboxylic acid group of hyaluronic acid and amine group of serotonin. Serotonin-loaded hydrogels were tested in vitro to evaluate biological efficacy.
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Kilbinger, Andreas Felix Michael. "Self-organising amphiphilic oligothiophene block co-polymers." Thesis, Durham University, 1999. http://etheses.dur.ac.uk/4389/.
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A new route to oligothiophene-PEO-block-co-polymers has been developed, in which well-defined a-oligothiophene blocks (from bithiophene to sexithiophene) alternate with poly(ethylene oxide) blocks. These materials show high solubility in common organic solvents. Sexithiophene derivatives with short PEO chains attached at the a-positions have been synthesised as model systems for the above sexithiophene polymer. PEO side-chains as short as pentaethylene glycol had a good solubilising effect on the otherwise insoluble sexithiophene. All compounds prepared exhibited surface activity, as shown by monolayer experiments on a Langmuir trough. Sexithiophene model compounds with short PEO side-chains could be compressed to form a two-dimensional condensed phase. X-ray diffraction of melt cast films of the oligothiophene polymers showed that a minimum oligothiophene block-length of five thiophenes (pentathiophene) was necessary to fully disturb PEO crystallisation. The sexithiophene polymer formed regions of crystalline/aggregated sexithiophene in the bulk. UV/Vis and fluorescence studies in solution indicated that the oligothiophene segments were molecularly dissolved in good solvents like chloroform. Aggregation of the oligothiophenes occurred in THF/water mixtures, which was consistent with observed shifts of the UV absorption maxima towards the blue and quenching of the fluorescence. An oligothiophene length of four thiophenes (quaterthiophene) was necessary to observe this aggregation phenomenon. A sexithiophene derivative with chiral pentaethylene glycol side chains showed a large circular dichroism effect in aqueous solution and no effect in chloroform solution, indicating the formation of a chiral superstructure upon aggregation.
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Wang, Yi. "The Synthesis and Characterization of Amphiphilic Poly(Ethylene Oxide)-Block-Poly(Octadecyl Acrylate) Block Copolymers." University of Akron / OhioLINK, 2014. http://rave.ohiolink.edu/etdc/view?acc_num=akron1399491109.
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ZHOU, YIFAN. "SELF-ASSEMBLY AND SELF-RECOGNITION BEHAVIORS OF AMPHIPHILIC MACROMOLECULES IN SOLUTION." University of Akron / OhioLINK, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=akron1619093496152417.
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Alexander, Nicolas Edward. "Multidimensional Mass Spectrometry of Amphiphilic Systems." University of Akron / OhioLINK, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=akron1532773038466757.
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Roebuck, Deborah Anne. "Investigation into synthetic amphiphilic polymers for intracellular delivery." Thesis, Imperial College London, 2015. http://hdl.handle.net/10044/1/32273.
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Delivery of siRNA therapeutics to their target site within the cell interior is a challenge that hinders their effective use in disease treatment. PP-75, a pH-responsive polymer, demonstrates potential to enhance intracellular siRNA-delivery by overcoming endosomal entrapment. PP-75 also provides a promising platform for development of targeted delivery, following conjugation of DARPin targeting ligands. Novel PP-75 cross-linker derivatives, PP-75-aminofluorescein, PP-75-siRNA and PP-75-DARPin conjugates have been developed and characterised for in vitro application. PP-75 delivery to SK-BR-3 (Her2+) and MDA-MB-231 (Her2-) breast cancer cells has been demonstrated for the first time. The membrane-lytic activity of PP-75 was limited at physiological pH but effective within the pH range typical of early endosomes. PP-75 did not demonstrate cytoxicity, with cells tolerating treatments up to 2.5 mg/mL over 72 h. Cellular internalisation and endosomal escape of PP-75 aminofluorescein (AFC) was confirmed via confocal microscopy, demonstrated by diffuse cytoplasmic delivery. Flow cytometry confirmed cellular internalisation of PP-75 AFC was via endocytosis. As reporter cells expressing firefly and Renilla luciferases, the breast cancer lines offered a robust assay read out capable of distinguishing between target specific and non-specific gene knockdown. The functionality of novel siRNA payloads that targeted firefly luciferase was confirmed by mRNA and protein knockdown and provided the foundation for delivery of PP-75 siRNA conjugates. Target specific DARPin affinity was confirmed for the SK-BR-3 (Her2+) cells and not MDA-MD-231 (Her2-) cells, demonstrating selective binding to the extracellular Her2 protein. The expression of a novel but structurally comparable negative control DARPin (5K D1) demonstrated no affinity for either cell line. The introduction of a free cysteine residue to the DARPin sequences facilitated attachment onto PP-75. PP-75 therefore has the potential to demonstrate intracellular delivery of siRNA payloads, capable of delivery to specific cell populations via DARPin targeting.
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Vandevoorde, Colleen A. (Colleen Anne). "Amphiphilic star polymers as solubilizing agents for environmental spearations." Thesis, Massachusetts Institute of Technology, 1996. http://hdl.handle.net/1721.1/10635.
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Rhyner, Matthew N. "Development of cancer diagnostics using nanoparticles and amphiphilic polymers." Diss., Atlanta, Ga. : Georgia Institute of Technology, 2008. http://hdl.handle.net/1853/22582.
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Thesis (Ph. D.)--Biomedical Engineering, Georgia Institute of Technology, 2008.Committee Chair: Nie, Shuming; Committee Member: Bao, Gang; Committee Member: Chung, Leland; Committee Member: Murthy, Niren; Committee Member: Prausnitz, Mark.
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Watt, Shannon L. "Synthesis and Characterization of Regioregular, Amphiphilic Semifluoroalkyl-Substituted Polythiophenes and Cofacial Bis(oligothienyl)naphthalenes." Diss., Georgia Institute of Technology, 2007. http://hdl.handle.net/1853/19787.
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Conjugated polymers and oligomers have been widely studied based on their wide range of useful properties and applications. Given the importance of self-assembly and charge transfer in the development of conjugated materials for use in electronic applications, it is crucial to: (i) prepare functional materials by molecular design, (ii) evaluate the structure-property relationships of new materials, and (iii) develop fundamental understanding of electronic structure and charge transport behavior.
The use of conjugated polymeric materials in electronic applications relies on control of the assembly and orientation of the polymer chains in the solid state. Conjugated polymers with liquid crystalline behavior could be used to implement an additional level of control over orientation and resultant properties. Substitution of the conjugated polythiophene backbone with semifluoroalkyl side chains (i.e., the diblock -(CH2)m(CF2)nF) has afforded materials with unusual properties. The mutual immiscibility of the aromatic backbone, the alkyl side-chain segments, and the fluoroalkyl side-chain termini provides control over supramolecular packing. A series of eight polymers has been synthesized, in which the lengths of the alkyl (m) and fluoroalkyl (n) segments are varied. One regiorandom analogue and two poly(3-alkylthiophene)s were also synthesized for comparative purposes. The structure, molecular weight, and regioregularity of the polymers were evaluated using a variety of techniques.
The semifluoroalkyl-substituted polymers have been systematically studied to determine the effect of side chain length and m:n block ratios on their solution state, liquid crystalline, and solid state properties. The effect of side chains on conjugation was determined, where solubility allowed, by solution-state UV-visible and fluorescence spectroscopy. The thermal and liquid crystalline properties of the homopolymers were evaluated by DSC, variable-temperature X-ray diffraction, and polarized optical microscopy. Several semifluoroalkyl-substituted polythiophene homologues show liquid crystalline behavior.
Molecular packing and charge transport are key factors governing the use of conjugated materials in electronic applications. A wide variety of oligomers have been studied as models for charge migration in conjugated polymers. One-dimensional models do not adequately represent two-dimensional charge transport; thus, a variety of two-dimensional, covalently-linked models have been developed. Previous work by our group, and others, led to the proposal of bis(oligothienyl) compounds as models to study the interaction of the ð-conjugated chains. Previous reports by other researchers described the synthesis and characterization of hydrogen-terminated analogues of 1,8-bis(oligothienyl)naphthalenes. However, these materials proved to be unsuitable for use as charge transport models, as they were subject to irreversible polymerization upon oxidation. Installation of methyl groups at the terminal a-positions of 1,8-bis(oligothienyl)naphthalenes allowed us to create a series of models in which conjugated chains are held in close proximity. This provides access to multiple redox states, and future systems based on these molecules may be used as models for charge transport or as functional materials for incorporation into devices.
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Baker, James Stewart Jr. "Synthesis of Functional Vinylbenzocyclobutenes for Use as Crosslinkers in the Preparation of Amphiphilic Nanoparticles." University of Akron / OhioLINK, 2011. http://rave.ohiolink.edu/etdc/view?acc_num=akron1321304647.
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Balster, Russell. "Synthesis and characterisation of initiators and amphiphilic miktoarm star polymers." Thesis, Durham University, 2016. http://etheses.dur.ac.uk/11638/.
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This project involves the development of several novel heterofunctional initiators with a calix[4]arene centre that can facilitate a “core” first method for the synthesis of miktoarm star polymers. Chapter 1 introduces main concepts on calixarenes, single electron transfer living radical polymerisation and the ring opening polymerisation of ε-caprolactone. Chapter 2 describes the synthetic strategy employed for the synthesis of a novel A2B2 heterofunctional initiator that incorporated an alkyl halogen moiety and a primary hydroxyl. p-tert-butylcalix[4]arene was modified via a six step process to introduce the required functionality and was fully characterised at each stage using 1D and 2D NMR spectroscopy, ASAP MS and IR spectroscopy. Chapter 3 describes how the A2B2 heterofunctional initiator was used to synthesise a novel 2-armed PCL polymer centred on a calixarene core. This was further used for copper(0) mediated polymerisation of 2-hydroxyethylacrylate due to the alkyl halide moieties remaining in the calixarene core, leading to the formation of several amphiphilic A2B2 miktoarm star polymers. Both polymers were fully characterised using 1D and 2D NMR spectroscopy, SEC, DSC, TGA and IR spectroscopy. Chapter 4 describes the synthetic strategy employed for the synthesis of a novel A4B4 heterofunctional initiator that incorporated an alkyl halogen moiety and a primary hydroxyl. p-tert-butylcalix[4]arene was modified via a seven step process to introduce the required functionality and was fully characterised at each stage using 1D and 2D NMR spectroscopy, ASAP MS and IR spectroscopy. Chapter 5 describes how the A4B4 heterofunctional initiator was used to synthesise a novel 4-armed star PCL polymer centred on a calixarene core. This was further used for copper(0) mediated polymerisation of 2-hydroxyethylacrylate due to the alkyl halide moieties remaining in the calixarene core, leading to the formation of several amphiphilic A4B4 miktoarm star polymers. Both polymers were fully characterised using 1D and 2D NMR spectroscopy, SEC, DSC, TGA and IR spectroscopy. Chapter 6 described the self-assembly of A2B2 and A4B4 amphiphilic miktoarm star polymers calixarene-A2B2starPCL100PHEAm, 8-10, where m = 75, 100 and 270, respectively and calixarene-A4B4starPCL20PHEAm, 18, 19 and 20 where m = 10, 25 and 48, respectively). The TEM analysis on polymer systems 8 - 10 and 18 - 20, revealed spherical micelles, with the size of the micelle decreasing as the proportion of hydrophilic PHEA increased. The CMC determinations for polymers 8 – 10 revealed that the length of the hydrophilic chain does not appear to have a significant effect on the CMC. For polymers 18 – 20, the CMC increases as the length of the hydrophilic polymer chain increases. For both polymeric systems 8 - 10 and 18 - 20, low CMC values were calculated. This work showed the system has a potential in medical applications, with their ability to form micelles in the range of 5 to 110 nm and have the ability to encapsulate highly hydrophobic material, such as the fluorescent probe pyrene. In chapter 7 general conclusions and future perspectives for the work are discussed.
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Bansal, Kuldeep Kumar. "Novel amphiphilic polymers from renewable feedstock : synthesis, characterisation and applications." Thesis, University of Nottingham, 2015. http://eprints.nottingham.ac.uk/30858/.
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Development of novel biodegradable polymers from renewable resources has attracted attention due to the limitations associated with polymers obtained from petroleum resources. The objective of the work presented in this thesis was to develop various novel biodegradable amphiphilic block copolymers from commercially available sustainable feedstocks for drug delivery applications. Synthesis was performed using a reported method under mild reaction conditions. Renewable δ-decalactone was chosen as a key monomer to synthesise novel amphiphilic block copolymers via ROP using PEG as initiator. A diblock (i.e. mPEG-b-PDL) and a triblock (i.e. PDL-b-PEG-b-PDL) copolymer of poly(decalactone) (PDL) was synthesised and purified successfully. Additionally, a novel triblock copolymer (i.e. mPEG-b-PDL-b-PPDL) was synthesised using ω-pentadecalactone as monomer and mPEG-b-PDL as initiator via ROP to generate a copolymer with different physical properties. Further, a di-block copolymer of ε-caprolactone (i.e. mPEG-b-PCL) was synthesised for comparative studies with novel block copolymers. Micelles of synthesised block copolymers were fabricated using a reported nanoprecipitation method. Micelles fabricated from these novel block copolymers were of sizes <200nm and possessed low critical micelle concentration (CMC) values. Curcumin and Amphotericin B were successfully encapsulated in the novel block copolymer micelles via nanoprecipitation method. The results obtained from curcumin loading and release studies suggested that these novel PDL block copolymers could perform in similar fashion when compared with poly(caprolactone) (PCL) block copolymer micelles. However, in subsequent study micelle of mPEG-b-PDL gave high loading content compared to mPEG-b-PCL micelles when amphotericin B was used as a drug. Further, a preliminary in vitro degradation study of mPEG-b-PDL micelles was performed and the results proposed that the ester linkage of PDL chain were susceptible to hydrolytic degradation in physiological condition. Additionally, in vitro cytotoxicity studies performed on HCT-116 human colon cancer cells revealed that the novel mPEG-b-PDL micelles have similar toxicity profiles when compared to the well-established mPEG-b-PCL micelles. Ligand mediated targeting efficiency of novel diblock copolymer micelles was also studied for potential future applications in cancer therapy. Amphiphilic block copolymers using PEG and PDL were synthesised via click chemistry to generate functionalised block copolymers. Folic acid and rhodamine B were used as targeting ligand and tracker dye respectively. Mixed micelles fabricated from functionalised block copolymers (i.e. FA-PEG-b-PDL, RhB-PEG-b-PDL and mPEG-b-PDL) were tested on folate receptor positive (MCF-7 FR+ve) and folate receptor negative (A549 FR-ve) human cancer cell lines for receptor mediated endocytosis. The acquired confocal images demonstrated the nonspecific uptake of the PEG-b-PDL micelles formulations (targeted and non-targeted) in both cell lines selected in current study. The results obtained from this thesis study suggested that the synthesised novel PDL block copolymer micelles have potential to act as a novel drug delivery system. However, further studies have been proposed to explore the possible applications of these renewable block copolymers.
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Liu, Yuqing. "Synthesis and Characterization of Well-Defined, Amphiphilic, Ionic Copolymers." University of Akron / OhioLINK, 2011. http://rave.ohiolink.edu/etdc/view?acc_num=akron1318440986.
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Siew, Adeline Jing Leng. "Oral absorption enhancement of hydrophobic drugs by chitosan based amphiphilic polymers." Thesis, University College London (University of London), 2009. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.509402.
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Foster, Beth Mary. "Amphiphilic polymers for controlled release : synthesis, solution properties and release characteristics." Thesis, University of Bristol, 2009. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.549685.
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Amphiphilic polymers have long been known to display associative effects which can be exploited in controlled release applications. In particular, controlled drug delivery can benefit from the biocompatible nature of many polymers, as well as evidence of membrane affinity. This thesis describes the study of a series of amphiphilic polymers with potential for use in pharmaceutical applications. The work has ranged from development of new polymer structures with physical characteristics which may aid controlled release, through studies of polymer-drug association and disassociation in solution, to development of controlled release formulations incorporating the polymers. Novel polymers combining the controlled release potential of Pluronic triblock copolymers with that of cyclodextrins have been synthesised, via "Click Chemistry". The specificity and strong driving force behind this mechanism ensure that the molecules react covalently, to leave the cyclodextrin cavity free for complexation and controlled release of guest molecules. Commercial (unmodified) Pluronics have also been studied with drug molecules in solution, using small-angle neutron scattering and pulsed-field gradient NMR. Ibuprofen has been found to act as a cosurfactant for the Pluronic, causing an increase in aggregation but a decrease in the critical micelle concentration and temperature. Release of ibuprofen from the micelles may be triggered by an increase in solution pH, which influences the dynamic equilibrium of ibuprofen between the solution and micellar phases. Finally, new graft copolymers of polyisoprene and poly( ethylene oxide) have been found to display interesting behaviour in aqueous solution. Despite showing limited aqueous solubility, the polymers can be solubilised either by addition of other surfactant molecules, or by pre-dissolution in methanol, which is believed to enable the hydrophilic graft segments to orient outwards. The graft copolymers are capable of stabilising hydrophobic drug molecules in aqueous solution, and have also been successfully incorporated into controlled release formulations for drug delivery.
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Wang, Zeyu. "Amphiphilic Triblock Copolymers for 3D Printable and Biodegradable Hydrogels." University of Akron / OhioLINK, 2020. http://rave.ohiolink.edu/etdc/view?acc_num=akron1588277239478144.
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Sun, Hao-Jan. "Phase Behaviors and Janus Hierarchical Supramolecular Structures Based on Geometrically and Chemically Asymmetric Building Blocks." University of Akron / OhioLINK, 2012. http://rave.ohiolink.edu/etdc/view?acc_num=akron1333457824.
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Costanza, Frankie. "Design, Synthesis and Applications of Polymer Biomaterials." Scholar Commons, 2015. https://scholarcommons.usf.edu/etd/5462.
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The emergence of antibiotic resistant bacteria has prompted the research into novel kinds of antibacterial small molecules and polymers. Nature has solved this issue with the use of cationic antimicrobial peptides, which act as nonspecific antibiotics against invading species. Herein, we have tried to mimic this general mechanism in a biocompatible and biodegradable polymer micelle based on the polymerization of naturally occurring amino acids lysine and phenylalanine linked to a PEG tether. This amphiphilic structure allows for the spontaneous collapse into stable nanoparticles in solution, which contains a hydrophilic outer layer and a hydrophobic core. Our polymers have shown activity against clinically relevant strains including Methicillin Resistant S. epidermidis, B. subtilis, K. pneumoniae, and P. aeruginosa.
To further the application of our biopolymers, we have used them as drug delivery vehicles as well. First, we have used an anionic analogue based on glutamic acid to encapsulate a super hydrophobic drug Tanshinone IIA, and use it against a hepatoma bearing mouse model. Second, we have used a cationic analogue to form a complex with miRNA-139 and use it against a hepatoma bearing mouse model as well. In both cases, our PEG poly(amino acids)s have shown promising efficacy in drastically reducing the tumor size compared to the control only. Taken together, our results show that our nanoparticles have the potential to be versatile biomaterials as antibacterials as well as drug delivery vehicles in vivo.
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Chattopadhyay, Subrata [Verfasser]. "Multifunctional amphiphilic polymers, bearing azetidinium groups : synthesis and antimicrobial studies / Subrata Chattopadhyay." Aachen : Hochschulbibliothek der Rheinisch-Westfälischen Technischen Hochschule Aachen, 2014. http://d-nb.info/1059322595/34.
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Prasitnok, Khongvit. "Coarse-grained molecular modelling of amphiphilic polymers at a water/air interface." Thesis, Durham University, 2012. http://etheses.dur.ac.uk/5563/.
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Previous atomic-level simulations have been shown to provide invaluable insight into the adsorption behaviour of amphiphilic polymers at a water-air interface. Neutron reflectivity profiles generated from these simulations showed good agreement with experiment, particularly at low surface concentrations. Unfortunately, previous detailed atomistic simulations have failed to produce adequate results at high surface concentrations due to crowded configurations, which could not relax within the simulation times available. To tackle this problem, a coarse-graining (CG) technique, where the structure of the simulated molecule is simplified to a chain of beads, has been employed in this study. This provides for the simulation of larger time and length scales allowing for a more detailed study of the capture of polymer chains by a surface and the structure of surface layers. The work presented in this thesis involves development of coarse-grained models for water and for poly(ethylene oxide) (PEO)/water systems, with the aim of reproducing the properties of key importance for the bulk and liquid/vapour interfacial states. These models are then used in the coarse-grained simulation studies of di-and trifluoro dendritic end-capped PEO at an air-water interface; the amphiphilic polymers that have been studied recently by neutron reflectivity experiments. It is shown in this study that simulation of very large polymer chains comparable to that used in real experiments, is achievable using coarse-grained molecular dynamics. Neutron reflectivity profiles generated from simulations of di- and trifluoro dendritic end-capped PEO materials at low polymer concentrations are in good agreement with experiment data. Simulations at high polymer concentrations showed no evidence of a stretched brush structure, in accordance with experimental findings. It is shown from these simulations that there are polymers adsorbed to the interface by a combination of fluorocarbon ends and ethylene oxide segments,resulting in a rather at layer structure. At high surface concentrations of polymers, it proved possible to see the formation of polymer micelles in bulk water. The process of micelle capture by the surface and incorporation of the micelle contents into the surface, were also observed.
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Hoskins, Clare. "The use of novel poly(allylamine) based amphiphilic polymers for drug delivery." Thesis, Robert Gordon University, 2010. http://hdl.handle.net/10059/511.
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Fourteen novel comb shaped amphiphilic polymers were successfully synthesised to determine the effect of polymer architecture on the potential of these amphiphilic polymers for hydrophobic drug delivery. Polyallylamine (PAA) was grafted with four different types of hydrophobic pendant groups (Cholesteryl (Ch), (Fmoc), (Dansyl)and (Naphth)). Some amphiphilic polymers were further reacted with methyl orange to form quaternary ammonium moieties. The polymers were characterised by elemental analysis and nuclear magnetic resonance spectroscopy (NMR). In the aqueous environment the amphiphilic polymers formed nano self assemblies with particle size from 99 to 284 nm. The critical aggregation concentration (CAC) of the self assemblies was successfully determined by surface tension measurement. The CAC ranged from the lowest value of 0.093 to the highest 1.5 mgmL-1 (Ch5 and Fmoc5 respectively). The Fmoc and Naphth grafted polymers showed the presence of two CMC values, this phenomenon was due to stacking of the planar hydrophobic ring structures resulting in excimer formation. The theory of excimer formation was confirmed by the observation of peak shifting on the emission spectra of the compounds in water over a large concentration range (0.023 – 3 mgmL-1). The drug loading potential of the polymers was investigated using five model hydrophobic drugs, propofol, prednisolone griseofulvin, etoposide and novel anticancer agent BNIPDaoct. The Ch5 and Dansyl10 showed excellent drug solubilisation capacities. At 6 mgmL-1 the Ch5 achieved propofol solubility 70-fold greater than its aqueous solubility, prednisolone, griseofulvin and etoposide solubility’s were increased 20-fold, 30-fold and 7-fold respectively. Similarly at 6 mgmL-1 the Dansyl10 achieved a 200-fold increase on the aqueous solubility of propofol and increased the solubility of prednisolone, griseofulvin and etoposide by 100-fold and 400-fold and 12-fold respectively. The Ch5 (at 1 mgmL-1) was also used to solubilise the novel anticancer agent Bisnaphthalimidopropyl diaminooctane (BNIPDaoct) which was otherwise insoluble achieving a solubilisation of 0.3 mgmL-1. The sizes of the optimal formulations differed greatly for both modified polymers. This was possibly due to the varying architectures of both the drug and the modified polymers and their ability to expand the hydrophobic core and shield the drugs from the ‘hostile’ aqueous environment. The in vitro drug release profiles, showed controlled release of the hydrophobic drugs from the core of the nano aggregates (Ch5 and Dansyl10), the time span for 100% of the drugs to be released ranged from 48- 96 h. Biological characterisation of the polymers found that most of the polymers showed negligible haemolytic activity over the concentrations tested (0.05 – 1 mgmL-1), the IC50 values for the cytotoxicity assay ranged from 0.01740 - 0.05585 mgmL-1 on Caco-2 cells (Fmoc5 to QCh5 respectively). The quaternized polymers showed a slightly better safety profile than their unquaternized counterparts, despite exhibiting low drug solubilisation capacities. The optimal formulations of Ch5 and Dansyl10 loaded with etoposide and BNIPDaoct were tested for their cytotoxicity in vitro on Caco-2 and HEK293 cells. All formulations were capable of lowering the IC50 values when compared with the free anticancer drugs, thus increasing their therapeutic effect. The Ch5 decreased the solubility of etoposide 2.2-fold and BNIPDaoct 1.3-fold on Caco-2 cells, with Dansyl10 achieving a 14 -fold and 16–fold reduction respectively. In vivo oral administration of Ch5 and Dansyl10, griseofulvin formulations demonstrated significantly enhanced the absorption of griseofulvin absorption in rats compared with griseofulvin in water (8.89-fold and 5.20-fold increase respectively on total concentration of griseofulvin solubilised over 24 h study). A formulation of Ch5, BNIPDaoct was also shown to significantly decrease the tumour growth when treated on tumour bearing nude mice over a 4 week period. This is the first time these novel PAA’s grafted with cholesteryl and dansyl have shown promising potential in hydrophobic drug delivery.
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Hevus, Ivan. "Amphiphilic Invertible Polymers: Self-Assembly into Functional Materials Driven by Environment Polarity." Diss., North Dakota State University, 2012. https://hdl.handle.net/10365/26814.
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Stimuli-responsive polymers adapt to environmental changes by adjusting their chain conformation in a fast and reversible way. Responsive polymeric materials have already found use in electronics, coatings industry, personal care, and bio-related areas. The current work aims at the development of novel responsive functional polymeric materials by manipulating environment-dependent self-assembly of a new class of responsive macromolecules strategically designed in this study, – amphiphilic invertible polymers (AIPs). Environment-dependent micellization and self-assembly of three different synthesized AIP types based on poly(ethylene glycol) as a hydrophilic fragment and varying hydrophobic constituents was demonstrated in polar and nonpolar solvents, as well as on the surfaces and interfaces. With increasing concentration, AIP micelles self-assemble into invertible micellar assemblies composed of hydrophilic and hydrophobic domains. Polarity-responsive properties of AIPs make invertible micellar assemblies functional in polar and nonpolar media including at interfaces. Thus, invertible micellar assemblies solubilize poorly soluble substances in their interior in polar and nonpolar solvents. In a polar aqueous medium, a novel stimuli-responsive mechanism of drug release based on response of AIP-based drug delivery system to polarity change upon contact with the target cell has been established using invertible micellar assemblies loaded with curcumin, a phytochemical drug. In a nonpolar medium, invertible micellar assemblies were applied simultaneously as nanoreactors and stabilizers for size-controlled synthesis of silver nanoparticles stable in both polar and nonpolar media. The developed amphiphilic nanosilver was subsequently used as seeds to promote anisotropic growth of CdSe semiconductor nanoparticles that have potential in different applications ranging from physics to medicine. Amphiphilic invertible polymers were shown to adsorb on the surface of silica nanoparticles strongly differing in polarity. AIP modified silica nanoparticles are able to adsolubilize molecules of poorly water-soluble 2-naphthol into the adsorbed polymer layer. The adsolubilization ability of adsorbed invertible macromolecules makes AIP-modified silica nanoparticles potentially useful in wastewater treatment or biomedical applications. Finally, the invertible micellar assemblies were used as functional additives to improve the appearance of electrospun silicon wires based on cyclohexasilane, a liquid silicon precursor. AIP-assisted fabrication of silicon wires from the liquid cyclohexasilane precursor has potential as a scalable method for developing electronic functional materials.
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O'Neill, Jason Michael. "Multidimensional Mass Spectrometry Studies on Amphiphilic Polymer Blends and Cross-Linked Networks." University of Akron / OhioLINK, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=akron1624375174939496.
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Gide, Mussie. "Design, Synthesis, Application of Biodegradable Polymers." Scholar Commons, 2018. https://scholarcommons.usf.edu/etd/7625.
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Bacterial infections have posed a serious threat to the public health due to the significant rise of the infections caused by antibiotic-resistant bacteria. There has been considerable interest in the development of antimicrobial agents which mimic the natural HDPs, and among them biodegradable polymers are newly discovered drug candidates with ease of synthesis and low manufacture cost compared to synthetic host defense peptides. Herein, we present the synthesis of biocompatible and biodegradable polymers including polycarbonate polymers, unimolecular micelle hyperbranched polymers and dendrimers that mimic the antibacterial mechanism of HDPs by compromising bacterial cell membranes. The developed amphiphilic polycarbonates are highly selective to Gram-positive bacteria, including multidrug-resistant pathogens and the unimolecular micelle hyperbranched polymers showed promising broad-spectrum activity. However, lipidated amphiphilic dendrimers with low molecular weight display potent and selective antimicrobial activity against both Gram-positive and Gram-negative bacteria, including multidrug-resistant strains. In addition to antibacterial activity against planktonic bacteria, these dendrimers were also shown to inhibit bacterial biofilms effectively. These class of polymers may lead to a useful generation of antibiotic agents with practical applications.
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Nimmagadda, Alekhya. "Design, Synthesis, Applications of Polymers and Dendrimers." Scholar Commons, 2017. https://scholarcommons.usf.edu/etd/7430.
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WHO has reported that antibiotic resistance is the third major cause of human death all over the globe. Recent study, has focused on the development of new antibacterial resistance drugs. Herein, we tried to synthesis a series of polymers that can mimic the HDPs. HDPs can target the bacterial cell membrane and they have less chances to develop bacterial resistance. We synthesized the amphiphilic polycarbonates that are highly selective to Gram-positive bacteria, including multidrug resistant pathogens. The membrane disruption activity of these polymers was proved by fluorescence and TEM studies and the drug resistance study showed that the polymers don’t develop bacterial resistance. In order to further design the molecules that can target a broad spectrum of bacteria, we have designed a series of lipidated dendrimers that can target the Gram-positive and Gram-negative bacteria. These dendrimers mimic the HDPs and target the bacterial cell membrane. Dendrimers are reported to inhibit the formation of bacterial biofilm which makes them promising for their future development of antibiotic agents.
Apart from the synthesis of polymers and dendrimers as antibacterial agents, we have designed a series of small molecular antibacterial agents that are based on the acylated reduced amide scaffold and small dimeric cyclic guanidine derivatives. These molecules display good potency against a panel of multidrug-resistant Gram-positive and Gram-negative bacterial strains. Meanwhile, they also effectively inhibit the biofilm formation. Mechanistic studies suggest that these compounds kill bacteria by compromising bacterial membranes, a mechanism analogous to that of host-defense peptides (HDPs). Lastly, we also demonstrate that these molecules have excellent in vivo activity against MRSA in a rat model. This class of compounds could lead to an appealing class of antibiotic agents combating drug-resistant bacterial strains.
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Storms, William Kenneth. "Polymeric Amphiphilic Nanoparticles Via Intramolecular Chain Collapse Using 1-Functionalized Vinylbenzocyclobutenes." University of Akron / OhioLINK, 2015. http://rave.ohiolink.edu/etdc/view?acc_num=akron1436548338.
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Schulz, Sarah Gwendolyn. "The phase behavior of amphiphilic surfactants and polymers : a dissipative particles dynamics study." kostenfrei, 2004. http://deposit.ddb.de/cgi-bin/dokserv?idn=976770164.
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Kim, Cheol Joo. "Physical and Immunological Characterization of Molecular Assemblies Comprising Poly(sarcosine)-Based Amphiphilic Polymers." Kyoto University, 2017. http://hdl.handle.net/2433/225966.
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Cochin, D., P. Hendlinger, and André Laschewsky. "Polysoaps with fluorocarbon hydrophobic chains." Universität Potsdam, 1995. http://opus.kobv.de/ubp/volltexte/2008/1734/.
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A series of amphiphilic copolymers is prepared by copolymerization of choline methacrylate with 1,1,2,2-tetrahydroperfluorooctyl methacrylate in varying amounts. The copolymers bearing fluorocarbon chains are studied concerning their effects on viscosity, solubilization and surface activity in aqueous solution, exhibiting a general behavior characteristic for polysoaps. The results are compared with the ones obtained for an analogous series of amphiphilic copolymers bearing hydrocarbon chains.
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Guzman, Cardozo Gustavo A. Guzman. "Bimodal Amphiphilic Polymer Conetworks: Structure-Property Characterization, Processing and Applications." University of Akron / OhioLINK, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=akron1471428782.
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Herfurth, Christoph. "Einstufen-Synthese und Charakterisierung amphiphiler Sternpolymere als multifunktionale assoziative Verdicker." Phd thesis, Universität Potsdam, 2012. http://opus.kobv.de/ubp/volltexte/2012/6244/.
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Typische assoziative Verdicker für wässrige Systeme basieren auf linearen, doppelt hydrophob endmodifizierten Poly(ethylenglykolen) (PEGs). Diese Polymere aggregieren aufgrund ihrer Struktur in wässriger Lösung und bilden ein Netzwerk aus verbrückten Polymer-Mizellen. Dabei kann ein Polymer-Molekül maximal zwei Mizellen miteinander verbinden. Bisher ist unklar, wie die Anzahl der Endgruppen eines verzweigten, mehrfach hydrophob endmodifizierten hydrophilen Polymers die Struktur und Dynamik solcher Netzwerke beeinflusst. Die Synthese verzweigter Polymere auf PEG-Basis erfolgt mittels lebender ionischer Polymerisation und ist experimentell aufwändig. Das Einführen hydrophober Endgruppen erfordert zusätzliche Synthese-Schritte.
In dieser Arbeit wurden hydrophile Sternpolymere mit hydrophoben Endgruppen in einem Schritt hergestellt. Dazu wurde die Technik der radikalischen Polymerisation unter Kettenübertragung durch reversible Addition und anschließende Fragmentierung (reversible addition-fragmentation chain transfer, RAFT) genutzt. Die Synthese der Sternpolymere erfolgte von einem multifunktionalen Kern, der die R-Gruppe der RAFT-Kettenüberträger (chain transfer agents, CTAs) bildete. Die dazu benötigten CTAs wurden so konzipiert, dass mit ihrer Hilfe sowohl die Anzahl der Arme des Sternpolymers (von 2 bis 4), als auch die Länge der hydrophoben Endgruppe (C4, C12, C18) variiert werden konnte. Der große Vorteil der RAFT-Polymerisation ist, dass sie viele polare Monomere für die Synthese der hydrophilen Arme des Sternpolymers toleriert. In dieser Arbeit wurden als Modell-Monomere Oligo(ethylenglykol)methylether-acrylat (OEGA) und N,N-Dimethylacrylamid (DMA) eingesetzt. Beide Monomere bilden nicht-ionische hydrophile Polymere. Poly(OEGA) ist ein Kammpolymer, das auf PEG basiert. Poly(DMA) besitzt dagegen eine deutlich kompaktere Struktur.
Die erhaltenen amphiphilen Sternpolymere wurden umfassend molekular charakterisiert. Die Molmassen wurden mit verschiedenen GPC-Systemen bestimmt und der Grad der Endgruppenfunktionalisierung wurde mittels UV/Vis- und 1H-NMR-Spektroskopie überprüft. Die Polymerisation von OEGA zeigt mit den CTAs einige Charakteristika der Polymerisation mit reversibler Deaktivierung (RDRP, auch „kontrollierte radikalische Polymerisation“), wird aber durch Kettenübertragung zum Monomer bzw. Polymer gestört. Diese Nebenreaktion ist auf die Struktur des Monomers als Oligoether zurückzuführen.
Bei allen untersuchten Polymerisationen von DMA mit den multifunktionalen CTAs steigt die Molmasse linear mit dem Umsatz. Die erhaltenen Polymere zeigen durchweg monomodale und enge Molmassenverteilungen (PDI ≤ 1,2). Die Molmassen lassen sich in einem weiten Bereich von 25 kg/mol bis 150 kg/mol einstellen und die Endgruppen der Polymere bleiben zu 90 % erhalten. Während die Polymerisation von DMA sowohl mit den di- als auch den trifunktionalen CTAs innerhalb von 3 h zu quantitativen Umsätzen verläuft, wird der quantitative Umsatz des Monomers bei der Polymerisation mit tetrafunktionalen CTAs erst nach 4 h erreicht. Diese Verzögerung ist auf eine Retardierung in der Anfangsphase der Polymerisation zurückzuführen, die sich aus der besonderen Struktur der tetrafunktionalen CTAs erklärt.
Auf dem System zur Polymerisation von DMA aufbauend ließen sich Gradienten-Block-Copolymere in Eintopfreaktionen herstellen. Dazu wurde nach Erreichen des quantitativen Umsatzes von DMA ein zweites Monomer zur Reaktionsmischung gegeben. Mit Ethylacrylat (EtA) wurden so lineare amphiphile symmetrische Triblock-Copolymere erhalten. Dabei wurde die Länge des hydrophoben Blocks durch unterschiedliche Mengen an EtA variiert. Mit N,N-Diethylacrylamid (DEA) wurden lineare symmetrische Triblock-Copolymere sowie 3-Arm Stern-Diblock-Copolymere hergestellt, die über einen thermisch schaltbaren zweiten Block verfügen. Bei diesen Polymeren lässt sich die Länge des hydrophoben Teils in situ durch Veränderung der Temperatur variieren.
Das Verhalten der amphiphilen Sternpolymere in wässriger Lösung und in Mikroemulsion wurde im Rahmen einer Kooperation an der TU Berlin mit Hilfe von Kleinwinkel-Neutronenstreuung (SANS), dynamischer Lichtstreuung (DLS) und Rheologie untersucht. Die Polymere wirken durch Assoziation der hydrophoben Endgruppen als effektive Verdicker sowohl allein in wässriger Lösung als auch in Mikroemulsion. Die Struktur des gebildeten Netzwerks hängt dabei von der Konzentration des Polymers in der Lösung und der Länge der Endgruppe (Hydrophobie) ab. Die dynamischen Eigenschaften der Lösungen werden außerdem durch die Anzahl der Arme der Polymere bestimmt.Typically, associative thickeners for aqueous system consist of linear, hydrophobically α,ω-end-capped poly(ethylene glycols) (PEGs). Owing to their structure, these polymers aggregate in aqueous solution, forming a network of bridged micelles. Thus, one polymer molecule can link not more than two micelles. Until now it is unclear whether the structure and dynamics of such networks are influenced by the number of end groups of a branched multiply hydrophobically end-capped hydrophilic polymers. Branched PEG-based polymers are synthesized using the laborious and limited techniques of living ionic polymerization. Introducing hydrophobic end groups demands a multiple-step process. This work presents the one-step synthesis of hydrophilic star polymers with hydrophobic end groups, using reversible addition fragmentation chain transfer (RAFT) polymerization. This radical polymerization method is easy to use and tolerates a large number of polar monomers for the synthesis of the hydrophilic arms of the star polymers. The arms of the polymer were grown from a multifunctional core that formed the R-group of the chain transfer agents (CTAs). The CTAs where tailored to be able to vary the number of arms of the star polymers from 2 to 4 and to vary the length (and therefore the hydrophobicity) of the end groups (C4, C12, C18). Two different polar monomers where used as model monomers: Oligo(ethylene glycol)methyl ether acrylate (OEGA) and N,N-Dimethylacrylamide (DMA). Both monomers yield non-ionic hydrophilic polymers. While poly(OEGA) is a comb polymer based on PEG, poly(DMA) exhibits a more compact structure. The amphiphilic star polymers were characterized extensively. The molar masses were determined using GPC in various solvents and the degree of end functionalisation was monitored using 1H NMR and UV/Vis spectroscopy. The polymerization of OEGA shows some of the expected characteristics of reversible deactivation radical polymerization (RDRP). However, chain transfer to monomer and polymer is a prominent side reaction, limiting the use of this monomer for the fabrication of well-defined material. This reaction can be attributed to the structure of the monomer being an oligoether. For all examined polymerizations of DMA with the multifunctional CTAs the molar mass increased linearly with conversion. The molar mass distributions were monomodal and narrow (PDI ≤ 1.2). Expected values were reached for molar masses from 25 to 150 kg/mol and the end group functionality was about 90 % in all cases. While the polymerization of DMA using di- and trifunctional CTAs proceeded to quantitative conversion within 3 h, an initial retardation period of about 60 min was observed for the polymerization using tetrafunctional CTAs. This retardation was attributed to the peculiar molecular structure of these CTAs. Owing to the well-controlled features of the polymerization of DMA using the multifunctional CTAs, this system was used to obtain tapered block copolymers in a one-pot process. These structures were achieved by adding a second monomer to the reaction mixture after the quantitative conversion of DMA. Using ethyl acrylate (EtA), linear amphiphilic symmetrical triblock copolymers were synthesized. The length of the hydrophobic block was tailored by the addition of varying amounts of EtA. With N,N-Diethylacrylamide as a second monomer, linear symmetric triblock copolymers as well as 3-arm star diblock copolymers were obtained that contain a thermosensitve block. Altering the temperature of aqueous solutions of these polymers varies the length of the hydrophobic block in situ. At the TU Berlin, the behavior of the polymers was studied in aqueous solution as well as in microemulsion. The solutions were characterized by small angle neutron scattering (SANS), dynamic light scattering (DLS) and rheology. The end groups of the polymers aggregate, making the polymers efficient thickeners both in aqueous solution and in microemulsion. The structure of the formed network depends on the concentration of the polymer in solution and on the length of the end group. The dynamic properties of the solutions are governed additionally by the number of arms.
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Salunke, Namrata. "Self-Assembly of Functional Amphiphilic Triblock Copolymer Thin Films." University of Akron / OhioLINK, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=akron1533137379044442.
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Rahimi, Alireza. "Investigation of Novel Approaches for Improved Amphiphilic Fouling-Release Coatings." Diss., North Dakota State University, 2020. https://hdl.handle.net/10365/32075.
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Marine biofouling has troubled mankind, both environmentally and economically, since they set sail, resulting in many undesired consequences such as increased drag, reduced maneuverability, increased fuel consumption and greenhouse gas emissions, and heightened maintenance costs. This problem is highly complex as it involves more than 4000 marine organisms with varying modes of adhesion and surface preferences as well as many aquatic environments. The common state-of-the-art approaches to contend with marine biofouling on the submerged surfaces of ships in seawater has antifouling (AF) and fouling-release (FR) surfaces.
As AF coating systems utilize biocides which are often toxic to the environment to prevent settlement of biofoulants, the endeavors have been shifted towards non-toxic FR marine system. Many FR systems take advantage of low surface energy and modulus polydimethylsiloxane (PDMS) on their surface, while the recent attempts explored the simultaneous effect of PDMS and hydrophilic moieties (i.e. polyethylene glycol (PEG) or zwitterionic polymers) on an FR surface, known as amphiphilic surfaces. Thus, the work in this dissertation focused on attaining amphiphilic surfaces with desirable FR performance.
The studies in this dissertation were investigated to deliver two goals: 1) Enhancing the (FR) fouling-release performance of previously developed coating systems; 2) Introducing novel fouling-release marine coatings with set criteria. To address the former, a series of amphiphilic additives containing PDMS and hydrophilic polymers (zwitterionic-based or PEG) were prepared in chapters two-five. These additives were incorporated in several previously developed FR coating systems in order to modify their surfaces and enhance their FR performance. To address the latter, two amphiphilic marine coating systems were explored for accessing durable, non-toxic, and effective FR surfaces using epoxy-amine crosslinking chemistry. Overall, the studies in this dissertation not only demonstrated viable FR surfaces with desirable performance against several representative marine organisms such as N. incerta, U. linza, C. lytica, barnacles, and mussels but also contributed a deeper understanding about the effect of amphiphilicity concentration/balance on surface and FR properties.
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Hall, Peter John. "The synthesis and study of amphiphilic side-chain polymers capable of forming lyotropic mesophases." Thesis, Cardiff University, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.277491.
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Zawadka, Aleksandra. "Amphiphilic self-assembly polymers with improved environmental profile for home and personal care products." Doctoral thesis, Università di Siena, 2022. http://hdl.handle.net/11365/1204458.
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Graft copolymers constitute an important class of copolymers since it is possible to tune their characteristics opportunely designing their macromolecular structure. There is a growing interest for the design and synthesis of graft copolymers with desired composition and functionality to be used in a wide range of applications. Free radical polymerization techniques offer the straightforward synthesis of amphiphilic graft copolymers materials thanks also to the vast choice of available monomers with different functional groups. Amphiphilic graft copolymers, or polymer containing both hydrophilic and hydrophobic parts in their structure, possess unique properties due to the distinct chemical nature of building blocks and can self-assembly to various morphologies to render the favorable interactions. Characteristics of graft copolymers can be adjusted through the variations of composition (type of the grafted chains, grafting densities) and architecture (length of backbone and grafted chains etc.). Therefore, understanding the relation between the macromolecular architecture, composition and characteristics is crucial to tailor polymers for specific applications. This thesis covers the synthesis, characterization, and applications of amphiphilic graft copolymers, to reveal the effects of their chemical structure on capsules formation, encapsulation of fragrance molecules, and biodegradability rate. A wide range of applications can be defined for the use of amphiphilic copolymers. This work focuses on the self-assembly properties of amphiphilic copolymers, with improved environmental profile, for potential use in perfume sustainable encapsulation technology in liquid home- and personal-care products.
To achieve the synthesis of copolymers with self-assembled structures, hydrophilic poly (ethylene glycols) (PEGs) of different molecular weights, hydrophilic and hydrophobic monomers like thermo-responsive N-vinyl caprolactam (VCL) and/or vinyl acetate (VAc), have been used. Amphiphilic copolymers were obtained through a radical polymerization method using peroxide as an initiator. Different molecular weights (lengths of the chain), grafting densities as well as various chemical moieties have been investigated. Synthetized materials were characterized by FT-IR, 1D NMR, 2D NMR, DSC, TGA, GPC, ToF-Sims. Biodegradability of copolymers was measured by OECD 301b test and capsules formation properties were investigated using fluorescence microscopy. The studies reported in this work demonstrated that the capsules formation by synthetized copolymers in liquid detergent formulations strongly depend on the molecular weight of hydrophobic content and the degree of grafting of hydrophobic graft chains. Among all synthetized copolymers and commercial copolymer Soluplus only copolymer S2, which has the highest molecular weight of hydrophobic PVAc-co-PVCL part and higher grafting degree, showed capsules formation and encapsulation of perfume and PRMs in both SLFE liquid detergent formulations and water matrix. All synthesized copolymers are 4 -5 folds more biodegradable than commercial Soluplus.
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Sharma, Arjun. "Molecular Dynamics Simulations of Stimuli-Responsive Polymers." ScholarWorks@UNO, 2016. http://scholarworks.uno.edu/td/2275.
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Polymers that undergo dramatic changes in structural conformations in response to numerous stimuli such as temperature, pH, electric and magnetic fields, light inten- sity, biological molecules, and solvent polarity, are known as stimuli-responsive or ”smart” polymers. There is a broad range of very promising applications of these materials in catalysis, environmental remediation, sensors or actuator systems, and as delivery systems of therapeutic agents. Researchers have been trying to mimic smart polymers based on properties of polymers found in nature such as proteins, carbohydrates and nucleic acids. Novel bio-compatible polymers with a variety of chemical functional groups, diverse topologies, and cross-linking patterns with the ability to self-assemble in vivo are being engineered.
Experimental and theoretical studies indicate that the thermodynamic properties relating to the hydrophobic effects play a pivotal role in determining the self-assembly process in smart polymers. At the same time, computational approaches based on simulation and modeling provide an understanding of this phenomenon on the micro- scopic level. Building empirical models based on statistical mechanics methods and
simulation data helps to design polymeric materials with desirable traits.
My research is mainly focused on investigating physicochemical characteristics of stimuli-responsive polymers under different conditions. I used atomistic molecular dynamics simulations to investigate these effects on polymer conformation. Given the size and complexity of our polymeric systems, we employed Graphical Process- ing Units (GPU) and enhanced sampling techniques such as REDS2 to increase the sampling time. These methods allow for the study of polymeric structural dynamics in solvents of varying polarity and in human skin epidermis.
Our constant pH simulation of poly(methacrylic acid) revealed that the overall response is made up of local and global structural changes. The local structural re- sponse depends on the tacticity of the polymer, which leads to distinct cooperative effects for polymers with varying stereochemistry. Such simulations help to under- stand the principal driving forces behind the mechanism of self-assembly processes.
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Embs, Frank, Dirk Funhoff, André Laschewsky, Ulrike Licht, Holger Ohst, Werner Prass, Helmut Ringsdorf, Gerhard Wegner, and Rolf Wehrmann. "Preformed polymers for Langmuir-Blodgett films- molecular concepts." Universität Potsdam, 1991. http://opus.kobv.de/ubp/volltexte/2008/1719/.
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The use of preformed polymers for the preparation of Langmuir-Blodgett (LB) multilayers is reviewed. Principles for polymer self-organization are outlined and the appropriate molecular designs are discussed. Recent developments in the different classes of polymers for LB multilayers are presented, and their outstanding properties highlighted.
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Zhang, Baofang. "Examination Of The Solution Behaviors Of The Giant Inorganic-Organic Amphiphilic Hybrids." University of Akron / OhioLINK, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=akron1460369559.
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Navarro, Navarro Salvador [Verfasser], and Henning [Akademischer Betreuer] Menzel. "Synthesis and Characterization of Amphiphilic Polyamine-based Polymers for Silica Precipitation / Salvador Navarro Navarro ; Betreuer: Henning Menzel." Braunschweig : Technische Universität Braunschweig, 2010. http://d-nb.info/1175828599/34.
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Nakano, Minoru. "Synthesis of Novel Amphiphilic Polymers and Investigation of Their Aggregation Behavior in Solution by Small-Angle Scattering." Kyoto University, 1998. http://hdl.handle.net/2433/77940.
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Kristen, Juliane Ute. "Amphiphilic BAB-triblock copolymers bearing fluorocarbon groups : synthesis and self-organization in aqueous media." Phd thesis, Universität Potsdam, 2011. http://opus.kobv.de/ubp/volltexte/2012/6178/.
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In this work new fluorinated and non-fluorinated mono- and bifunctional trithiocarbonates of the structure Z-C(=S)-S-R and Z-C(=S)-S-R-S-C(=S)-Z were synthesized for the use as chain transfer agents (CTAs) in the RAFT-process. All newly synthesized CTAs were tested for their efficiency to moderate the free radical polymerization process by polymerizing styrene (M3). Besides characterization of the homopolymers by GPC measurements, end- group analysis of the synthesized block copolymers via 1H-, 19F-NMR, and in some cases also UV-vis spectroscopy, were performed attaching suitable fluorinated moieties to the Z- and/or R-groups of the CTAs.
Symmetric triblock copolymers of type BAB and non-symmetric fluorine end- capped polymers were accessible using the RAFT process in just two or one polymerization step. In particular, the RAFT-process enabled the controlled polymerization of hydrophilic monomers such as N-isopropylacrylamide (NIPAM) (M1) as well as N-acryloylpyrrolidine (NAP) (M2) for the A-blocks and of the hydrophobic monomers styrene (M3), 2-fluorostyrene (M4), 3-fluorostyrene (M5), 4-fluorostyrene (M6) and 2,3,4,5,6-pentafluorostyrene (M7) for the B-blocks.
The properties of the BAB-triblock copolymers were investigated in dilute, concentrated and highly concentrated aqueous solutions using DLS, turbidimetry, 1H- and 19F-NMR, rheology, determination of the CMC, foam height- and surface tension measurements and microscopy. Furthermore, their ability to stabilize emulsions and microemulsions and the wetting behaviour of their aqueous solutions on different substrates was investigated. The behaviour of the fluorine end-functionalized polymers to form micelles was studied applying DLS measurements in diluted organic solution.
All investigated BAB-triblock copolymers were able to form micelles and show surface activity at room temperature in dilute aqueous solution. The aqueous solutions displayed moderate foam formation. With different types and concentrations of oils, the formation of emulsions could be detected using a light microscope. A boosting effect in microemulsions could not be found adding BAB-triblock copolymers. At elevated polymer concentrations, the formation of hydrogels was proved applying rheology measurements.Im Rahmen dieser Arbeit wurden neue fluorierte und unfluorierte mono- und bifunktionelle Trithiocarbonate der Typen Z-C(=S)-S-R und Z-C(=S)-S-R-S-C(=S)-Z zur Anwendung als CTAs (chain- transfer agents) im RAFT-Polymerisationsverfahren hergestellt. Alle CTAs wurden erfolgreich auf ihre Effizienz zur Steuerung des radikalischen Polymerisationsverfahrens hin durch Polymerisation von Styrol (M3) getestet. Neben GPC-Messungen wurden Endgruppenanalysen der synthetisierten Blockcopolymere mittels 1H-, 19F-NMR und in manchen Fällen auch UV-Vis Spektroskopie durchgeführt. Dazu wurden die Z- und/oder R-Gruppen der CTAs mit geeigneten fluorierten Gruppen versehen. Durch Anwendung des RAFT Verfahrens konnten symmetrische Triblockcopolymere vom Typ BAB bzw. mit einer Fluoralkylgruppe endgecappte unsymmetrische Polymere in nur zwei bzw. einem Polymerisationsschritt hergestellt werden. Das RAFT- Polymerisationsverfahren ermöglicht sowohl die Polymerisation hydrophiler Monomere wie N-Isopropylacrylamid (NIPAM) (M1) oder N-Acryloylpyrrolidin (NAP) (M2) für die A-Blöcke als auch der hydropoben Monomere Styrol (M3), 2-Fluorostyrol (M4), 3-Fluorostyrol (M5), 4- Fluorostyrol (M6) und 2,3,4,5,6- Pentafluorostyrol (M7) für die B-Blöcke. Die Eigenschaften der Blockcopolymere in verdünnten, konzentrierten und hochkonzentrierten wässrigen Lösungen wurden mittels DLS, Trübungsphotometrie, 1H- und 19F-NMR, Rheologie, CMC- sowie Schaumhöhen- und Oberflächenspannungsmessungen und Lichtmikroskopie untersucht. Weiterhin wurden ihre Eigenschaften als Emulgatoren und in Mikroemulsion untersucht. Das Micellbildungsverhalten der hydrophob endfunktionalisierten Polymere wurde mittels DLS Messungen in verdünnter organischer Lösung untersucht. Alle untersuchten BAB-Triblöcke bildeten Micellen und zeigten Oberflächenaktivität bei Raumtemperatur in verdünnter, wässriger Lösung. Weiterhin zeigen die wässrigen Lösungen der Polymere mäßige Schaumbildung. Mit verschiedenen Öltypen und Ölkonzentrationen wurden Emulsionen bzw. Mikroemulsionen gebildet. In Mikroemulsion wurde durch Zugabe von BAB-Triblockopolymeren kein Boosting-Effekt erzielt werden. Bei Untersuchung höherer Polymerkonzentrationen wurde die Bildung von Hydrogelen mittels rheologischer Messungen nachgewiesen. Verschiedene Substrate konnten benetzt werden. Die hydrophob endgecappten Polymere bilden in verdünnter organischer Lösung Micellen, die mittels DLS untersucht wurden, und zeigen somit Tensidverhalten in nichtwässriger Lösung.
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Kutikov, Artem B. "Amphiphilic Degradable Polymer/Hydroxyapatite Composites as Smart Bone Tissue Engineering Scaffolds: A Dissertation." eScholarship@UMMS, 2014. https://escholarship.umassmed.edu/gsbs_diss/755.
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Over 600,000 bone-grafting operations are performed each year in the United States. The majority of the bone used for these surgeries comes from autografts that are limited in quantity or allografts with high failure rates. Current synthetic bone grafting materials have poor mechanical properties, handling characteristics, and bioactivity. The goal of this dissertation was to develop a clinically translatable bone tissue engineering scaffold with improved handling characteristics, bioactivity, and smart delivery modalities. We hypothesized that this could be achieved through the rational selection of Food and Drug Administration (FDA) approved materials that blend favorably with hydroxyapatite (HA), the principle mineral component in bone. This dissertation describes the development of smart bone tissue engineering scaffolds composed of the biodegradable amphiphilic polymer poly(D,L-lactic acid-co-ethylene glycol-co- D,L-lactic acid) (PELA) and HA. Electrospun nanofibrous HA-PELA scaffolds exhibited improved handling characteristics and bioactivity over conventional HApoly( D,L-lactic acid) composites. Electrospun HA-PELA was hydrophilic, elastic, stiffened upon hydration, and supported the attachment and osteogenic differentiation of rat bone marrow stromal cells (MSCs). These in vitro properties translated into robust bone formation in vivo using a critical-size femoral defect model in rats. Spiral-wrapped HA-PELA scaffolds, loaded with MSCs or a lowdose of recombinant human bone morphogenetic protein-2, templated bone formation along the defect. As an alternate approach, PELA and HA-PELA were viii rapid prototyped into three-dimensional (3-D) macroporous scaffolds using a consumer-grade 3-D printer. These 3-D scaffolds have differential cell adhesion characteristics, swell and stiffen upon hydration, and exhibit hydration-induced self-fixation in a simulated confined defect. HA-PELA also exhibits thermal shape memory behavior, enabling the minimally invasive delivery and rapid (>3 sec) shape recovery of 3-D scaffolds at physiologically safe temperatures (~ 50ºC). Overall, this dissertation demonstrates how the rational selection of FDA approved materials with synergistic interactions results in smart biomaterials with high potential for clinical translation.
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Kutikov, Artem B. "Amphiphilic Degradable Polymer/Hydroxyapatite Composites as Smart Bone Tissue Engineering Scaffolds: A Dissertation." eScholarship@UMMS, 2011. http://escholarship.umassmed.edu/gsbs_diss/755.
Full textAbstract:
Over 600,000 bone-grafting operations are performed each year in the United States. The majority of the bone used for these surgeries comes from autografts that are limited in quantity or allografts with high failure rates. Current synthetic bone grafting materials have poor mechanical properties, handling characteristics, and bioactivity. The goal of this dissertation was to develop a clinically translatable bone tissue engineering scaffold with improved handling characteristics, bioactivity, and smart delivery modalities. We hypothesized that this could be achieved through the rational selection of Food and Drug Administration (FDA) approved materials that blend favorably with hydroxyapatite (HA), the principle mineral component in bone. This dissertation describes the development of smart bone tissue engineering scaffolds composed of the biodegradable amphiphilic polymer poly(D,L-lactic acid-co-ethylene glycol-co- D,L-lactic acid) (PELA) and HA. Electrospun nanofibrous HA-PELA scaffolds exhibited improved handling characteristics and bioactivity over conventional HApoly( D,L-lactic acid) composites. Electrospun HA-PELA was hydrophilic, elastic, stiffened upon hydration, and supported the attachment and osteogenic differentiation of rat bone marrow stromal cells (MSCs). These in vitro properties translated into robust bone formation in vivo using a critical-size femoral defect model in rats. Spiral-wrapped HA-PELA scaffolds, loaded with MSCs or a lowdose of recombinant human bone morphogenetic protein-2, templated bone formation along the defect. As an alternate approach, PELA and HA-PELA were viii rapid prototyped into three-dimensional (3-D) macroporous scaffolds using a consumer-grade 3-D printer. These 3-D scaffolds have differential cell adhesion characteristics, swell and stiffen upon hydration, and exhibit hydration-induced self-fixation in a simulated confined defect. HA-PELA also exhibits thermal shape memory behavior, enabling the minimally invasive delivery and rapid (>3 sec) shape recovery of 3-D scaffolds at physiologically safe temperatures (~ 50ºC). Overall, this dissertation demonstrates how the rational selection of FDA approved materials with synergistic interactions results in smart biomaterials with high potential for clinical translation.
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Zaki, Afroditi Maria. "Molecular dynamics study of biomembrane interactions with biologically active polymers." Thesis, University of Manchester, 2018. https://www.research.manchester.ac.uk/portal/en/theses/molecular-dynamics-study-of-biomembrane-interactions-with-biologically-active-polymers(0e61623d-d73c-4f84-a1ef-6698026c4aa2).html.
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Among the great breakthroughs in nanoscience and nanotechnology is the emergence of synthetic polymers that demonstrate biological activity and thus can be exploited for biomedical applications, extending from agents in therapeutics to drug delivery and tissue engineering. A key factor in the fabrication of such polymeric materials is the ability to tune and control their properties. To this end, an insight into the mode of interactions with biological systems is imperative. Computer simulations have proved to be a valuable tool that can compliment experiments and provide -otherwise inaccessible- information. In the context of this thesis, different aspects of the polymeric biological activity were investigated by studying two polymeric materials suitable for different types of applications, aiming to clarify yet undisclosed mechanisms that govern the polymers' behaviour either in solution or in conjunction with model lipid membranes. The first part of the thesis is dedicated to a nonionic amphiphilic copolymer known as Pluronic L64 that is considered as a candidate for the design of novel hybrid polymer-lipid vesicles that will act as carriers for drugs or genes. The hybrid bilayers are subjected to mechanical stress and their properties are compared to those of pure lipid bilayers. The simulations showed that the hybrid membranes can sustain increased surface tension prior to rupture, are stiffer, thicker and the polymers can induce higher lipid tail packing and also reduce the lipid mobility, rendering the membranes more ordered and less fluid. At high values of lateral pressure, which leads to pore formation, the copolymer chains decelerate the pore growth. The examination of the defect formation mechanism reveals that the hydrophilic PEO segment plays the most vital role. The same systems were also observed in varying temperatures and the impact of the inserted polymers on the phase behaviour was investigated. The data suggested that the polymers change the nature of the phase transition from a discontinuous to a continuous one. The hybrid membranes transform between the ordered and the disordered phase in a continuous manner and not at a critical melting temperature. Interestingly, the effect of polymers is different at the low and high temperature regions, as proved by the analysis of the mechanical, structural and dynamic membrane properties. The second part is focused on the study of polyhexamethylene biguanide (PHMB), a biguanide-based polyelectrolyte, that possesses remarkable biocidal properties. Even though PHMB's activity is known, the specific mode of action against bacterial membranes is still puzzling. Our work revealed that the polyelectrolyte assumes a counterintuitive behaviour in aqueous solution tending to self-organise into ordered compact structures, despite the repulsive electrostatic interactions of its positively charged segments. The formed nano-objects are thermodynamically stable, as was confirmed by free energy calculations and could be linked to PHMB's antibacterial mechanism. These findings pave the way for further computational and experimental exploration of these fascinating and promising materials that could lead to the design of novel smart biologically active nanoparticles.
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Díaz, Sebastián Andrés. "Water Soluble Photochromic Fluorescent Nanoprobes based on Diheteroarylethenes and Polymer Coated Quantum Dots." Doctoral thesis, Niedersächsische Staats- und Universitätsbibliothek Göttingen, 2013. http://hdl.handle.net/11858/00-1735-0000-0022-60A5-2.
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Samanta, Susruta [Verfasser]. "Theoretical Study of the Interaction of Amphiphilic Block Co-Polymers with Biological Interfaces and Small Molecules / Susruta Samanta." Bremen : IRC-Library, Information Resource Center der Jacobs University Bremen, 2013. http://d-nb.info/1037011961/34.
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Viswanathan, Kalpana. "Synthesis and Characterization of Novel Polymers for Functional and Stimuli Responsive Silicon Surfaces." Diss., Virginia Tech, 2006. http://hdl.handle.net/10919/27052.
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The synthesis of a variety of novel functionalized polymers using living polymerization techniques to achieve functional and stimuli responsive coatings on silica surfaces are described. Since microscopic features on a surface influence the overall wetting properties of the surface, a systematic investigation of the influence of polymer architecture on the microscopic characteristics of the modified surfaces was studied using silane-functionalized linear and novel star-branched polystyrene (PS). Star-branched modifiers provide functional and relatively well-defined model systems for probing surface properties compared to ill-defined highly branched systems and synthetically challenging dendrimers. Using these simple star-shaped macromolecules it was shown that the topographies of the polymer-modified surfaces were indeed influenced by the polymer architecture. A model explaining the observed surface features was proposed.
A living polymerization strategy was also used to synthesize centrally functionalized amphiphilic triblock copolymers. The amphiphilic copolymers exhibited stimuli responsive changes in surface hydrophobicity. In spite of multiple solvent exposures, the copolymer films remained stable on the surface indicating that the observed changes in surface properties were due to selective solvent induced reversible rearrangement of the copolymer blocks. The chemical composition of the copolymers was tailored in order to tune the response time of the surface anchored polymer chains. Thus, the polymer coatings were used to reversibly change the surface polarities in an on-demand fashion and could find possible applications as smart adhesives, sensors and reusable membrane devices.
In contrast to the afore-mentioned covalent modification approach, which often leads to permanent modification of surfaces, renewable surfaces exhibiting â universalâ adhesion properties were also obtained through non-covalent modification. By employing hydrogen bonding interactions between DNA bases, surfaces functionalized with adenine groups were found to reversibly associate with thymine-functionalized polymers. This study describing the solvato-reversible polymer coating was the first demonstration on silica surfaces. A systematic investigation of the influence of surface concentration of the multiple hydrogen bonding groups and their structure on the extent of polymer recognition by the modified surfaces is also discussed.Ph. D.
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Bolley, Anaëlle. "Catalyse de la polymérisation pour l'obtention de polyesters à caractères hydrophile biodégradable." Thesis, Strasbourg, 2019. http://www.theses.fr/2019STRAF015.
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Des adduits carbéniques à base de métaux du groupe 13 (aluminium, gallium et indium) ainsi qu’un nouveau cation d’aluminium stabilisé par des groupements alkyles, ont permis la ROP du lactide dans des conditions réactionnelles douces et simples. Dans un second temps, des copolymères amphiphiles ont été synthétisés par la ROP du lactide en présence de poly(éthylène glycol) menant aux PEG-co-PLLA désirés. Les complexes organométalliques ont encore mis en avant leurs avantages grâce à l’utilisation de salen d’aluminium qui permet d’ouvrir la voie sur la ROP de l’α-chloro-ε-caprolactone menant à la poly(α-chloro-ε-caprolactone). La synthèse de nouveaux copolymères, diblocs et stéréocomplexe a permis de moduler les propriétés de l’homopolymère obtenu, telles qu’ont pu le confirmer les diverses mesures physico-chimiques effectuées sur ces derniers. Enfin, la post-fonctionnalisation partielle, grâce à la réaction de Williamson, suivie par la réaction d’hydrogénation a permis l’obtention de polymères hydrophilesCarbene adducts with Group 13 metal (aluminium, gallium and indium) and a new aluminium cation stabilized by alkyl groups, have allowed the ROP of lactide under mild and simple conditions. In a second step, amphiphilic copolymers were synthesized with poly(ethylene glycol) leading to the desired PEG-co-PLLA. Organometallic complexes have still put forward their advantages by the use of aluminium’s salen allowing to open the way on the ROP of the α-chloro-ε-caprolactone leading to the poly(α-chloro-ε-caprolactone). The formation of new copolymers, diblocks and stereocomplex has afforded to modulate the obtained homopolymer’s properties, confirmed by the use of the various physicochemical measurements effected on the latter. Finally, the partial post-functionalization according to the Williamson reaction followed by the hydrogenation reaction has led to the obtaining of hydrophilic polymers