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This research addressed the question, if it is possible to simplify current microcontact printing systems for the production of anisotropic building blocks or patchy particles, by using common chemicals while still maintaining reproducibility, high precision and tunability of the Janus-balance
Chapter 2 introduced the microcontact printing materials as well as their defined electrostatic interactions. In particular polydimethylsiloxane stamps, silica particles and high molecular weight polyethylenimine ink were mainly used in this research. All of these components are commercially available in large quantities and affordable, which gives this approach a huge potential for further up-scaling developments. The benefits of polymeric over molecular inks was described including its flexible influence on the printing pressure. With this alteration of the µCP concept, a new method of solvent assisted particle release mechanism enabled the switch from two-dimensional surface modification to three-dimensional structure printing on colloidal silica particles, without changing printing parameters or starting materials. This effect opened the way to use the internal volume of the achieved patches for incorporation of nano additives, introducing additional physical properties into the patches without alteration of the surface chemistry.
The success of this system and its achievable range was further investigated in chapter 3 by giving detailed information about patch geometry parameters including diameter, thickness and yield. For this purpose, silica particles in a size range between 1µm and 5µm were printed with different ink concentrations to change the Janus-balance of these single patched particles. A necessary intermediate step, consisting of air-plasma treatment, for the production of trivalent particles using "sandwich" printing was discovered and comparative studies concerning the patch geometry of single and double patched particles were conducted. Additionally, the usage of structured PDMS stamps during printing was described. These results demonstrate the excellent precision of this approach and opens the pathway for even greater accuracy as further parameters can be finely tuned and investigated, e.g. humidity and temperature during stamp loading.
The performance of these synthesized anisotropic colloids was further investigated in chapter 4, starting with behaviour studies in alcoholic and aqueous dispersions. Here, the stability of the applied patches was studied in a broad pH range, discovering a release mechanism by disabling the electrostatic bonding between particle surface and polyelectrolyte ink. Furthermore, the absence of strong attractive forces between divalent particles in water was investigated using XPS measurements. These results lead to the conclusion that the transfer of small PDMS oligomers onto the patch surface is shielding charges, preventing colloidal agglomeration. However, based on this knowledge, further patch modifications for particle self-assembly were introduced including physical approaches using magnetic nano additives, chemical patch functionalization with avidin-biotin or the light responsive cyclodextrin-arylazopyrazoles coupling as well as particle surface modification for the synthesis of highly amphiphilic colloids. The successful coupling, its efficiency, stability and behaviour in different solvents were evaluated to find a suitable coupling system for future assembly experiments. Based on these results the possibility of more sophisticated structures by colloidal self-assembly is given.
Certain findings needed further analysis to understand their underlying mechanics, including the relatively broad patch diameter distribution and the decreasing patch thickness for smaller silica particles. Mathematical assumptions for both effects are introduced in chapter 5. First, they demonstrate the connection between the naturally occurring particle size distribution and the broadening of the patch diameter, indicating an even higher precision for this µCP approach. Second, explaining the increase of contact area between particle and ink surface due to higher particle packaging, leading to a decrease in printing pressure for smaller particles.
These calculations ultimately lead to the development of a new mechanical microcontact printing approach, using centrifugal forces for high pressure control and excellent parallel alignment of printing substrates. First results with this device and the comparison with previously conducted by-hand experiments conclude this research. It furthermore displays the advantages of such a device for future applications using a mechanical printing approach, especially for accessing even smaller nano particles with great precision and excellent yield.
In conclusion, this work demonstrates the successful adjustment of the µCP approach using commercially available and affordable silica particles and polyelectrolytes for high flexibility, reduced costs and higher scale-up value. Furthermore, its was possible to increase the modification potential by introducing three-dimensional patches for additional functionalization volume. While keeping a high colloidal stability, different coupling systems showed the self-assembly capabilities of this toolbox for anisotropic particles.
Draft Art. 15 CCAH attempts to strike a balance between State autonomy and robust judicial supervision. It largely follows Article 22 CERD conditioning the jurisdiction of the ICJ on prior negotiations. Hence, the substance of the clause is interpreted in light of the Court’s recent case law, especially Georgia v. Russia. Besides, several issues regarding the scope ratione temporis of the compromissory clause are discussed. The article advances several proposals to further improve the current draft, addressing the missing explicit reference to State responsibility, as well as the relationship between the Court and a possible treaty body, It also proposes to recalibrate the interplay of a requirement of prior negotiations respectively the seizing of a future treaty body on the one hand and provisional measures to be indicated by the Court on the other.
A doppelalgebra is an algebra defined on a vector space with two binary linear associative operations. Doppelalgebras play a prominent role in algebraic K-theory. We consider doppelsemigroups, that is, sets with two binary associative operations satisfying the axioms of a doppelalgebra. Doppelsemigroups are a generalization of semigroups and they have relationships with such algebraic structures as interassociative semigroups, restrictive bisemigroups, dimonoids, and trioids.
In the lecture notes numerous examples of doppelsemigroups and of strong doppelsemigroups are given. The independence of axioms of a strong doppelsemigroup is established. A free product in the variety of doppelsemigroups is presented. We also construct a free (strong) doppelsemigroup, a free commutative (strong) doppelsemigroup, a free n-nilpotent (strong) doppelsemigroup, a free n-dinilpotent (strong) doppelsemigroup, and a free left n-dinilpotent doppelsemigroup. Moreover, the least commutative congruence, the least n-nilpotent congruence, the least n-dinilpotent congruence on a free (strong) doppelsemigroup and the least left n-dinilpotent congruence on a free doppelsemigroup are characterized.
The book addresses graduate students, post-graduate students, researchers in algebra and interested readers.
Cell-free protein synthesis as a novel tool for directed glycoengineering of active erythropoietin
(2018)
As one of the most complex post-translational modification, glycosylation is widely involved in cell adhesion, cell proliferation and immune response. Nevertheless glycoproteins with an identical polypeptide backbone mostly differ in their glycosylation patterns. Due to this heterogeneity, the mapping of different glycosylation patterns to their associated function is nearly impossible. In the last years, glycoengineering tools including cell line engineering, chemoenzymatic remodeling and site-specific glycosylation have attracted increasing interest. The therapeutic hormone erythropoietin (EPO) has been investigated in particular by various groups to establish a production process resulting in a defined glycosylation pattern. However commercially available recombinant human EPO shows batch-to-batch variations in its glycoforms. Therefore we present an alternative method for the synthesis of active glycosylated EPO with an engineered O-glycosylation site by combining eukaryotic cell-free protein synthesis and site-directed incorporation of non-canonical amino acids with subsequent chemoselective modifications.
Background: Individuals with aphasia after stroke (IWA) often present with working memory (WM) deficits. Research investigating the relationship between WM and language abilities has led to the promising hypothesis that treatments of WM could lead to improvements in language, a phenomenon known as transfer. Although recent treatment protocols have been successful in improving WM, the evidence to date is scarce and the extent to which improvements in trained tasks of WM transfer to untrained memory tasks, spoken sentence comprehension, and functional communication is yet poorly understood.
Aims: We aimed at (a) investigating whether WM can be improved through an adaptive n-back training in IWA (Study 1–3); (b) testing whether WM training leads to near transfer to unpracticed WM tasks (Study 1–3), and far transfer to spoken sentence comprehension (Study 1–3), functional communication (Study 2–3), and memory in daily life in IWA (Study 2–3); and (c) evaluating the methodological quality of existing WM treatments in IWA (Study 3). To address these goals, we conducted two empirical studies – a case-controls study with Hungarian speaking IWA (Study 1) and a multiple baseline study with German speaking IWA (Study 2) – and a systematic review (Study 3).
Methods: In Study 1 and 2 participants with chronic, post-stroke aphasia performed an adaptive, computerized n-back training. ‘Adaptivity’ was implemented by adjusting the tasks’ difficulty level according to the participants’ performance, ensuring that they always practiced at an optimal level of difficulty. To assess the specificity of transfer effects and to better understand the underlying mechanisms of transfer on spoken sentence comprehension, we included an outcome measure testing specific syntactic structures that have been proposed to involve WM processes (e.g., non-canonical structures with varying complexity).
Results: We detected a mixed pattern of training and transfer effects across individuals: five participants out of six significantly improved in the n-back training. Our most important finding is that all six participants improved significantly in spoken sentence comprehension (i.e., far transfer effects). In addition, we also found far transfer to functional communication (in two participants out of three in Study 2) and everyday memory functioning (in all three participants in Study 2), and near transfer to unpracticed n-back tasks (in four participants out of six). Pooled data analysis of Study 1 and 2 showed a significant negative relationship between initial spoken sentence comprehension and the amount of improvement in this ability, suggesting that the more severe the participants’ spoken sentence comprehension deficit was at the beginning of training, the more they improved after training. Taken together, we detected both near far and transfer effects in our studies, but the effects varied across participants. The systematic review evaluating the methodological quality of existing WM treatments in stroke IWA (Study 3) showed poor internal and external validity across the included 17 studies. Poor internal validity was mainly due to use of inappropriate design, lack of randomization of study phases, lack of blinding of participants and/or assessors, and insufficient sampling. Low external validity was mainly related to incomplete information on the setting, lack of use of appropriate analysis or justification for the suitability of the analysis procedure used, and lack of replication across participants and/or behaviors. Results in terms of WM, spoken sentence comprehension, and reading are promising, but further studies with more rigorous methodology and stronger experimental control are needed to determine the beneficial effects of WM intervention.
Conclusions: Results of the empirical studies suggest that WM can be improved with a computerized and adaptive WM training, and improvements can lead to transfer effects to spoken sentence comprehension and functional communication in some individuals with chronic post-stroke aphasia. The fact that improvements were not specific to certain syntactic structures (i.e., non-canonical complex sentences) in spoken sentence comprehension suggest that WM is not involved in the online, automatic processing of syntactic information (i.e., parsing and interpretation), but plays a more general role in the later stage of spoken sentence comprehension (i.e., post-interpretive comprehension). The individual differences in treatment outcomes call for future research to clarify how far these results are generalizable to the population level of IWA. Future studies are needed to identify a few mechanisms that may generalize to at least a subpopulation of IWA as well as to investigate baseline non-linguistic cognitive and language abilities that may play a role in transfer effects and the maintenance of such effects. These may require larger yet homogenous samples.