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search.filters.applied.f.access: openAccess × End date: 2023 × Start date: 2023 × DDC: 540 × Has files: Yes × Type: Text × WGL Institute: IFWD × WGL Institute: IPF ×

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    Systematic evaluation of oligodeoxynucleotide binding and hybridization to modified multi-walled carbon nanotubes
    (London : Biomed Central, 2017) Kaufmann, Anika; Hampel, Silke; Rieger, Christiane; Kunhardt, David; Schendel, Darja; Füssel, Susanne; Schwenzer, Bernd; Erdmann, Kati
    Background: In addition to conventional chemotherapeutics, nucleic acid-based therapeutics like antisense oligodeoxynucleotides (AS-ODN) represent a novel approach for the treatment of bladder cancer (BCa). An efficient delivery of AS-ODN to the urothelium and then into cancer cells might be achieved by the local application of multi-walled carbon nanotubes (MWCNT). In the present study, pristine MWCNT and MWCNT functionalized with hydrophilic moieties were synthesized and then investigated regarding their physicochemical characteristics, dispersibility, biocompatibility, cellular uptake and mucoadhesive properties. Finally, their binding capacity for AS-ODN via hybridization to carrier strand oligodeoxynucleotides (CS-ODN), which were either non-covalently adsorbed or covalently bound to the different MWCNT types, was evaluated. Results: Pristine MWCNT were successfully functionalized with hydrophilic moieties (MWCNT-OH, -COOH, -NH2, -SH), which led to an improved dispersibility and an enhanced dispersion stability. A viability assay revealed that MWCNT-OH, MWCNT-NH2 and MWCNT-SH were most biocompatible. All MWCNT were internalized by BCa cells, whereupon the highest uptake was observed for MWCNT-OH with 40% of the cells showing an engulfment. Furthermore, all types of MWCNT could adhere to the urothelium of explanted mouse bladders, but the amount of the covered urothelial area was with 2-7% rather low. As indicated by fluorescence measurements, it was possible to attach CS-ODN by adsorption and covalent binding to functionalized MWCNT. Adsorption of CS-ODN to pristine MWCNT, MWCNT-COOH and MWCNT-NH2 as well as covalent coupling to MWCNT-NH2 and MWCNT-SH resulted in the best binding capacity and stability. Subsequently, therapeutic AS-ODN could be hybridized to and reversibly released from the CS-ODN coupled via both strategies to the functionalized MWCNT. The release of AS-ODN at experimental conditions (80 °C, buffer) was most effective from CS-ODN adsorbed to MWCNT-OH and MWCNT-NH2 as well as from CS-ODN covalently attached to MWCNT-COOH, MWCNT-NH2 and MWCNT-SH. Furthermore, we could exemplarily demonstrate that AS-ODN could be released following hybridization to CS-ODN adsorbed to MWCNT-OH at physiological settings (37 °C, urine). Conclusions: In conclusion, functionalized MWCNT might be used as nanotransporters in antisense therapy for the local treatment of BCa.
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    Polyethenetetrathiolate or polytetrathiooxalate? Improved synthesis, a comparative analysis of a prominent thermoelectric polymer and implications to the charge transport mechanism
    (Cambridge : RSC Publ., 2018) Tkachov, Roman; Stepien, Lukas; Grafe, Robert; Guskova, Olga; Kiriy, Anton; Simon, Frank; Reith, Heiko; Nielsch, Kornelius; Schierning, Gabi; Kasinathan, Deepa; Leyens, Christoph
    1,1,2,2-Ethenetetrathiolate (ett4-) coordination polymers, such as poly[Kx(Ni-ett)], have been known for decades for their excellent thermoelectric properties. However in reality, ett4- is neither a "true" comonomer which participates in the polymerization, nor represents a "true" repeat unit of the target polymer. Indeed, poly[K2(Ni-ett)], which is formally the product of Ni-induced polymerization of ett4-, has a poor conductivity and needs to be oxidized to show attractive thermoelectric characteristics. The polymerization and oxidation processes are poorly controllable which causes irreproducibility of the polymer properties. To improve the synthesis reproducibility, we studied polymerization of potassium tetrathiooxalate (K2tto), the convenient synthesis of which was developed in our recent work. Because K2tto is the "true monomer", and not its precursor, a high quality product is reproducibly formed simply by mixing K2tto with NiCl2 at room temperature. The procedure does not require additional components (bases), or special conditions (prolonged heating), which are usually needed for the preparation of this polymer from the monomer precursor 1,3,4,6-tetrathiapentalene-2,5-dione (TPD). Furthermore, as tto2- is formally the product of two-electron oxidation of ett4-, the poorly controllable oxidation process is avoided and poly[Ni-tto] almost free from K is directly formed upon the complexation of Ni2+ and tto2-. Thus-obtained poly[Ni-tto] possesses conductivity in the range of 27-47 S cm-1 and a Seebeck coefficient in the range of -38 to -55 μV K-1, which are superior thermoelectric properties compared to poly[Kx(Ni-ett)] samples obtained by the previously reported methods. Redox and structural properties of poly[Ni-tto] were compared with those of poly[Kx(Ni-ett)] obtained by the reported methods. Furthermore, DFT calculations were performed to shed more light on generally promising properties of this class of materials. Particularly, possible packing models have been predicted for polymers, and the molecular dynamics simulations have been used to simulate the molecular arrangements under ambient conditions.