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Institute
- Institut für Chemie (3405) (remove)
Funktionalisierte Poly(2-oxazoline) als neue Materialien stellen sowohl unter strukturellen Gesichtspunkten als auch im Hinblick auf potentielle Anwendungen eine interessante Polymerklasse dar. Die Ausbildung von hierarchischen Strukturen mit Poly(2-oxazolinen) über intermolekulare Wasserstoffbrückenbindungen ist hierbei ein bisher nicht beachteter Aspekt. Über einen bioinspirierten Ansatz sollten gezielt funktionelle Gruppen, die für einen hierarchischen Aufbau, z.B. in Proteinen, verantwortlich sind, in vereinfachter Weise auf die synthetische Substanzklasse der Poly(2-oxazoline) übertragen werden. Die vorliegende Arbeit beschäftigt sich mit der modularen Synthese neuer, funktionalisierter Poly(2-oxazolin) Homo- und Copolymere. Ausgehend von der Synthese von 2-(3-Butenyl)-2-oxazolin wurden definierte Präpolymere in einer kationischen Isomerisierungspolymerisation unter kontrolliert/„lebenden“ Bedingungen hergestellt. In einer anschließenden „Thio-Click“ (Thiol-En-Reaktion) Modifizierungsreaktion wurden die gewünschten funktionellen Gruppen quantitativ eingeführt. Hydroxylierte Poly(2-oxazoline) wurden hinsichtlich ihres Aggregationsverhaltens in Wasser untersucht. Bereits die jeweiligen Homopolymere bildeten aufgrund von intermolekularen Wasserstoffbrückenbindungen supramolekulare tubuläre Nanofasern aus. Durch Einsatz verschiedener analytischer Methoden konnte die innere Struktur der Nanoröhren beschrieben und ein entsprechendes Modell aufgestellt werden. Die dargestellten funktionellen Poly(2-oxazoline) wurden hinsichtlich ihrer Anwendung als potentielle, synthetische „antifreeze additives“ untersucht. Alle Polymere besitzen eine ausgeprägte Tendenz zur Nukleierung von Wasser und führen daher zu signifikanten Änderungen der Eismorphologie. Des weiteren wurde ein carboxyliertes Derivat zur biomimetischen Mineralisation von Kalziumcarbonat eingesetzt und nach phänomenologischen Gesichtspunkten untersucht.
Nanostructured materials are materials consisting of nanoparticulate building blocks on the scale of nanometers (i.e. 10-9 m). Composition, crystallinity and morphology can enhance or even induce new properties of the materials, which are desirable for todays and future technological applications. In this work, we have shown new strategies to synthesise metal oxide and metal nitride nanomaterials. The first part of the work deals with the study of nonaqueous synthesis of metal oxide nanoparticles. We succeeded in the synthesis of In2O3 nanopartcles where we could clearly influence the morphology by varying the type of the precursors and the solvents; of ZnO mesocrystals by using acetonitrile as a solvent; of transition metal oxides (Nb2O5, Ta2O5 and HfO2) that are particularly hard to obtain on the nanoscale and other technologically important materials. Solvothermal synthesis however is not restricted to formation of oxide materials only. In the second part we show examples of nonaqueous, solvothermal reactions of metal nitrides, but the main focus lies on the investigation of the influence of different morphologies of metal oxide precursors on the formation of the metal nitride nanoparticles. In spite of various reports, the number and variety of nanocrystalline metal nitrides is marginally small by comparison to metal oxides; hence preformed metal oxides as precursors for the preparation of metal nitrides are a logical choice. By reacting oxide nanoparticles with cyanamide, urea or melamine, at temperatures of 800 to 900 °C under nitrogen flow metal nitrides could be obtained. We studied in detail the influence of the starting material and realized that size, crystallinity, type of nitrogen source and temperature play the most important role. We have managed to propose and verify a dissolution-recrystallisation model as the formation mechanism. Furthermore we could show that the initial morphology of the oxides could be retained when ammonia flow was used instead.
In dieser Arbeit wird durch Modellrechnungen gezeigt, wie die Stickstoffinversion in Azacyclen als molekularer Schalter genutzt werden könnte. Hierzu werden ein Fluorazetidin- und ein Fluorazacyclopentanderviat quantenchemisch untersucht. Das letztere Molekül wird auch quantendynamisch untersucht. Jedes der beiden Moleküle besitzt zwei stabile Konformationen. Es wird gezeigt, dass das Azabicyclopentanderivat von der einen Konformation mittels zweier linear polarisierter IR-Laserpulse durch sogenanntes “ladder climbing” in die andere überführt werden kann.
For more than 70 years, understanding of the mechanism of particle nucleation in emulsion polymerization has been one of the most challenging issues in heterophase polymerization research. Within this work a comprehensive experimental study of particle nucleation in emulsion polymerization of styrene at 70 °C and variety of conditions has been performed. To follow the onset of nucleation, on-line conductivity measurements were applied. This technique is highly sensitive to the mobility of conducting species and hence, it can be employed to follow aggregation processes leading to particle formation. On the other hand, by recording the optical transmission (turbidity) of the reaction mixture particle growth was followed. Complementary to the on-line investigations, off-line characterizations of the particle morphology and the molecular weight have been performed. The aim was to achieve a better insight in the processes taking place after starting the reaction via particle nucleation until formation of colloidally stable latex particles. With this experimental protocol the initial period of styrene emulsion polymerization in the absence as well as in the presence of various surfactants (concentrations above and below the critical micellization concentration) and also in the presence of seed particles has been investigated. Ionic and non-ionic initiators (hydrophilic and hydrophobic types) have been applied to start the polymerizations. Following the above algorithm, experimental evidence has been obtained showing the possibility of performing surfactant-free emulsion polymerization of styrene with oil-soluble initiators. The duration of the pre-nucleation period (that is the time between starting the polymerization and nucleation) can be precisely adjusted with the initiator hydrophobicity, the equilibration time of styrene in water, and the surfactant concentration. Spontaneous emulsification of monomer in water, as soon as both phases are brought into contact, is a key factor to explain the experimental results. The equilibration time of monomer in water as well as the type and concentration of other materials in water (surfactants, seed particles, etc.) control the formation rate and the size of the emulsified droplets and thus, have a strong influence on the particle nucleation and the particle morphology. One of the main tasks was to investigate the effect of surfactant molecules and especially micelles on the nucleation mechanism. Experimental results revealed that in the presence of emulsifier micelles the conductivity pattern does not change essentially. This means that the presence of emulsifiers does not change the mechanism of particle formation qualitatively. However, surfactants assist in the nucleation process as they lower the activation free energy of particle formation. Contrary, seed particles influence particle nucleation, substantially. In the presence of seed particles above a critical volume fraction the formation of new particles can be suppressed. However, micelles and seed particles as absorbers exhibit a common behavior under conditions where monomer equilibration is not allowed. Results prove that the nucleation mechanism comprises the initiation of water soluble oligomers in the aqueous phase followed by their aggregation. The process is heterogeneous in nature due to the presence of monomer droplets.
Chitooligosaccharides are composed of linear β-(1→4)-linked 2-acetamido-2-deoxy-β-D-glucopyranose (GlcNAc) and/or 2-amino-2-deoxy-β-D-glucopyranose (GlcN). They are of interest due to their remarkable biological properties including antibacterial, antitumor, antifungal and elicitor activities. They can be obtained from the aminoglucan chitosan by chemical or enzymatic degradation which obviously affords rather heterogenous mixtures. On the other hand, chemical synthesis provides pure compounds with defined sequences of GlcNAc and GlcN monomers. The synthesis of homo- and hetero-chitobioses and hetero-chitotetraoses is described in this thesis. Dimethylmaleoyl and phthaloyl groups were used for protection of the amines. The donor was activated as the trichloroacetimidate in order to form the β-linkages. Glycosylation in the presence of trimethylsilyl trifluoromethanesulfonate, followed by N- and O-deprotection furnished chitobioses and chitotetraoses in good yields.
Die Arbeit beschreibt die Synthese, Charakterisierung und Anwendung von meso- und mikroporösen Hochleistungspolymeren. Im ersten Teil wird die Synthese von mesoporösen Polybenzimidazol (PBI) auf der Basis einer Templatierungsmethode vorgestellt. Auf der Grundlage kommerzieller Monomere und Silikatnanopartikel sowie eines neuen Vernetzers wurde ein Polymer-Silikat-Hybridmaterial aufgebaut. Das Herauslösen des Silikats mit Ammoniumhydrogendifluorid führt zu mesoporösen Polybenzimidazolen mit spherischen Poren von 9 bis 11 nm Durchmesser. Die Abhängigkeit der beobachteten Porosität vom Massenverhältnis Silikat zu Polymer wurde ebenso untersucht wie die Abhängigkeit der Porosität vom Vernetzergehalt. Die Porosität vollvernetzter Proben zeigt eine lineare Abhängigkeit vom Verhältnis Silikat zu Polymer bis zu einem Grenzwert von 1. Wird der Grenzwert überschritten, ist teilweiser Porenkollaps zu beobachten. Die Abhängigkeit der Porosität vom Vernetzergehalt bei festem Silikatgehalt ist nichtlinear. Oberhalb einer kritischen Vernetzerkonzentration wird eine komplette Replikation der Nanopartikel gefunden. Ist die Vernetzerkonzentration dagegen kleiner als der kritische Wert, so ist der völlige Kollaps einiger Poren bei Stabilität der verbleibenden Poren zu beobachten. Ein komplett unporöses PBI resultiert bei Abwesenheit des Vernetzers. Die mesoporösen PBI-Netzwerke konnten kontrolliert mit Phosphorsäure beladen werden. Die erhaltenen Addukte wurden auf ihre Protonenleitfähigkeit untersucht. Es kann gezeigt werden, dass die Nutzung der vordefinierten Morphologie im Vergleich zu einem unstrukturierten PBI in höheren Leitfähigkeiten resultiert. Durch die vernetzte Struktur war des Weiteren genügend mechanische Stabilität gegeben, um die Addukte reversibel und bei sehr guten Leitfähigkeiten bis zu Temperaturen von 190°C bei 0% relativer Feuchtigkeit zu untersuchen. Dies ist für unstrukturierte Phosphorsäure/PBI - Addukte aus linearem PBI nicht möglich. Im zweiten Teil der Arbeit wird die Synthese intrinsisch mikroporöser Polyamide und Polyimide vorgestellt. Das Konzept intrinsisch mikroporöser Polymere konnte damit auf weitere Polymerklassen ausgeweitet werden. Als zentrales, strukturinduzierendes Motiv wurde 9,9'-Spirobifluoren gewählt. Dieses Molekül ist leicht und vielfältig zu di- bzw. tetrafunktionellen Monomeren modifizierbar. Dabei wurden bestehende Synthesevorschriften modifiziert bzw. neue Vorschriften entwickelt. Ein erster Schwerpunkt innerhalb des Kapitels lag in der Synthese und Charakterisierung von löslichen, intrinsisch mikroporösen, aromatischen Polyamid und Polyimid. Es konnte gezeigt werden, dass das Beobachten von Mikroporosität stark von der molekularen Architektur und der Verarbeitung der Polymere abhängig ist. Die Charakterisierung der Porosität erfolgte unter Nutzung von Stickstoffsorption, Kleinwinkelröntgenstreuung und Molecular Modeling. Es konnte gezeigt werden, dass die Proben stark vom Umgebungsdruck abhängigen Deformationen unterliegen. Die starke Quellung der Proben während des Sorptionsvorgangs konnte durch Anwendung des "dual sorption" Modells, also dem Auftreten von Porenfüllung und dadurch induzierter Henry-Sorption, erklärt werden. Der zweite Schwerpunkt des Kapitels beschreibt die Synthese und Charakterisierung mikroporöser Polyamid- und Polyimidnetzwerke. Während Polyimidnetzwerke auf Spirobifluorenbasis ausgeprägte Mikroporosität und spezifische Oberflächen von ca. 1100 m²/g aufwiesen, war die Situation für entsprechende Polyamidnetzwerke abweichend. Mittels Stickstoffsorption konnte keine Mikroporosität nachgewiesen werden, jedoch konnte mittels SAXS eine innere Grenzfläche von ca. 300 m²/g nachgewiesen werden. Durch die in dieser Arbeit gezeigten Experimente kann die Grenze zwischen Polymeren mit hohem freien Volumen und mikroporösen Polymeren somit etwas genauer gezogen werden. ausgeprägte Mikroporosität kann nur in extrem steifen Strukturen nachgewiesen werden. Die Kombination der Konzepte "Mesoporosität durch Templatierung" und "Mikroporosität durch strukturierte Monomere" hatte ein hierarchisch strukturiertes Polybenzimidazol zum Ergebnis. Die Präsenz einer Strukturierung im molekularen Maßstab konnte SAXS bewiesen werden. Das so strukturierte Polybenzimidazol zeichnete sich durch eine höhere Protonenleitfähigkeit im Vergleich zu einem rein mesoporösen PBI aus. Der letzte Teil der Arbeit beschäftigte sich mit der Entwicklung einer neuen Synthesemethode zur Herstellung von Polybenzimidazol. Es konnte gezeigt werden, dass lineares PBI in einer eutektischen Salzschmelze aus Lithium- und Kaliumchlorid synthetisiert werden kann. Die Umsetzung der spirobifluorenbasierten Monomere zu löslichem oder vernetztem PBI ist in der Salzschmelze möglich.
Characterisation of silica in Equisetum hyemale and its transformation into biomorphous ceramics
(2007)
Equisetum spp. (horsetail / “Schachtelhalm”) is the only surviving genus of the primitive Sphenopsids vascular plants which reached their zenith during the Carboniferous era. It is an herbaceous plant and is distinguished by jointed stems with fused whorl of nodal leaves. The plant has been used for scouring kitchen utensils and polishing wood during the past time due to its high silica encrustations in the epidermis. Equisetum hyemale (scouring rush) can accumulate silica up to 16% dry weight in its tissue, which makes this plant an interesting candidate as a renewable resource of silica for the synthesis of biomorphous ceramics. The thesis comprises a comprehensive experimental study of silica accumulations in E.hyemale using different characterisation techniques at all hierarchical levels. The obtained results shed light on the local distribution, chemical form, crystallinity, and nanostructure of biogenic silica in E.hyemale which were quite unclear until now. Furthermore, isolation of biogenic silica from E.hyemale to obtain high grade mesoporous silica with high purity is investigated. Finally, syntheses of silicon carbide (b-SiC) by a direct thermoconversion process of E.hyemale is attempted, which is a promising material for high performance ceramics. It is found that silica is deposited continuously on the entire epidermal layer with the highest concentration on the knobs. The highest silicon content is at the knob tips (≈ 33%), followed by epidermal flank (≈ 17%), and inner lower knob (≈ 6%), whereas there is almost no silicon found in the interior parts. Raman spectroscopy reveals the presence of at least two silica modifications in E.hyemale. The first type is pure hydrated amorphous silica restricted to the knob tips. The second type is accumulated on the entire continuous outer layer adjacent to the epidermis cell walls. It is lacking silanol groups and is intimately associated with polysaccharides (cellulose, hemicellulose, pectin) and inorganic compounds. Silica deposited in E.hyemale is found to be mostly amorphous with almost negligible amounts of crystalline silica in the form of a-quartz (< 7%). The silica primary particles have a plate-like shape with a thickness of about 2 nm. Pure mesoporous amorphous silica with an open surface area up to 400 m2/g can be obtained from E.hyemale after leaching the plant with HCl to remove the inorganic impurities followed by a calcination treatment. The optimum calcination temperature appears to be around 500°C. Calcination of untreated E.hyemale causes a collapse of the biogenic silica structure which is mainly attributed to the detrimental action of alkali ions present in the native plant. Finally, pure b-SiC with a surface area of about 12 m2/g is obtained upon direct pyrolysis of HCl-treated E.hyemale samples in argon atmosphere. The original structure of native E.hyemale is substantially retained in the biomorphous b-SiC. The results of this thesis lead to a better understanding of the silicification process and allow to draw conclusions about the role of silica in E.hyemale. In particular, a templating role of the plant biopolymers for the synthesis of the nanostructured silica within the plant body can be deduced. Moreover, the high grade ultrafine amorphous silica isolated from E.hyemale promises applications as adsorbent and catalyst support and as silica source for the fabrication of silica-based composites. The synthesis of biomorphous b-SiC from sustainable and low-cost E.hyemale is still in its initial stage. The present thesis demonstrates the principal possibility of carbothermal synthesis of SiC from E.hyemale with the prospect of potential applications, for instance as refractory materials, catalyst supports, or high performance advanced ceramics.
The aim of this work was the generation of carbon materials with high surface area, exhibiting a hierarchical pore system in the macro- and mesorange. Such a pore system facilitates the transport through the material and enhances the interaction with the carbon matrix (macropores are pores with diameters > 50 nm, mesopores between 2 – 50 nm). Thereto, new strategies for the synthesis of novel carbon materials with designed porosity were developed that are in particular useful for the storage of energy. Besides the porosity, it is the graphene structure itself that determines the properties of a carbon material. Non-graphitic carbon materials usually exhibit a quite large degree of disorder with many defects in the graphene structure, and thus exhibit inherent microporosity (d < 2nm). These pores are traps and oppose reversible interaction with the carbon matrix. Furthermore they reduce the stability and conductivity of the carbon material, which was undesired for the proposed applications. As one part of this work, the graphene structures of different non-graphitic carbon materials were studied in detail using a novel wide-angle x-ray scattering model that allowed precise information about the nature of the carbon building units (graphene stacks). Different carbon precursors were evaluated regarding their potential use for the synthesis shown in this work, whereas mesophase pitch proved to be advantageous when a less disordered carbon microstructure is desired. By using mesophase pitch as carbon precursor, two templating strategies were developed using the nanocasting approach. The synthesized (monolithic) materials combined for the first time the advantages of a hierarchical interconnected pore system in the macro- and mesorange with the advantages of mesophase pitch as carbon precursor. In the first case, hierarchical macro- / mesoporous carbon monoliths were synthesized by replication of hard (silica) templates. Thus, a suitable synthesis procedure was developed that allowed the infiltration of the template with the hardly soluble carbon precursor. In the second case, hierarchical macro- / mesoporous carbon materials were synthesized by a novel soft-templating technique, taking advantage of the phase separation (spinodal decomposition) between mesophase pitch and polystyrene. The synthesis also allowed the generation of monolithic samples and incorporation of functional nanoparticles into the material. The synthesized materials showed excellent properties as an anode material in lithium batteries and support material for supercapacitors.
Zur selektiven Entfernung von Schwermetallen aus industriellen Abwässern und Prozesslösungen der metallverarbeitenden Industrie werden synthetische metallkomplexierende funktionelle Polymere – mit Iminodiessigsäure (IDE) als aktive Spezies – seit Jahren erfolgreich zur Eliminierung störender Kationen eingesetzt. Ständig steigende Anforderungen an die Qualität der aufzubereitenden Wässer verlangen nach leistungsfähigen Selektivaustauschern, die den Erhalt der Eigenschaften von Prozesslösungen (z. B. pH-Wert, Salzgehalt) ermöglichen. Ziel der Untersuchungen war es, die strukturellen Matrixeinflüsse auf Beladung, Kapazität, Selektivität und Kinetik durch Variation der Matrix und der experimentellen Bedingungen näher zu untersuchen. Auf Basis einer monodispersen Erstsubstitution eines Styren-Divinylbenzen-Copolymerisates wurde durch gezielten Einbau funktioneller Gruppen – Synthese mit differenziertem Substitutionsgrad (TK/N 1-2) – versucht, systematisch den Einfluss des Substitutionsgrades der Matrix auf die Eigenschaften der Ionenaustauscher zu analysieren. Methodisch geordnet wurden zunächst die Versuche nach dem Batch- und anschließend nach dem Säulenverfahren durchgeführt und parallel dazu die Matrix charakterisiert. Das Verhalten der funktionellen Ankergruppen in Abhängigkeit vom pH-Wert der Lösung (pH-Bereich 2 - 5) wurde untersucht, der optimale Anreicherungs-pH-Wert, die maximale Beladung (Kapazität) und Selektivität der unterschiedlich substituierten Proben für die Schwermetall-Ionen Cu, Zn, Ni, Cd, Pb und Co ermittelt. Den statischen Versuchen folgten dynamische Untersuchungen im Säulenverfahren. Ziel war die Ermittlung des Durchbruchverhaltens und der Durchbruchkapazität bei optimalem pH-Wert in Abhängigkeit vom Substitutionsgrad gegenüber den Einzelmetallionen (Cu, Ni, Zn) und ausgewählten Paaren (Cu/Ni, Cu/Zn, Ni/Zn). Alle Ionenaustauscher wurden ausschließlich in der Ca-Form eingesetzt.
Die vorliegende Arbeit beschäftigt sich mit der Synthese monodisperser, multifunktionaler Poly(amidoamine) (PAAs). Die Klasse der PAAs ist besonders interessant für eine Anwendung im Bereich der Biomedizin, da sie meist nicht toxisch ist, eine sehr geringe Immunogenizität zeigt und eine erhöhte Zellmembranpermeabilität besitzt. Allerdings ist der Einsatz linearer PAAs bisher limitiert, da ihre Synthese nur den Zugang von hoch-polydispersen Systemen mit einer streng alternierenden oder statistischen Verteilung von Funktionalitäten erlaubt. Es ist daher von großem Interesse diese Polymerklasse durch die Möglichkeit eines sequenzdefinierten Aufbaus und der Integration von neuen Funktionalitäten zu verbessern. Um dies zu ermöglichen, wurden, vergleichbar mit der etablierten Festphasensynthese von Peptiden, schrittweise funktionale Disäure- und Diamin-Bausteine an ein polymeres Träger-Harz addiert. Der sequenzielle Aufbau ermöglicht die Synthese monodisperser PAAs und die Kontrolle über die Monomersequenz. Die Wahl der Monomer-Bausteine und ihrer Funktionalitäten kann dabei für jede Addition neu getroffen werden und entscheidet so über die Sequenz der Funktionalitäten im Polymerrückgrat. Die verwendete Chemie entspricht dabei der Standardpeptidchemie, so dass mit Hilfe eines Peptidsynthese-Automaten die Synthese vollständig automatisiert werden konnte. Die Verwendung spezieller Trägerharze, die bereits mit einem synthetischen Polymerblock wie PEO oder auch mit einem Peptid vorbeladen waren, erlaubt die direkte Synthese von PEO- und Peptid-PAA Blockcopolymeren. Da die hier dargestellten PAAs später auf ihre Eignung als multivalente Polykationen in der Gentherapie getestet werden sollten, wurden zunächst Bausteine gewählt, die den Einbau verschiedener Aminfunktionalitäten ermöglichen. Die Bausteine müssen dabei so gewählt sein, dass sie kompatibel sind mit der Chemie des Peptidsynthesizers und eine quantitative Addition ohne Neben- oder Abbruchreaktionen garantieren. Darüber hinaus ist der Einbau von Peptidsequenzen und Disulfid-Einheiten in die PAA-Kette möglich, die z. B. für einen selektiven Abbau des Polymers im Organismus genutzt werden können. Zusammenfassend lässt sich feststellen, dass die in dieser Arbeit vorgestellten PAA-Systeme großes Potenzial als nicht-virale Vektoren für die Gentransfektion bieten. Sie sind nicht toxisch und zeigen Zellaufnahme-Effizienzen von bis zu 77%. Die Gentransfereffizienz ist im Vergleich zu etablierten Polymer-Vektoren zwar noch sehr gering, aber die bisherigen Versuche zeigen bereits eine mögliche Ursache, nämlich die schlechte Freisetzung des Genmaterials innerhalb der Zelle. Eine Lösung dieses Problems bietet jedoch die weitere Modifizierung der PAA-Systeme durch den Einbau von Sollbruchstellen. Diese Sollbruchstellen ermöglichen einen programmierten Abbau des Polymers innerhalb der Zelle und damit sollte die Freisetzung des Genmaterials vom Träger deutlich erleichtert werden. Mögliche Bruchstellen sind z. B. enzymatisch gezielt spaltbare Peptideinheiten oder Disulfid-Einheiten, wie sie bereits als Bausteine für die PAA-Synthese vorgestellt wurden (vergl. Kapitel 4.4). Da nur innerhalb der Zelle ein reduzierendes elektrochemisches Potential besteht, werden z. B. Disulfid-Einheiten auch nur dort gespalten und bieten außerhalb der Zelle ausreichende Stabilität zum Erhalt der Polyplexstruktur. Neben einer Anwendung in der Gentherapie bieten die hier vorgestellten PAA-Systeme den Vorteil einer systematischen Untersuchung von Struktur-Eigenschafts-Beziehungen der Polyplexe. Es wurden verschiedene Zusammenhänge zwischen der chemischen Struktur der PAA-Segmente und der Art und Stärke der DNS-Komprimierung aufgezeigt. Die Komprimierungsstärke wiederum zeigte deutlichen Einfluss auf die Internalisierungsrate und damit auch Transfektionseffizienz. Darüber hinaus zeigte sich ein drastischer Einfluss des PEO-Blocks auf die Stabilisierung der Polyplexe sowie deren intrazelluläre Freisetzung bei Zusatz von Chloroquin. Dennoch bleiben aufgrund der Komplexität der Zusammenhänge noch viele Mechanismen der Transfektion unverstanden, und es muss Aufgabe folgender Arbeiten sein, das Potential der hier eingeführten monodispersen PAA-Systeme weiter auszuloten. So wäre z. B. eine Korrelation der Kettenlänge mit den Parametern der Polyplexbildung, der Zellaufnahme und Transfektionseffizienz von großem Interesse. Darüber hinaus bietet der Einbau von Sollbruchstellen wie kurzen Peptidsequenzen oder den hier bereits eingeführten Disulfid-Einheiten neue Möglichkeiten der gezielten Freisetzung und des programmierten Abbaus, die näher untersucht werden müssen. Neben der Anwendung im Bereich der Gentransfektion sind außerdem andere Gebiete für den Einsatz von monodispersen multifunktionalen PAAs denkbar, da diese kontrollierbare und einstellbare Wechselwirkungen ermöglichen.