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Technologically important, environmentally friendly InP quantum dots (QDs) typically used as green and red emitters in display devices can achieve exceptional photoluminescence quantum yields (PL QYs) of near-unity (95-100%) when the-state-of-the-art core/shell heterostructure of the ZnSe inner/ZnS outer shell is elaborately applied. Nevertheless, it has only led to a few industrial applications as QD liquid crystal display (QD–LCD) which is applied to blue backlight units, even though QDs has a lot of possibilities that able to realize industrially feasible applications, such as QD light-emitting diodes (QD‒LEDs) and luminescence solar concentrator (LSC), due to their functionalizable characteristics.
Before introducing the main research, the theoretical basis and fundamentals of QDs are described in detail on the basis of the quantum mechanics and experimental synthetic results, where a concept of QD and colloidal QD, a type-I core/shell structure, a transition metal doped semiconductor QDs, the surface chemistry of QD, and their applications (LSC, QD‒LEDs, and EHD jet printing) are sequentially elucidated for better understanding. This doctoral thesis mainly focused on the connectivity between QD materials and QD devices, based on the synthesis of InP QDs that are composed of inorganic core (core/shell heterostructure) and organic shell (surface ligands on the QD surface). In particular, as for the former one (core/shell heterostructure), the ZnCuInS mid-shell as an intermediate layer is newly introduced between a Cu-doped InP core and a ZnS shell for LSC devices. As for the latter one (surface ligands), the ligand effect by 1-octanethiol and chloride ion are investigated for the device stability in QD‒LEDs and the printability of electro-hydrodynamic (EHD) jet printing system, in which this research explores the behavior of surface ligands, based on proton transfer mechanism on the QD surface.
Chapter 3 demonstrates the synthesis of strain-engineered highly emissive Cu:InP/Zn–Cu–In–S (ZCIS)/ZnS core/shell/shell heterostructure QDs via a one-pot approach. When this unconventional combination of a ZCIS/ZnS double shelling scheme is introduced to a series of Cu:InP cores with different sizes, the resulting Cu:InP/ZCIS/ZnS QDs with a tunable near-IR PL range of 694–850 nm yield the highest-ever PL QYs of 71.5–82.4%. These outcomes strongly point to the efficacy of the ZCIS interlayer, which makes the core/shell interfacial strain effectively alleviated, toward high emissivity. The presence of such an intermediate ZCIS layer is further examined by comparative size, structural, and compositional analyses. The end of this chapter briefly introduces the research related to the LSC devices, fabricated from Cu:InP/ZCIS/ZnS QDs, currently in progress.
Chapter 4 mainly deals with ligand effect in 1-octanethiol passivation of InP/ZnSe/ZnS QDs in terms of incomplete surface passivation during synthesis. This chapter demonstrates the lack of anionic carboxylate ligands on the surface of InP/ZnSe/ZnS quantum dots (QDs), where zinc carboxylate ligands can be converted to carboxylic acid or carboxylate ligands via proton transfer by 1-octanethiol. The as-synthesized QDs initially have an under-coordinated vacancy surface, which is passivated by solvent ligands such as ethanol and acetone. Upon exposure of 1-octanethiol to the QD surface, 1-octanthiol effectively induces the surface binding of anionic carboxylate ligands (derived from zinc carboxylate ligands) by proton transfer, which consequently exchanges ethanol and acetone ligands that bound on the incomplete QD surface. The systematic chemical analyses, such as thermogravimetric analysis‒mass spectrometry and proton nuclear magnetic resonance spectroscopy, directly show the interplay of surface ligands, and it associates with QD light-emitting diodes (QD‒LEDs).
Chapter 5 shows the relation between material stability of QDs and device stability of QD‒LEDs through the investigation of surface chemistry and shell thickness. In typical III–V colloidal InP quantum dots (QDs), an inorganic ZnS outermost shell is used to provide stability when overcoated onto the InP core. However, this work presents a faster photo-degradation of InP/ZnSe/ZnS QDs with a thicker ZnS shell than that with a thin ZnS shell when 1-octanethiol was applied as a sulfur source to form ZnS outmost shell. Herein, 1-octanethiol induces the form of weakly-bound carboxylate ligand via proton transfer on the QD surface, resulting in a faster degradation at UV light even though a thicker ZnS shell was formed onto InP/ZnSe QDs. Detailed insight into surface chemistry was obtained from proton nuclear magnetic resonance spectroscopy and thermogravimetric analysis–mass spectrometry. However, the lifetimes of the electroluminescence devices fabricated from InP/ZnSe/ZnS QDs with a thick or a thin ZnS shell show surprisingly the opposite result to the material stability of QDs, where the QD light-emitting diodes (QD‒LEDs) with a thick ZnS shelled QDs maintained its luminance more stable than that with a thin ZnS shelled QDs. This study elucidates the degradation mechanism of the QDs and the QD light-emitting diodes based on the results and discuss why the material stability of QDs is different from the lifetime of QD‒LEDs.
Chapter 6 suggests a method how to improve a printability of EHD jet printing when QD materials are applied to QD ink formulation, where this work introduces the application of GaP mid-shelled InP QDs as a role of surface charge in EHD jet printing technique. In general, GaP intermediate shell has been introduced in III–V colloidal InP quantum dots (QDs) to enhance their thermal stability and quantum efficiency in the case of type-I core/shell/shell heterostructure InP/GaP/ZnSeS QDs. Herein, these highly luminescent InP/GaP/ZnSeS QDs were synthesized and applied to EHD jet printing, by which this study demonstrates that unreacted Ga and Cl ions on the QD surface induce the operating voltage of cone jet and cone jet formation to be reduced and stabilized, respectively. This result indicates GaP intermediate shell not only improves PL QY and thermal stability of InP QDs but also adjusts the critical flow rate required for cone-jet formation. In other words, surface charges of quantum dots can have a significant role in forming cone apex in the EHD capillary nozzle. For an industrially convenient validation of surface charges on the QD surface, Zeta potential analyses of QD solutions as a simple method were performed, as well as inductively coupled plasma optical emission spectrometry (ICP-OES) for a composition of elements.
Beyond the generation of highly emissive InP QDs with narrow FWHM, these studies talk about the connection between QD material and QD devices not only to make it a vital jumping-off point for industrially feasible applications but also to reveal from chemical and physical standpoints the origin that obstructs the improvement of device performance experimentally and theoretically.
Facing the environmental crisis, new technologies are needed to sustain our society. In this context, this thesis aims to describe the properties and applications of carbon-based sustainable materials. In particular, it reports the synthesis and characterization of a wide set of porous carbonaceous materials with high nitrogen content obtained from nucleobases. These materials are used as cathodes for Li-ion capacitors, and a major focus is put on the cathode preparation, highlighting the oxidation resistance of nucleobase-derived materials. Furthermore, their catalytic properties for acid/base and redox reactions are described, pointing to the role of nitrogen speciation on their surfaces. Finally, these materials are used as supports for highly dispersed nickel loading, activating the materials for carbon dioxide electroreduction.
Functional materials, also called "Smart Materials", are described by their ability to fulfill a desired task through targeted interaction with its environment. Due to this functional integration, such materials are of increased interest, especially in areas where the increasing micronization of components is required. Modern manufacturing processes (e.g. microfluidics) and the availability of a wide variety of functional materials (e.g. shape memory materials) now enable the production of particle-based switching components. This category includes micropumps and microvalves, whose basic function is the active control of liquid flows. One approach in realizing those microcomponents as pursued by this work, enables variable size-switching of water-filled microballoons by implementing a stimulus-sensitive switching motif in the capsule's membrane shell, while being under the influence of a constant driving force. The switching motif with its gatekeeper function has a critical influence on one or more material parameters, which modulate the capsule's resistance against the driving force in microballoon expansion process. The advantage of this concept is that even non-variable analyte conditions, such as concentration levels of ions, can be capitalized to generate external force fields that, under the control of the membrane, cause an inflation of the microballoon by an osmotically driven water influx. In case of osmotic pressure gradients as the driving force for the capsule expansion, material parameters associated with the gatekeeper function are specifically the permeability and the mechanical stiffness of the shell material. While a modulation of the shell permeability could be utilized to kinetically impede the water influx on large time scales, a modulation of the shell's mechanical stiffness even might be utilized to completely prevent the capsule inflation due to a possible non-deformability beneath a certain threshold pressure. In polymer networks, which are a suitable material class for the demanded capsule shell because of their excellent elasticity, both the permeability and the mechanical properties are strongly influenced by the crystallinity of the material. Since the permeability is effectively reduced with increasing crystallinity, while the mechanical stiffness is simultaneously greatly increased, both effects point in the same direction in terms of their functional relationship. For this reason and due to a reversible and contactless modulation of the membrane crystallinity by heat input, crystallites may be suitable switching motifs for controlling the capsule expansion. As second design element of reversible expandable microballoons, the capsule geometry, defined by an aqueous core enveloped by the temperature-sensitive polymer network membrane, should allow an osmotic pressure gradient across the membrane layer. The strength of the inflation pressure and the associated inflation velocity upon membrane melting should be controlled by the salt concentration within the aqueous core, while a turn in the osmotic gradient should furthermore allow the reversible process of capsule deflation. Therefore, it should be possible to build either microvalves and micropumps, while their intended action of either pumping or valving is determined by their state of expansion and the direction of the osmotic pressure gradient.. Microballoons of approximately 300 µm in diameter were formed via droplet-based microfluidics from double-emulsion templates (w/o/w). The elastomeric capsule membrane was formed by photo-crosslinking of methacrylate (MA) functionalized oligo(ε-caprolactone) precursors (≈ 3.8 MA-arms, Mn ≈ 12000 g mol-1) within the organic medium layer (o) via UV-exposure after droplet-formation. After removal of the toluene/chloroform mixture by slow extraction via the continuous aqueous phase, the capsules solidified under the development of a characteristic "mushroom"-like shape at specific experimental conditions (e.g. λ = 308 nm, 57 mJ·s-1·cm-2, 16 min). It could be furthermore shown that in dependency to the process parameters: oligomer concentration and curing-time also spherical capsules were accessible. Long curing-times and high oligomer concentrations at a fixed light-intensity favored the formation of "mushroom"-like capsules, whereas the contrary led to spherical shaped capsules. A comparative study on thin polymer network films of same composition and equal treatment proved a correlation between the film's crosslink density and their contraction capability, while stronger crosslinked polymer networks showed a stronger contraction after solvent removal. In combination with observations during capsule solidification via light-microscopy, where a continuous shaping from almost spherical crosslinked templates to "mushroom"-shaped and solidified capsules was stated, the following mechanism was proposed. In case of low oligomer contents and short curing-times, the contraction of the capsule shell during solvent removal is strongly diminished due to a low degree of crosslinking. Therefore, the solidifying shell could freely collapse onto the aqueous core. In the other case, high oligomer concentrations and long curing-times will favor the formation of highly crosslinked capsule membranes with a strong contraction capability. Due to an observed decentered location of the aqueous core within the swollen polymer network, an uneven radial stress along the capsule's circumference is exerted to the incompressible core. This lead to an uneven contraction during solvent removal and a directed flow of the core fluid into the direction of the minimal stress vector. In consequence, the initially thicker spherical cap contracts, whereas the opposing thinner spherical cap get stretched. The "mushroom"-shape over some advantages over their spherical shaped counterparts, why they were selected for the further experiments. Besides the necessity of a high density of crosslinking for the purpose of extraordinary elasticity and toughness, the form-anisotropy promotes a faster microballoon expandability due to a partial reduction of the membrane thickness. Additionally, pre-stretched regions of thin thickness might provide a better resistance against inflation pressure than spherical but non-stretched capsules of equal membrane thickness. The resulting "mushroom"-shaped microcapsules exhibited a melting point of Tm ≈ 50 - 60 °C and a degree of crystallinity of Xc ≈ 29 - 38 % depending on the membrane thickness and internal salt content, which is slightly lower than for the non-crosslinked oligomer and reasoned by a limited chain mobility upon crosslinking. Nonetheless, the melting transition of the polymer network was associated with a strong drop in its mechanical stiffness, which was shown to have a strong influence on the osmotic driven expansion of the microcapsules. Capsules that were subjected to osmotic pressures between 1.5 and 4.7 MPa did not expand if the temperature was well below the melting point of the capsule's membrane, i.e. at room temperature. In contrast, a continuous expansion, while approaching asymptotically to a final capsule size, was observed if the temperature exceeded the melting point, i.e. 60 °C. Microballoons, which were kept for 56 days at ∆Π = 1.5 MPa and room temperature, did not change significantly in diameter, why the impact of the mechanical stiffness on the expansion behavior is considered to be the greater than the influence of the shell permeability. The time-resolved expansion behavior of the microballoons above their Tm was subsequently modeled, using difusion equations that were corrected for shape anisotropy and elastic restoring forces. A shape-related and expansion dependent pre-factor was used to dynamically address the influence of the shell thickness differences along the circumference on the inflation velocity, whereas the microballoon's elastic contraction upon inflation was rendered by the inclusion of a hyperelastic constitutive model. An important finding resulting from this model was the pronounced increase in inflation velocity compared to hypothetical capsules with a homogeneous shell thickness, which stresses the benefit of employing shape anisotropic balloon-like capsules in this study. Furthermore, the model was able to predict the finite expandability on basis of entropy-elastic recovery forces and strain-hardening effects. A comparison of six different microballoons with different shell thicknesses and internal salt contents showed the linear relationship between the volumetric expansion, the shell thickness and the applied osmotic pressure, as represented by the model. As the proposed model facilitates the prediction of the expansion kinetics depending on the membranes mechanical and diffusional characteristics, it might be a screening tool for future material selections. In course of the microballoon expansion process, capsules of intermediate diameters could be isolated by recrystallization of the membrane, which is mainly caused by a restoration of the membrane's mechanical stiffness and is otherwise difficult to achieve with other stimuli-sensitive systems. The capsule's crystallinity of intermediate expansion states was nearly unchanged, whereas the lamellar crystal size tends to decreased with the expansion ratio. Therefore, it was assumed that the elastic modulus was only minimally altered and might increased due to the networks segment-chain extension. In addition to the volume increase achieved by inflation, a turn in the osmotic gradient also facilitated the reversible deflation, which was shown in inflation/deflation cycles. These both characteristics of the introduced microballoons are important parameter regarding the realization of micropumps and microvalves. The fixation of expanded microcapsules via recrystallization enabled the storage of entropy-elastic strain-energy, which could be utilized for pumping actions in non-aqueous media. Here, the pumping velocity depended on both, the type of surrounding medium and the applied temperature. Surrounding media that supported the fast transport of pumped liquid showed an accelerated deflation, while high temperatures further accelerate the pumping velocity. Very fast rejection of the incorporated payload was furthermore realized with pierced expanded microballoons, which were subjected to temperatures above their Tm. The possible fixation of intermediate particle sizes provide opportunities for vent constructions that allowed the precise adjustment of specific flow-rates and multiple valve openings and closings. A valve construction was realized by the insertion of a single or multiple microballoons in a microfluidic channel. A complete and a partial closing of the microballoon-valves was demonstrated as a function of the heating period. In this context, a difference between the inflation and deflation velocity was stated, summarizing slower expansion kinetics. Overall, microballoons, which presented both on-demand pumping and reversible valving by a temperature-triggered change in the capsule's volume, might be suitable components that help to design fully integrated LOC devices, due to the implementation of the control switch and controllable inflation/deflation kinetics. In comparison to other state of the art stimuli-sensitive materials, one has to highlight the microballoons capability of stabilizing almost continuously intermediate capsule sizes by simple recrystallization of the microballoon's membrane.
Eine reflexive Haltung gegenüber der eigenen Lehrtätigkeit gilt als Schlüsselqualifikation in Bezug auf die Professionalisierung von Lehrer:innen in allen Didaktiken (GFD, 2004, S. 4). Das universitäre Seminarformat Lehr-Lern-Labor (LLLS) kann diese Haltung fördern (Rehfeldt et al., 2018). Das Lehrformat eignet sich außerdem zur Steigerung des Professionswissens und der unterrichtlichen Handlungsfähigkeit angehender Lehrer:innen (Rehfeldt et al., 2020; Brämer & Köster, 2021). Dieser Beitrag stellt, neben der grundsätzlichen Konzeption des Seminarformats, dessen Implementierung in vier verschiedenen Fachdidaktiken (Didaktiken des Englischen, der Geschichte, der Physik und Sachunterricht und seine Didaktik) vor. Ein Fokus liegt dabei auf der unterschiedlichen Umsetzung der Reflexionsphasen.
Reflexion ist eine Schlüsselkategorie für die professionelle Entwicklung von Lehrkräften, welche als Ausbildungsziel in den Bildungsstandards für die Lehrkräftebildung verankert ist. Eine Verstetigung universitär geprägter Forschung und Modellierung in der praxisnahen Anwendung im schulischen Kontext bietet Potentiale nachhaltiger Professionalisierung. Die Stärkung reflexionsbezogener Kompetenzen durch Empirie und Anwendung scheint eine phasenübergreifende Herausforderung der Lehrkräftebildung zu sein, die es zu bewältigen gilt. Ziele des Tagungsbandes Reflexion in der Lehrkräftebildung sind eine theoretische Schärfung des Konzeptes „Reflexive Professionalisierung“ und der Austausch über Fragen der Einbettung wirksamer reflexionsbezogener Lerngelegenheiten in die Lehrkräftebildung. Forschende und Lehrende der‚ drei Phasen (Studium, Referendariat sowie Fort- und Weiterbildung) der Lehrkräftebildung stellen Lehrkonzepte und Forschungsprojekte zum Thema Reflexion in der Lehrkräftebildung vor und diskutieren diese. Gemeinsam mit Teilnehmenden aller Phasen und von verschiedenen Standorten der Lehrkräftebildung werden zukünftige Herausforderungen identifiziert und Lösungsansätze herausgearbeitet.
In diesem Beitrag wird ein geplantes digitales Lehrkonzept für die universitäre Begleitung des Praxissemesters in den Fächern Biologie und Mathematik vorgestellt. Darin setzen sich Studierende im Praxissemester selbstständig fachspezifische Schwerpunkte für die Planung, Durchführung und Reflexion von Unterrichtsprojekten in der Schule. Optimalerweise ergibt sich aus den Unterrichtsprojekten auch eine fachbezogene Fragestellung, die von den Studierenden im Zuge Forschenden Lernens ergründet werden kann. Begleitet wird der gesamte Prozess durch systematisch angeleitete E-Peer-Assessments (E-PA). Dabei treten Studierende in Peers in den digitalen, schriftlichen Dialog über Unterricht und durchlaufen gemeinsam Reflexions- und Feedbackschleifen, welche durch die universitäre Seminarleitung instruiert werden.
Reflexion wird in diesem Artikel als Rückmeldung (Feedback) zu einem Sprachlernstand begriffen. Es soll anhand eines Fallbeispiels (IRF-Sequenz) aus dem Unterricht Deutsch als Zweitsprache (DaZ) der Frage nachgegangen werden, wie sich die Feedback-Interaktion gestaltet und inwiefern sich ihr Gelingen oder Misslingen erklären lässt. Dazu wird die evidenzbasierte Forschung zum effektiven Feedback nach Hattie (u. a. Hattie 2020; Hattie & Zierer 2020; Wisniewski & Zierer 2018) in die Analyse einbezogen. Zu wissen, welche Wirkung Feedbacks erzielen, hilft (angehenden) Lehrer:innen, das eigene Handeln zu reflektieren.
Die Professionalisierung angehender Lehrer:innen für Fragen rund um sprachliche Bildung, Deutsch als Zweitsprache und Mehrsprachigkeit ist in den letzten Jahren verstärkt in den Blick der Praxis und Forschung der Lehrer:innenbildung gerückt. Während der Fachdiskurs im Hinblick auf die Konstrukte (Handlungs-)Kompetenz und Einstellungen bereits vorgeschritten ist, stellen die Modellierung und Erforschung des Konstrukts Reflexion im Fach Deutsch als Fremd- und Zweitsprache (DaF*Z) noch ein Desiderat dar. Im Beitrag wird die Fachspezifik der Reflexion als eines der Qualifizierungsziele der Ausbildung von Lehrer:innen für die sprachlich und kulturell heterogene Schülerschaft diskutiert und eine Modellierung vorgestellt.
Reflexion im Dialog
(2023)
Fast 40 Jahre nach dem Erscheinen von Donald Schöns Buch „The Reflective Practitioner: How Professionals Think In Action“ (1984) ist das Konzept der „reflexiven Kompetenz“ immer noch hochaktuell und wird daher in akademischen Kreisen weiterhin intensiv diskutiert. Der Artikel greift die Diskussionen zu diesem Thema im Bereich der Fremdsprachenlehrkräftebildung auf und unterstreicht sie mit Beispielen aus der universitären Aus- und Fortbildungspraxis für Deutsch als Fremd- und Zweitsprache in Brasilien und Deutschland. Auffällig ist dabei, dass es sowohl bei den Fragestellungen als auch bei den Maßnahmen und Instrumenten zahlreiche Überschneidungen gibt. Reflexion als Ziel in der Lehrkräftebildung kann somit als übergreifendes Thema wahrgenommen und weiterentwickelt werden.
Auf der Zeitachse von Zyklusmodellen des Unterrichts wird der Handlungsreflexion eine zentrale Bedeutung zugesprochen: Vor seiner Umsetzung im Unterricht soll das kommende Handeln zunächst in einer antizipierenden Reflexion gedanklich entworfen werden, um seine Erfolgswahrscheinlichkeit zu erhöhen. Nach dem Unterricht soll es einer retrospektiven Reflexion unterzogen werden, in der die Handlungsumsetzung vor dem Hintergrund der Handlungsplanung evaluiert wird und Konsequenzen für künftige Handlungsplanungen gezogen werden. Trotz der Plausibilität dieses postulierten Zusammenhangs von antizipierender und retrospektiver Reflexion steht seine genauere empirische Untersuchung allerdings noch aus. In einer querschnittlichen Onlineerhebung werden diese beiden Reflexionsformen deshalb als generische Unterrichtsplanungsfähigkeit und Reflexionskompetenz spezifiziert, um ihren Zusammenhang mit Hilfe einer Stichprobe von angehenden Lehrkräften (N = 479) aus zwei Universitäten zu explorieren. Die gefundenen schwachen Zusammenhänge werden vor dem Hintergrund der Operationalisierungen und der Testmotivation der Teilnehmenden diskutiert.