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Erel-Göktepe, İrem

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İrem

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Erel-Göktepe

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Erel-Göktepe, İrem

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2011 - 20123

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    Effect of structural isomerism and polymer end group on the pH-stability of hydrogen-bonded multilayers
    (Elsevier, 2011) Schlaad, Helmut; Department of Chemistry; Department of Chemistry; Erel-Göktepe, İrem; Demirel, Adem Levent; Researcher; Faculty Member; Department of Chemistry; College of Sciences; College of Sciences; 109862; 6568
    Association of tannic acid (TA) with structurally isomeric poly(N-isopropylacrylamide) (PNIPAM) and poly(2-isopropyl-2-oxazoline) (PIPOX) has been examined at surfaces to understand the effect of different molecular arrangements in a polymer repeating unit of structural isomers on the construction and pH-stability of hydrogen-bonded multilayers. Films were fabricated using layer-by-layer (LbL) technique through hydrogen-bonding interactions primarily between carbonyl groups of neutral polymers and hydroxyl groups of TA molecules at pH 2. PIPOX and TA formed thinner and more stable films in the pH scale with a critical dissolution pH of 9 when compared to films of PNIPAM and TA with a critical pH of 8. The differences in the thickness and pH-stability were due to different conformational behavior of PNIPAM and PIPOX in water which affects the accessibility of carbonyl groups for participation in the hydrogen bonding and the number of binding sites between the polymer pairs. Addition of electrostatic interactions by introducing amino groups only at the PIPOX chain end shifted the critical dissolution pH to higher values and resulted in gradual dissolution of the films in a wide pH range of 9-12. Such films hold promise for use in biomedical field due to biocompatibility and lower critical solution temperature (LCST) behavior at near physiological temperature of PNIPAM and PIPOX together with the pH-response of the hydrogen-bonded films. (C) 2011 Elsevier Inc. All rights reserved.
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    Hydrogen-bonded layer-by-layer films of block copolymer micelles with pH-responsive cores
    (Elsevier, 2011) Zhu,Zhichen; Zhuk, Aliaksandr; Sukhishvili, Svetlana A.; Department of Chemistry; Erel-Göktepe, İrem; Researcher; Department of Chemistry; College of Sciences; 109862
    We report on construction of hydrogen-bonded monolayers and multilayers of micelles of the poly(2-(diethylamino)ethyl methacrylate)-block-poly(N-isopropyl acrylamide) (PDEA-b-PNIPAM) with PNIPAM-corona and polybasic PDEA cores. Films were constructed at pH 7.5 and 25 degrees C to assure the deposition of PDEA-b-PNIPAM in the micellar form. When monolayers of block copolymer micelles (BCMs) were exposed to moderately acidic pH values, micellar cores dissolved, while PDEA-b-PNIPAM remained adsorbed at the surface as unimers. In contrast to reversible micellization of PDEA-b-PNIPAM in solution, micelle-to-unimer transition was irreversible at the surface. Adsorption of a layer of tannic acid (TA) or polyethacrylic acid (PEAA) on top of BCM monolayers inhibited pH-triggered morphological changes within adsorbed BCMs. By taking advantage of the high pK(a) values of TA and PEAA, we were also able to construct multilayers of PDEA-b-PNIPAM micelles through hydrogen bonding interactions between micellar PNIPAM coronas and TA or PEAA. Similar to BCM monolayers coated with TA or PEAA, dissolution of BCMs was also inhibited when incorporated within hydrogen-bonded multilayers. Such inhibition of dissolution is due to enhanced hydrogen bonding interactions between coronal PNIPAM chains and protonated TA molecules or PEAA chains at decreasing pH values restricting the pH-induced conformational changes of the micellar core chains within the adsorbed layer. Films of responsive BCMs are attractive coatings for controlled delivery of functional molecules from surfaces due to a combination of stimuli-response properties with the relatively high loading capacity for functional molecules. (C) 2010 Elsevier Inc. All rights reserved.
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    Hydrogen-bonded multilayers of micelles of a dually responsive dicationic block copolymer
    (Royal Society of Chemistry (RSC), 2012) Tuncer, Cansel; Bütün, Vural; Department of Chemistry; Erel-Göktepe, İrem; Karahan, Hüseyin Enis; Demirel, Adem Levent; PhD Student; Faculty Member; Department of Chemistry; College of Sciences; N/A; N/A; 6568
    We report the fabrication of hydrogen-bonded multilayers of micelles of a dually responsive, dicationic block copolymer, poly[2-(N-morpholino)ethyl methacrylate-block-2-(diisopropylamino)ethyl methacrylate] (PMEMA-b-PDPA). By taking advantage of the difference in the hydrophilicity of PMEMA and PDPA blocks, micelles with a PMEMA-corona and a PDPA-core were obtained above pH 6.5 and were assembled layer-by-layer at the surface with tannic acid (TA) at pH 7.4 through hydrogen bonding interactions between morpholino units of PMEMA and hydroxyl groups of TA. Destruction of PMEMA-b-PDPA micelles/TA films could be controlled at both acidic and basic conditions. At basic pH (pH = 8.75), multilayers disintegrated due to ionization of TA and disruption of hydrogen bonding interactions between layers of micelles and TA. At moderately acidic pH values, partially dissolved PMEMA-b-PDPA micelles and monomers underwent a restructuring with TA molecules and remained adsorbed at the surface. Complete dissolution of the multilayers occurred at around pH 3.6 due to further protonation of the tertiary amino groups on both blocks of PMEMA-b-PDPA, resulting in a charge imbalance between PMEMA-b-PDPA and TA layers followed by disintegration of the films. We have also encapsulated pyrene in the micellar cores and found that pyrene released from PMEMA-b-PDPA micelles/TA films increased 1.5- and 2.5-fold when the pH was decreased from 7.5 to 6 and 5, respectively. Such an increase in the amount of pyrene released was due to pH-controlled dissolution of the micellar cores. We have also found that at pH 7.5, increasing the temperature to 40 degrees C enhanced the release of pyrene by approximately 2-fold. Such an increase is due to lower critical solution temperature (LCST) behaviour of coronal PMEMA chains leading to temperature-induced conformational changes on the coronal chains, facilitating the release of pyrene through the coronal chains into the solution. Hydrogen bonded multilayers of micelles of a dicationic block copolymer are interesting due to the response of both multilayers and micellar cores at different pH paving the way for multiple pH-controlled delivery of functional molecules from surfaces.