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831.
Hahn KR Tricoli A Santarossa G Vargas A Baiker A 《Langmuir : the ACS journal of surfaces and colloids》2012,28(2):1646-1656
Both associative and dissociative H(2)O adsorption on SnO(2)(110), TiO(2)(110), and Ti-enriched Sn(1-x)Ti(x)O(2)(110) surfaces have been investigated at low ((1)/(12) monolayer (ML)) and high coverage (1 ML) by density functional theory calculations using the Gaussian and plane waves formalism. The use of a large supercell allowed the simulation at low symmetry levels. On SnO(2)(110), dissociative adsorption was favored at all coverages and was accompanied by stable associative H(2)O configurations. Increasing the coverage from (1)/(12) to 1 ML stabilized the (associatively or dissociatively) adsorbed H(2)O on SnO(2)(110) because of the formation of intermolecular H bonds. In contrast, on TiO(2)(110), the adsorption of isolated H(2)O groups ((1)/(12) ML) was more stable than at high coverage, and the favored adsorption changed from dissociative to associative with increasing coverage. For dissociative H(2)O adsorption on Ti-enriched Sn(1-x)Ti(x)O(2)(110) surfaces with Ti atoms preferably located on 6-fold-coordinated surface sites, the analysis of the Wannier centers showed a polarization of electrons surrounding bridging O atoms that were bound simultaneously to 6-fold-coordinated Sn and Ti surface atoms. This polarization suggested the formation of an additional bond between the 6-fold-coordinated Ti(6c) and bridging O atoms that had to be broken upon H(2)O adsorption. As a result, the H(2)O adsorption energy initially decreased, with increasing surface Ti content reaching a minimum at 25% Ti for (1)/(12) ML. This behavior was even more accentuated at high H(2)O coverage (1 ML) with the adsorption energy decreasing rapidly from 145.2 to 101.6 kJ/mol with the surface Ti content increasing from 0 to 33%. A global minimum of binding energies at both low and high coverage was found between 25 and 33% surface Ti content, which may explain the minimal cross-sensitivity to humidity previously reported for Sn(1-x)Ti(x)O(2) gas sensors. Above 12.5% surface Ti content, the binding energy decreased with increasing coverage, suggesting that the partial desorption of H(2)O is facilitated at a high fractional coverage. 相似文献
832.
Felix Schmidt-Stein Jan-Frederik Gnichwitz Jarno Salonen Robert Hahn Andreas Hirsch Patrik Schmuki 《Electrochemistry communications》2009,11(10):2000-2003
This work reports on an electrochemical system which allows the control of surface wettability properties by voltage induced changes in contact angle (Θ) of ΔΘ 50°. For this we used conductive TiO2 nanotubular layers that were modified with ferrocene coupled to the TiO2 surface via triethoxysilane. To enhance the hydrophobic character of the nanotubular TiO2 surface, also mixed organic monolayers namely perfluorotriethoxysilane, were explored. Formation of the ferrocene and mixed organic monolayer was confirmed by X-ray-photoelectron-spectroscopy (XPS). Contact angle combined with electrochemical measurements show that ferrocene in these monolayers can successfully be switched from Fe2+ to Fe3+ and that this change in the redox state considerably alters the wetting properties. Using a conductive nanotube substrate allows us to amplify this change by a factor of more than 10, and thus this surface can be used to trigger significant wetting alterations. 相似文献
833.
Laubsch A. Sabathil M. Baur J. Peter M. Hahn B. 《Electron Devices, IEEE Transactions on》2010,57(1):79-87
In this paper, we report on the latest advancements in improving AlGaInN-based visible-light-emitting-diode (LED) efficiency in epitaxy, chip, and package designs. We investigate the fundamental origin of the typical high current ?droop? of efficiency observed in such LEDs. We show that this effect is most likely not caused by incomplete carrier injection or carrier escape but that it is rather a fundamental material property of InGaN/GaN-heterostructure-based light emitters. The droop can be reduced in improved epitaxial LED active-layer designs. We show how this can be achieved by lowering InGaN volume carrier density in multiple quantum wells (MQWs) and thick InGaN layers. Improved epitaxial MQW structures are then combined with a new advanced chip concept. It is optimized for high efficiency at high current operation and arbitrary scalability and can be manufactured at low cost. This is accomplished by improving light-extraction efficiency, homogenizing the emission pattern, reducing forward voltage, and lowering thermal resistance. The improved high current efficiency can be fully exploited by mounting the chip in the highly versatile new OSLON SSL package. It features very stable package materials, a small footprint, and an electrically isolated design decoupling electrical and thermal contacts. 相似文献
834.
Elisabeth Schmoeger Martin Wellhoefer Astrid Dürauer Alois Jungbauer Rainer Hahn 《Journal of chromatography. A》2010,1217(38):5950-5956
Matrix-assisted refolding is an excellent technique for performing refolding of recombinant proteins at high concentration because aggregation during refolding is partially suppressed. The autoprotease Npro and its engineered mutant EDDIE can be efficiently refolded on cation-exchangers. In the current work, denatured fusion proteins were loaded at different column saturations (5 and 50 mg mL−1 gel), and refolding and self-cleavage were initiated during elution. The contact time of the protein with the matrix significantly influenced the refolding rate and yield. On POROS 50 HS, the refolding rate was comparable to a batch refolding process, but yield was substantially higher; at a protein concentration of 1.55 mg mL−1, an almost complete conversion was observed. With Capto S, the rate of self-cleavage increased by a factor of 20 while yield was slightly reduced. Processing the autoprotease fusion protein on Capto S at a high protein loading of 50 mg mL−1 gel and short contact time (0.5 h) yielded the highest productivity. 相似文献
835.
Seungsoo Hahn Orr Ashenberg Gevorg Grigoryan Amy E. Keating 《Journal of computational chemistry》2010,31(16):2900-2914
Protein design involves searching a vast space for sequences that are compatible with a defined structure. This can pose significant computational challenges. Cluster expansion is a technique that can accelerate the evaluation of protein energies by generating a simple functional relationship between sequence and energy. The method consists of several steps. First, for a given protein structure, a training set of sequences with known energies is generated. Next, this training set is used to expand energy as a function of clusters consisting of single residues, residue pairs, and higher order terms, if required. The accuracy of the sequence‐based expansion is monitored and improved using cross‐validation testing and iterative inclusion of additional clusters. As a trade‐off for evaluation speed, the cluster‐expansion approximation causes prediction errors, which can be reduced by including more training sequences, including higher order terms in the expansion, and/or reducing the sequence space described by thecluster expansion. This article analyzes the sources of error and introduces a method whereby accuracy can be improved by judiciously reducing the described sequence space. The method is applied to describe the sequence–stability relationship for several protein structures: coiled‐coil dimers and trimers, a PDZ domain, and T4 lysozyme as examples with computationally derived energies, and SH3 domains in amphiphysin‐1 and endophilin‐1 as examples where the expanded pseudo‐energies are obtained from experiments. Our open‐source software package Cluster Expansion Version 1.0 allows users to expand their own energy function of interest and thereby apply cluster expansion to custom problems in protein design. © 2010 Wiley Periodicals, Inc. J Comput Chem, 2010 相似文献
836.
Because of uncertainties in material and geometrical parameters in ultrasonic devices, experimental characterization is an indispensable part in their successful application for the manipulation of particles or cells. Its miniaturized size precludes the use of many of the usual tools used for macroscopic systems. Also, a further challenge is the fact that the resulting motion due to the electromechanical actuation has both high frequency and small amplitudes. Contactless methods like laser interferometry are therefore promising methods. In addition, as long as there is strong electromechanical coupling between the transducer and the device also electrical measurements like admittance curves give insight into the frequencies at which the devices might work best. This is the case for example for piezoelectric transducers working at one of their resonance frequencies. Because the devices usually are used in resonant modes, narrow frequency detection methods like lock in amplifiers help to improve the signal to noise ratio. Also many analysis tools have been established in the context of modal analysis, which is based on frequency domain methods. Special emphasis is placed here on the determination of the quality factor Q of the resonator, as Q determines the efficiency of a device. 相似文献
837.
Microfluidics with aqueous two-phase systems 总被引:1,自引:0,他引:1
An overview is given about research activities in which aqueous two phase systems (ATPSs) are utilized in microfluidic setups. ATPSs consist of two immiscible aqueous phases and have traditionally been used for the separation and purification of biological material such as proteins or cells. Microfluidic implementations of such schemes are usually based on a number of co-flowing streams of immiscible phases in a microchannel, thereby replacing the standard batch by flow-through processes. Some aspects of the stability of such flow patterns and the recovery of the phases at the channel exit are reviewed. Furthermore, the diffusive mass transfer and sample partitioning between the phases are discussed, and corresponding applications are highlighted. When diffusion is superposed by an applied electric field normal to the liquid/liquid interface, the transport processes are accelerated, and under specific conditions the interface acts as a size-selective filter for molecules. Finally, the activities involving droplet microflows of ATPSs are reviewed. By either forming ATPS droplets in an organic phase or a droplet of one aqueous phase inside the other, a range of applications has been demonstrated, extending from separation/purification schemes to the patterning of surfaces covered with cells. 相似文献
838.
839.
Sebastian Förster Torsten Hahn Claudia Loose Christian Röder Simon Liebing Wilhelm Seichter Frank Eißmann Jens Kortus Edwin Weber 《Journal of Physical Organic Chemistry》2012,25(10):856-863
Four new azulene derivatives featuring two π‐conjugated and sulfur terminated rigid side arms in the 1,3‐positions of the azulene core were designed, synthesized, and characterized. The syntheses were carried out on the basis of a palladium cross‐coupling procedure in the key reaction step. The crystal structures of the target compound 3 and of the intermediate compounds 7 and 9 have been studied. Supporting density functional theory calculations reveal insights into the electronic properties of the particular azulenes. The comparison of measured UV–Vis, infrared, and Raman data to calculated values allowed assignment of major spectral features to the particular structural differences of the new compounds and comparison to plain azulene. Cyclic voltammetry measurements were performed showing the redox characteristics of the new azulene derivatives. Copyright © 2012 John Wiley & Sons, Ltd. 相似文献
840.