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Lokalisierung von Adsorptionsplätzen im Wirt-Gast-System Thionin in Zeolith NaYMüller, Marco. Unknown Date (has links)
Techn. Universiẗat, Diss., 2000--Darmstadt.
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Cytotoxic Compounds of Plant Origin – Biological and Chemical Diversity / Cytotoxiska föreningar från växter – biologisk och kemisk diversitetLindholm, Petra January 2005 (has links)
<p>The development of resistance by tumour cells to chemotherapeutic agents is a major problem in cancer treatments. One way to counter this is to find compounds with cytotoxic mechanisms other than those of drugs in clinical use today. The biological and chemical diversity encountered in Nature provide opportunities to discover completely new chemical classes of compounds. Some of these may represent previously unknown anticancer agents, and in some cases, novel, potentially relevant cytotoxic mechanisms. </p><p>The selection of plants for the cytotoxic investigation in this project was designed to cover large parts of the angiosperm system, providing a broad representation of species. Extracts of the plants were subjected to a polypeptide fractionation protocol, followed by bioassay-guided isolation, yielding series of fractions with increasing purity and cytotoxicity. The cytotoxicity assay included tumour cells from patients and a cell-line panel including ten different cell lines representing several types of resistant and non-resistant tumours. This screening strategy allowed fractions and compounds acting with novel mechanisms to be detected at an early stage. </p><p>The compounds isolated represent substantial chemical diversity and originate from diverse parts of the phylogenetic spectrum examined. They include the highly potent cytotoxic alkaloid, thiobinupharidine, the structure of which was determined by NMR techniques. Furthermore, two types of compound were shown to have previously unreported cytoxic activity: cyclotides (small macrocyclic polypeptides, in this case from violets) and polypeptides, possibly of thionine type, of loranthaceaeous mistletoes (collected in Panama). The well known cardiac glycosides from the foxglove, Digitalis, were identified as being responsible for the anti-tumour activity of this species.</p><p>In conclusion, the results obtained in this project show that selection based on phylogenetic information, together with a robust and reliable method to detect cytotoxicity, can be a useful approach for exploring the plant kingdom for cytotoxic substances.</p>
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Cytotoxic Compounds of Plant Origin – Biological and Chemical Diversity / Cytotoxiska föreningar från växter – biologisk och kemisk diversitetLindholm, Petra January 2005 (has links)
The development of resistance by tumour cells to chemotherapeutic agents is a major problem in cancer treatments. One way to counter this is to find compounds with cytotoxic mechanisms other than those of drugs in clinical use today. The biological and chemical diversity encountered in Nature provide opportunities to discover completely new chemical classes of compounds. Some of these may represent previously unknown anticancer agents, and in some cases, novel, potentially relevant cytotoxic mechanisms. The selection of plants for the cytotoxic investigation in this project was designed to cover large parts of the angiosperm system, providing a broad representation of species. Extracts of the plants were subjected to a polypeptide fractionation protocol, followed by bioassay-guided isolation, yielding series of fractions with increasing purity and cytotoxicity. The cytotoxicity assay included tumour cells from patients and a cell-line panel including ten different cell lines representing several types of resistant and non-resistant tumours. This screening strategy allowed fractions and compounds acting with novel mechanisms to be detected at an early stage. The compounds isolated represent substantial chemical diversity and originate from diverse parts of the phylogenetic spectrum examined. They include the highly potent cytotoxic alkaloid, thiobinupharidine, the structure of which was determined by NMR techniques. Furthermore, two types of compound were shown to have previously unreported cytoxic activity: cyclotides (small macrocyclic polypeptides, in this case from violets) and polypeptides, possibly of thionine type, of loranthaceaeous mistletoes (collected in Panama). The well known cardiac glycosides from the foxglove, Digitalis, were identified as being responsible for the anti-tumour activity of this species. In conclusion, the results obtained in this project show that selection based on phylogenetic information, together with a robust and reliable method to detect cytotoxicity, can be a useful approach for exploring the plant kingdom for cytotoxic substances.
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Desenvolvimento de nanopartículas fotossensibilizadoras / Development of photosensitizing nanoparticlesTada, Dayane Batista 14 December 2007 (has links)
No presente trabalho são apresentadas a síntese e a caracterização estrutural, fotofísica, fotoquímica e fotobiológica de nanopartículas contendo os fotossensibilizadores (FS) Azul de Metileno (AM) e Tionina. AM e Tionina foram incorporados nas nanopartículas sil-AM e sil-Tio pelo processo sol-gel. Nas nanopartículas Cab-Tio, Tionina foi ligada à superfície de sílica CabOsil® através de ligação covalente com reagentes bifuncionais. Todas as nanopartículas mostraram-se esféricas e com de diâmetro médio na faixa de 30 a 60nm. A imobilização dos FS induziu a agregação destes em extensões diferentes para cada tipo de nanopartícula. Foi observado que a maior presença de dímeros de FS leva à menor eficiência de geração de 1O2. Constatou-se que as nanopartículas sofrem pouca influência do meio, uma vez que os FS a elas ligadas não sofreram redução química por NADPH, nem supressão do estado tripleto por íons ascorbato e a supressão de fluorescência por íon brometo foi diminuída. Foi testado também o efeito do recobrimento destas nanopartículas com lipídios dioleilfosfatidil colina (DOPC) e fosfatidilglicerol (PG) e com Polietileno glicol (PEG). A adsorção das nanopartículas sobre membranas miméticas foi reduzida após os recobrimentos, resultado que foi explicado pelas interações de carga superficial (potencial zeta) e pela força de hidratação. As nanopartículas sil-AM e Cab-Tio apresentaram fototoxicidades in vitro, 38% e 20% maiores que os respectivos FS livres. A modificação das nanopartículas de sil-AM com lipídios e com PEG diminuiu a fototoxicidade das mesmas e no caso do recobrimento com lipídios levou ao aumento da toxicidade no escuro. Imagens de microscopia confocal mostraram que as nanopartículas com e sem recobrimento de lipídios entram em células B16. No caso das nanopartículas recobertas, observou-se um perfil de distribuição difuso por todo o citoplasma e no caso de nanopartículas sem recobrimento, estas encontraram-se em poucas regiões vacuolares do citoplasma. O perfil de distribuição homogênea por todo o citoplasma no caso de nanopartículas recobertas com lipídios pode ser o responsável pelo aumento de toxicidade no escuro. Concluiu-se que a ligação dos FS em nanopartículas com diferentes graus de agregação pode ser uma estratégia para obtenção de sistemas com capacidade modulada de geração de 1O2 e com reduzida susceptibilidade às composições do meio. As atividades fototóxicas das nanopartículas contra células B16 mostraram que estas podem ser úteis em Terapia Fotodinâmica de Câncer / In this work we present the synthesis and the characterization (structural, photophysical, photochemical and photobiological) of nanoparticles with incorporated photosensitizers (PS) Methylene Blue (MB) and Thionin. MB and Thionin were incorporated in sil-MB and sil-Th nanoparticles through sol-gel process. In the case of Cab-Th nanoparticles Thionin was linked to the surface of CabOsil® nanoparticles through cross-linking reactions. All nanoparticles were spherical and presented average diameter in the range of 30 to 60nm. Different extension of PS aggregation was observed in each nanoparticle. It was characterized that the higher the proportion of dimers to monomers the smaller the efficiency of singlet oxygen (1O2) generation. It was shown that nanoparticles can protect PS from external interferences, since NADPH did not reduce them, neither were their triplet state quenched by ascorbate ions. Besides, fluorescence quenching by bromide ions was reduced compared to free PS. The effect of covering the nanoparticles with lipids, i.e., di-oleil phosphatidylcholine (DOPC) and phosphatidylglycerol (PG), and with Polyethylene glycol was also tested. The nanoparticle adsorption over membrane mimics was reduced, which was explained by the interaction among surface charges (zeta potential) and by hydration forces. Sil-MB and Cab-Th nanoparticles presented in vitro phototoxicity 38% and 20% higher than the respective free PS. It was observed that the nanoparticle coating with lipids and with PEG reduced their photoxicity. Nanoparticles coated with lipids showed higher toxicity in the dark. Confocal fluorescence images of B16 cells showed that nanoparticles with or without lipid coating enter the cells. In the case of lipid-coated nanoparticles a diffuse distribution profile was observed and in the case of nanoparticles without coating, they concentrated in specific vacuolar regions of the cytoplasm. The homogeneous cytoplasmic distribution profile of lipid-coated nanoparticles can explain the increased toxicity in the dark. It has been concluded that immobilization of PS with different aggregation degrees is a strategy to obtain systems in which the modulated efficiency of 1O2 generation is not affected by the external medium. Finally, based on the observed in vitro phototoxicity activity against B16 cells, these systems can be useful in Photodynamic Therapy of Cancer
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Desenvolvimento de nanopartículas fotossensibilizadoras / Development of photosensitizing nanoparticlesDayane Batista Tada 14 December 2007 (has links)
No presente trabalho são apresentadas a síntese e a caracterização estrutural, fotofísica, fotoquímica e fotobiológica de nanopartículas contendo os fotossensibilizadores (FS) Azul de Metileno (AM) e Tionina. AM e Tionina foram incorporados nas nanopartículas sil-AM e sil-Tio pelo processo sol-gel. Nas nanopartículas Cab-Tio, Tionina foi ligada à superfície de sílica CabOsil® através de ligação covalente com reagentes bifuncionais. Todas as nanopartículas mostraram-se esféricas e com de diâmetro médio na faixa de 30 a 60nm. A imobilização dos FS induziu a agregação destes em extensões diferentes para cada tipo de nanopartícula. Foi observado que a maior presença de dímeros de FS leva à menor eficiência de geração de 1O2. Constatou-se que as nanopartículas sofrem pouca influência do meio, uma vez que os FS a elas ligadas não sofreram redução química por NADPH, nem supressão do estado tripleto por íons ascorbato e a supressão de fluorescência por íon brometo foi diminuída. Foi testado também o efeito do recobrimento destas nanopartículas com lipídios dioleilfosfatidil colina (DOPC) e fosfatidilglicerol (PG) e com Polietileno glicol (PEG). A adsorção das nanopartículas sobre membranas miméticas foi reduzida após os recobrimentos, resultado que foi explicado pelas interações de carga superficial (potencial zeta) e pela força de hidratação. As nanopartículas sil-AM e Cab-Tio apresentaram fototoxicidades in vitro, 38% e 20% maiores que os respectivos FS livres. A modificação das nanopartículas de sil-AM com lipídios e com PEG diminuiu a fototoxicidade das mesmas e no caso do recobrimento com lipídios levou ao aumento da toxicidade no escuro. Imagens de microscopia confocal mostraram que as nanopartículas com e sem recobrimento de lipídios entram em células B16. No caso das nanopartículas recobertas, observou-se um perfil de distribuição difuso por todo o citoplasma e no caso de nanopartículas sem recobrimento, estas encontraram-se em poucas regiões vacuolares do citoplasma. O perfil de distribuição homogênea por todo o citoplasma no caso de nanopartículas recobertas com lipídios pode ser o responsável pelo aumento de toxicidade no escuro. Concluiu-se que a ligação dos FS em nanopartículas com diferentes graus de agregação pode ser uma estratégia para obtenção de sistemas com capacidade modulada de geração de 1O2 e com reduzida susceptibilidade às composições do meio. As atividades fototóxicas das nanopartículas contra células B16 mostraram que estas podem ser úteis em Terapia Fotodinâmica de Câncer / In this work we present the synthesis and the characterization (structural, photophysical, photochemical and photobiological) of nanoparticles with incorporated photosensitizers (PS) Methylene Blue (MB) and Thionin. MB and Thionin were incorporated in sil-MB and sil-Th nanoparticles through sol-gel process. In the case of Cab-Th nanoparticles Thionin was linked to the surface of CabOsil® nanoparticles through cross-linking reactions. All nanoparticles were spherical and presented average diameter in the range of 30 to 60nm. Different extension of PS aggregation was observed in each nanoparticle. It was characterized that the higher the proportion of dimers to monomers the smaller the efficiency of singlet oxygen (1O2) generation. It was shown that nanoparticles can protect PS from external interferences, since NADPH did not reduce them, neither were their triplet state quenched by ascorbate ions. Besides, fluorescence quenching by bromide ions was reduced compared to free PS. The effect of covering the nanoparticles with lipids, i.e., di-oleil phosphatidylcholine (DOPC) and phosphatidylglycerol (PG), and with Polyethylene glycol was also tested. The nanoparticle adsorption over membrane mimics was reduced, which was explained by the interaction among surface charges (zeta potential) and by hydration forces. Sil-MB and Cab-Th nanoparticles presented in vitro phototoxicity 38% and 20% higher than the respective free PS. It was observed that the nanoparticle coating with lipids and with PEG reduced their photoxicity. Nanoparticles coated with lipids showed higher toxicity in the dark. Confocal fluorescence images of B16 cells showed that nanoparticles with or without lipid coating enter the cells. In the case of lipid-coated nanoparticles a diffuse distribution profile was observed and in the case of nanoparticles without coating, they concentrated in specific vacuolar regions of the cytoplasm. The homogeneous cytoplasmic distribution profile of lipid-coated nanoparticles can explain the increased toxicity in the dark. It has been concluded that immobilization of PS with different aggregation degrees is a strategy to obtain systems in which the modulated efficiency of 1O2 generation is not affected by the external medium. Finally, based on the observed in vitro phototoxicity activity against B16 cells, these systems can be useful in Photodynamic Therapy of Cancer
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Estudo da transferência de energia tipo Förster em sistemas hóspede-hospedeiro a partir de corantes encapsulados em Zeólita L / Förster-type energy transfer study in host-guest systems of dyes encapsulated in Zeolite L.Trujillo, Loren Nieto 02 October 2015 (has links)
A coleta eficiente da radiação através de processos de transferência de energia de ressonância Förster (FRET, por sua sigla em inglês) constitui uma forma atraente de melhorar aplicações nanotecnológicas que envolvam o uso da radiação solar como fonte de energia. Sistemas constituídos de zeólita L funcionalizada em sua superfície com ftalocianina (PC) foram estudados visando a inativação de patógenos mediante o uso de luz solar natural. No entanto, na velocidade de fotoinativação observou-se uma dependência com a intensidade da radiação que foi relacionada com a absorção ineficiente de PC na região transversal de 400-650 nm da irradiância solar. Visando uma aplicação nesses sistemas, neste trabalho estudou-se a transferência de energia tipo Förster utilizando os corantes catiônicos Pironina Y (PyY) e Tionina (Th) encapsulados na zeólita L que se caracterizam por absorver na região espectral visível onde a absorção de PC é limitada. Os corantes foram inseridos no interior dos canais da zeólita L por um processo de troca iônica e a distância de separação entre estes foi variada com o carregamento das amostras (% de moléculas inseridas em relação ao espaço disponível na zeólita). Foram preparadas amostras com a inserção de PyY e Th nos canais da zeólita L, individualmente, bem como, amostras dos dois corantes misturados aleatoriamente na razão doador:receptor 1,0:1,4. A transferência de energia foi estudada mediante a detecção da emissão sensibilizada do receptor Th quando o doador PyY foi seletivamente excitado nas amostras de PyY-Th-zeólita L e, através da comparação dos tempos de vida de fluorescência do doador na presença e na ausência do receptor. O conjunto de resultados a diferentes carregamentos sugere a FRET nas amostras testadas, no entanto, devido à baixa emissão de Th detectada, o material preparado não seria adequado para a transferência de energia ao PC. / The efficient harvesting of solar energy through Förster Resonance Energy Transfer processes (FRET) is an attractive way to improve nanotechnology applications involving the use of solar radiation as energy source. Systems based on zeolite L functionalized on its surface with phthalocyanine (PC) have been studied to inactivate pathogens by natural sunlight. However, there was observed a dependency between the photoinactivation rate and the radiation intensity which was related to the inefficient absorption of PC in the vertical cross-section of 400-650 nm of the solar spectral irradiance. Aimed at applying in these systems, we studied the Förster type energy transfer between the cationic dyes Pyronin Y (PyY) and Thionin (Th) encapsulated into the zeolite L which are characterized by absorbing in the visible spectral region where the absorption of PC is limited. The dyes were inserted inside the zeolite L channels through ion exchange process, and the separation distance between them was tuned with the sample loading (% of inserted molecules in relation to the available space in the zeolite). Different samples were prepared with one and two randomly mixed dyes keeping the donor:acceptor ratio in 1.0:1.4. The energy transfer was studied by detection of the acceptor sensitized emission when the donor PyY was selectively excited in PyY-Th-zeolite L samples, and by comparison of the donor fluorescence lifetimes in the presence and absence of the acceptor. The set of results in different loadings suggests FRET in the samples tested, however, due to the low detected emission of Th the prepared material would not be appropriate for energy transfer to PC.
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Estudo da transferência de energia tipo Förster em sistemas hóspede-hospedeiro a partir de corantes encapsulados em Zeólita L / Förster-type energy transfer study in host-guest systems of dyes encapsulated in Zeolite L.Loren Nieto Trujillo 02 October 2015 (has links)
A coleta eficiente da radiação através de processos de transferência de energia de ressonância Förster (FRET, por sua sigla em inglês) constitui uma forma atraente de melhorar aplicações nanotecnológicas que envolvam o uso da radiação solar como fonte de energia. Sistemas constituídos de zeólita L funcionalizada em sua superfície com ftalocianina (PC) foram estudados visando a inativação de patógenos mediante o uso de luz solar natural. No entanto, na velocidade de fotoinativação observou-se uma dependência com a intensidade da radiação que foi relacionada com a absorção ineficiente de PC na região transversal de 400-650 nm da irradiância solar. Visando uma aplicação nesses sistemas, neste trabalho estudou-se a transferência de energia tipo Förster utilizando os corantes catiônicos Pironina Y (PyY) e Tionina (Th) encapsulados na zeólita L que se caracterizam por absorver na região espectral visível onde a absorção de PC é limitada. Os corantes foram inseridos no interior dos canais da zeólita L por um processo de troca iônica e a distância de separação entre estes foi variada com o carregamento das amostras (% de moléculas inseridas em relação ao espaço disponível na zeólita). Foram preparadas amostras com a inserção de PyY e Th nos canais da zeólita L, individualmente, bem como, amostras dos dois corantes misturados aleatoriamente na razão doador:receptor 1,0:1,4. A transferência de energia foi estudada mediante a detecção da emissão sensibilizada do receptor Th quando o doador PyY foi seletivamente excitado nas amostras de PyY-Th-zeólita L e, através da comparação dos tempos de vida de fluorescência do doador na presença e na ausência do receptor. O conjunto de resultados a diferentes carregamentos sugere a FRET nas amostras testadas, no entanto, devido à baixa emissão de Th detectada, o material preparado não seria adequado para a transferência de energia ao PC. / The efficient harvesting of solar energy through Förster Resonance Energy Transfer processes (FRET) is an attractive way to improve nanotechnology applications involving the use of solar radiation as energy source. Systems based on zeolite L functionalized on its surface with phthalocyanine (PC) have been studied to inactivate pathogens by natural sunlight. However, there was observed a dependency between the photoinactivation rate and the radiation intensity which was related to the inefficient absorption of PC in the vertical cross-section of 400-650 nm of the solar spectral irradiance. Aimed at applying in these systems, we studied the Förster type energy transfer between the cationic dyes Pyronin Y (PyY) and Thionin (Th) encapsulated into the zeolite L which are characterized by absorbing in the visible spectral region where the absorption of PC is limited. The dyes were inserted inside the zeolite L channels through ion exchange process, and the separation distance between them was tuned with the sample loading (% of inserted molecules in relation to the available space in the zeolite). Different samples were prepared with one and two randomly mixed dyes keeping the donor:acceptor ratio in 1.0:1.4. The energy transfer was studied by detection of the acceptor sensitized emission when the donor PyY was selectively excited in PyY-Th-zeolite L samples, and by comparison of the donor fluorescence lifetimes in the presence and absence of the acceptor. The set of results in different loadings suggests FRET in the samples tested, however, due to the low detected emission of Th the prepared material would not be appropriate for energy transfer to PC.
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