TY - BOOK A1 - Schulz, Burkhard A1 - Orgzall, Ingo A1 - Freydank, Anke-Christine A1 - Chenggang, Xü T1 - Self-organization of substituted 1,3,4-oxadizazoles in the solid state and at surfaces N2 - Different aspects of the structure formation for a class of molecules containing the diphenyl-1,3,4-oxadiazole fragment are discussed. Starting from the bulk state with the ideal crystal lattice and the derivation of some common packing motifs the formation of liquid-crystalline states are described. This leads to the consideration of structures found in Langmuir-Blodgett films and those obtained by organic molecular beam deposition. These structures may again be compared to those for the bulk crystalline state. Common features as well as characteristic differences due to peculiarities of the individual molecular structures are discussed. (c) 2005 Elsevier B.V. All rights reserved Y1 - 2005 ER - TY - THES A1 - Xü, Chenggang T1 - Preparation and characterization of vapour deposited films based on substituted 2,5-diphenyl-1,3,4-oxadiazole derivatives N2 - Diese Arbeit befasst sich mit dem Einfluss der molekularen Struktur von 2,5-Diphenyl-1,3,4-Oxadiazol-Derivaten auf die Präparierung dünner Schichten mittels Vakuumdeposition. Dünne Schichten von diesen Substanzen wurden auf Si/SiO2 aufgedampft und ihre Struktur systematisch mittels XSR, AFM und IR untersucht. Das Ergebnis zeigt, dass die Schichtstrukturen offenbar von Substratetemperatur (Ts) abhängig sind. Im untersuchten Ts-Bereich bilden etherverbrückte Oxadiazole immer geordnete Schichten und die Schichtperiodicität hängt linear von der Längen der aliphatischen Ketten, während sich bei den amidverbrückten Oxadiazolen nur bei hohen Ts geordnete Schichten bilden können. Diese Unterschiede sind auf die intermolekularen Wasserstoffbrücken zurückzuführen. Der Tilt-Winkel der Moleküle ist durch die Wechselwirkung zwischen dem aromatischen Teil bestimmt. Die Wechselwirkungen zwischen den Kopfgruppen können durch Tempern abgeschwächt werden und führen zur Strukturumwandlung von Schichten, die auf etherverbrückten Oxadiazolen basieren. Alle Schichten von etherverbrückten Oxadiazolen haben Doppelschicht-Struktur, aber amidverbrückte Oxadiazole bilden nur Doppelschicht-Strukturen, wenn die Moleküle eine Kopfgruppe besitzen. N2 - The correlations between the chemical structures of the 2,5-diphenyl-1,3,4-oxadiazole compounds and their corresponding vapour deposited film structures on Si/SiO2 were systematically investigated with AFM, XSR and IR for the first time. The result shows that the film structure depends strongly on the substrate temperature (Ts). For the compounds with ether bridge group, the film periodicity depends linearly on the length of the aliphatic chain. The films based on those oxadiazols have ordered structure in the investigated substrate temperature region, while die amide bridged compounds form ordered film only at high Ts due to the formation of intermolecular H-bond. The tilt angle of most molecules is determined by the pi-pi complexes between the molecules. The intermolecular interaction between head groups leads to the structural transformation during the thermal treatment after deposition. All the ether bridged oxadiazoles form films with bilayer structure, while amide bridged oxadiazole form film bilayer structure only when the molecule has a head group. KW - 1 KW - 3 KW - 4-oxadiazol KW - Vapour Deposition KW - Dünnschichten KW - AFM KW - X-ray KW - Infrarot Spektroskopie KW - intermolekülare Wechselwirkung KW - Hochvakuum KW - 1 KW - 3 KW - 4-oxadiazole KW - vapour deposition KW - Thin film KW - AFM KW - X-ray KW - Infrared spectroscopy KW - intermolecular interaction KW - high vacuum Y1 - 2004 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-0001358 ER - TY - JOUR A1 - Sarauli, David A1 - Xu, Chenggang A1 - Dietzel, Birgit A1 - Schulz, Burkhard A1 - Lisdat, Fred T1 - Differently substituted sulfonated polyanilines - the role of polymer compositions in electron transfer with pyrroloquinoline quinone-dependent glucose dehydrogenase JF - Acta biomaterialia N2 - Sulfonated polyanilines have become promising building blocks in the construction of biosensors, and therefore we use here differently substituted polymer forms to investigate the role of their structural composition and properties in achieving a direct electron transfer with the redox enzyme pyrroloquinoline quinone-dependent glucose dehydrogenase (PQQ-GDH). To this end, new copolymers containing different ratios of 2-methoxyaniline-5-sulfonic acid (MAS), 3-aminobenzenesulfonic acid (ABS) and 3-aminobenzoic acid (AB) units have been chemically synthesized. All polymers have been studied with respect to their ability to react directly with PQQ-GDH. This interaction has been monitored initially in solution, and subsequently on electrode surfaces. The results show that only copolymers with MAS and aniline units can directly react with PQQ-GDH in solution; the background can be mainly ascribed to the emeraldine salt redox state of the polymer, allowing rather easy reduction. However, when polymers and the enzyme are immobilized on the surface of carbon nanotube-containing electrodes, direct bioelectrocatalysis is also feasible in the case of copolymers composed of ABS/AB and MAS/AB units, existing initially in pernigraniline base form. This verifies that a productive interaction of the enzyme with differently substituted polymers is feasible when the electrode potential can be used to drive the reaction towards the oxidation of the substrate-reduced enzyme. These results clearly demonstrate that enzyme electrodes based on sulfonated polyanilines and direct bioelectrocatalysis can be successfully constructed. KW - Sulfonated polyaniline KW - PQQ-dependent glucose dehydrogenase KW - Direct electron transfer KW - Immobilization KW - Bioelectrocatalysis Y1 - 2013 U6 - https://doi.org/10.1016/j.actbio.2013.06.008 SN - 1742-7061 VL - 9 IS - 9 SP - 8290 EP - 8298 PB - Elsevier CY - Oxford ER - TY - JOUR A1 - Schulz, Burkhard A1 - Dietzel, Birgit A1 - Orgzall, Ingo A1 - Diez, Isabel A1 - Xu, Chenggang T1 - Aspects of morphology control during the oxidative synthesis of electrically conducting polymers N2 - The formation of micro- and nanostructures during the oxidative polymerization of polypyrrole and polyaniline is investigated using different sulfonic acid dopants. Rod- or tube-like structures are found in polypyrrole as well as in polyaniline without addition of further compounds to the initial reaction mixture of monomer, dopant and oxidant. In these cases, always a crystalline precursor complex composed of a dopand molecule and the pure monomer (aniline) or a trimeric moiety (pyrrole) serves as in-situ template. In most cases the surface of the growing polymer is covered by secondary structures with much smaller sizes so that a hierarchical order of structures at different length scales results. Corresponding model considerations for the polymerization process are outlined. Additionally, unusual structures like platelets, frames, rings, or ribbons are observed in the polypyrrole synthesis in the presence of fluorosurfactants. Y1 - 2009 UR - http://hip.sagepub.com/ U6 - https://doi.org/10.1177/0954008309339933 SN - 0954-0083 ER - TY - JOUR A1 - Sarauli, David A1 - Xu, Chenggang A1 - Dietzel, Birgit A1 - Schulz, Burkhard A1 - Lisdat, Fred T1 - A multilayered sulfonated polyaniline network with entrapped pyrroloquinoline quinone-dependent glucose dehydrogenase: tunable direct bioelectrocatalysis JF - Journal of materials chemistry : B, Materials for biology and medicine N2 - A feasible approach to construct multilayer films of sulfonated polyanilines - PMSA1 and PABMSA1 containing different ratios of aniline, 2-methoxyaniline-5-sulfonic acid (MAS) and 3-aminobenzoic acid (AB), with the entrapped redox enzyme pyrroloquinoline quinone-dependent glucose dehydrogenase (PQQ-GDH) on Au and ITO electrode surfaces, is described. The formation of layers has been followed and confirmed by electrochemical impedance spectroscopy (EIS), which demonstrates that the multilayer assembly can be achieved in a progressive and uniform manner. The gold and ITO electrodes subsequently modified with PMSA1:PQQ-GDH and PABMSA1 films are studied by cyclic voltammetry (CV) and UV-Vis spectroscopy which show a significant direct bioelectrocatalytical response to the oxidation of the substrate glucose without any additional mediator. This response correlates linearly with the number of deposited layers. Furthermore, the constructed polymer/enzyme multilayer system exhibits a rather good long-term stability, since the catalytic current response is maintained for more than 60% of the initial value even after two weeks of storage. This verifies that a productive interaction of the enzyme embedded in the film of substituted polyaniline can be used as a basis for the construction of bioelectronic units, which are useful as indicators for processes liberating glucose and allowing optical and electrochemical transduction. Y1 - 2014 U6 - https://doi.org/10.1039/c4tb00336e SN - 2050-750X SN - 2050-7518 VL - 2 IS - 21 SP - 3196 EP - 3203 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Sarauli, David A1 - Peters, Kristina A1 - Xu, Chenggang A1 - Schulz, Burkhard A1 - Fattakhova-Rohlfing, Dina A1 - Lisdat, Fred T1 - 3D-Electrode architectures for enhanced direct bioelectrocatalysis of pyrroloquinoline quinone-dependent glucose dehydrogenase JF - ACS applied materials & interfaces N2 - We report on the fabrication of a complex electrode architecture for efficient direct bioelectrocatalysis. In the developed procedure, the redox enzyme pyrroloquinoline quinone-dependent glucose dehydrogenase entrapped in a sulfonated polyaniline [poly(2-methoxyaniline-5-sulfonic acid)-co-aniline] was immobilized on macroporous indium tin oxide (macroITO) electrodes. The use of the 3D-conducting scaffold with a large surface area in combination with the conductive polymer enables immobilization of large amounts of enzyme and its efficient communication with the electrode, leading to enhanced direct bioelectrocatalysis. In the presence of glucose, the fabricated bioelectrodes show an exceptionally high direct bioelectrocatalytical response without any additional mediator. The catalytic current is increased more than 200-fold compared to planar ITO electrodes. Together with a high long-term stability (the current response is maintained for >90% of the initial value even after 2 weeks of storage), the transparent 3D macroITO structure with a conductive polymer represents a valuable basis for the construction of highly efficient bioelectronic units, which are useful as indicators for processes liberating glucose and allowing optical and electrochemical transduction. KW - 3D electrode structures KW - macroITO KW - conductive polymer KW - PQQ-GDH KW - direct bioelectrocatalysis KW - bioelectrochemistry Y1 - 2014 U6 - https://doi.org/10.1021/am5046026 SN - 1944-8244 VL - 6 IS - 20 SP - 17887 EP - 17893 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Sarauli, David A1 - Xu, Chenggang A1 - Dietzel, Birgit A1 - Stiba, Konstanze A1 - Leimkühler, Silke A1 - Schulz, Burkhard A1 - Lisdat, Fred T1 - Thin films of substituted polyanilines interactions with biomolecular systems JF - Soft matter N2 - We use substituted polyanilines for the construction of new polymer electrodes for interaction studies with the redox protein cytochrome c (cyt c) and the enzyme sulfite oxidase (SO). For these purposes four different polyaniline copolymers are chemically synthesized. Three of them are copolymers, containing 2-methoxyaniline-5-sulfonic acid with variable ratios of aniline; the fourth copolymer consists of 3-amino-benzoic acid and aniline. The results show that all polymers are suitable for being immobilized as thin stable films on gold wire and indium tin oxide (ITO) electrode surfaces from DMSO solution. This can be demonstrated by cyclic voltammetry and UV-Vis spectroscopy measurements. Moreover, cyt c can be electrochemically detected not only in solution, but also immobilized on top of the polymer films. Furthermore, the appearance of a significant catalytic current has been demonstrated for the sulfonated polyanilines, when the polymer-coated protein electrode is being measured upon addition of sulfite oxidase, confirming the establishment of a bioanalytical signal chain. Best results have been obtained for the polymer with highest sulfonation grade. The redox switching of the polymer by the enzymatic reaction can also be analyzed by following the spectral properties of the polymer electrode. Y1 - 2012 U6 - https://doi.org/10.1039/c2sm07261k SN - 1744-683X VL - 8 IS - 14 SP - 3848 EP - 3855 PB - Royal Society of Chemistry CY - Cambridge ER - TY - GEN A1 - Sarauli, David A1 - Xu, Chenggang A1 - Dietzel, Birgit A1 - Schulz, Burkhard A1 - Lisdat, Fred T1 - A multilayered sulfonated polyaniline network with entrapped pyrroloquinoline quinone-dependent glucose dehydrogenase BT - tunable direct bioelectrocatalysis N2 - A feasible approach to construct multilayer films of sulfonated polyanilines – PMSA1 and PABMSA1 – containing different ratios of aniline, 2-methoxyaniline-5-sulfonic acid (MAS) and 3-aminobenzoic acid (AB), with the entrapped redox enzyme pyrroloquinoline quinone-dependent glucose dehydrogenase (PQQ-GDH) on Au and ITO electrode surfaces, is described. The formation of layers has been followed and confirmed by electrochemical impedance spectroscopy (EIS), which demonstrates that the multilayer assembly can be achieved in a progressive and uniform manner. The gold and ITO electrodes subsequently modified with PMSA1:PQQ-GDH and PABMSA1 films are studied by cyclic voltammetry (CV) and UV-Vis spectroscopy which show a significant direct bioelectrocatalytical response to the oxidation of the substrate glucose without any additional mediator. This response correlates linearly with the number of deposited layers. Furthermore, the constructed polymer/enzyme multilayer system exhibits a rather good long-term stability, since the catalytic current response is maintained for more than 60% of the initial value even after two weeks of storage. This verifies that a productive interaction of the enzyme embedded in the film of substituted polyaniline can be used as a basis for the construction of bioelectronic units, which are useful as indicators for processes liberating glucose and allowing optical and electrochemical transduction. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 275 Y1 - 2014 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-98744 ER -