Real-time single-molecule imaging of oxidation catalysis at a liquid-solid interface

Many chemical reactions are catalysed by metal complexes, and insight into their mechanisms is essential for the design of future catalysts. A variety of conventional spectroscopic techniques are available for the study of reaction mechanisms at the ensemble level, and, only recently, fluorescence microscopy techniques have been applied to monitor single chemical reactions carried out on crystal faces and by enzymes. With scanning tunnelling microscopy (STM) it has become possible to obtain, during chemical reactions, spatial information at the atomic level. The majority of these STM studies have been carried out under ultrahigh vacuum, far removed from conditions encountered in laboratory processes. Here we report the single-molecule imaging of oxidation catalysis by monitoring, with STM, individual manganese porphyrin catalysts, in real time, at a liquid-solid interface. It is found that the oxygen atoms from an O2 molecule are bound to adjacent porphyrin catalysts on the surface before their incorporation into an alkene substrate.     

On the classification of prostate carcinoma with methods from spatial statistics.

Gleason grading is a common method used by pathologists to determine the aggressivity of prostate cancer on the basis of histological slide preparations. The advantage of this grading system is a good correlation with the biological behavior of the tumor, while its drawback is the subjectivity underlying the judgements of pathologists. Therefore, an automation of Gleason grading would be desirable. In this paper, we examined 780 digitized grayscale images of 78 different cases, which were split into a training and a test set. We developed two methods based on combinations of morphological characteristics like area fraction, line length, and Euler number to classify into the categories "Gleason score < 7" and "Gleason score > or = 7." In particular, the distinction between these two classes has great impact on the prognosis of patients. The agreement of each method with visual diagnosis was 87.18% and 92.31% within the training set and 66.67% and 64.10% within the test set, respectively.     

IR-MALDI-MS analysis of HPTLC-separated phospholipid mixtures directly from the TLC plate

The application of a recently developed direct coupling of high-performance thin-layer chromatography (HPTLC) and infrared matrix-assisted laser desorption/ionization orthogonal extracting time-of-flight mass spectrometry (Dreisewerd, K.; Müthing, J.; Rohlfing, A.; Meisen, I.; Vukelic, Z.; Peter-Katalinic, J.; Hillenkamp, F.; Berkenkamp, S. Anal. Chem. 2005, 77, 4098-4107) to the analysis of phospholipid mixtures is demonstrated. Mixtures of six phospholipid types were exemplarily analyzed. The sensitivity was found to be in the range between about 10 and 150 pmol of material spotted for HPTLC, depending on phospholipid acidity, Rf value, and ion polarity. The lateral resolution of the analysis is on the order of the laser focus diameter of about 220 x 300 microm2, allowing differentiation between phospholipid species of different acyl chain composition within one single HPTLC band, which were undistiguishable by a mere visual assessment. Analyte diffusion due to the addition of glycerol to the HPTLC plate was found to be-if at all notable-of only minor importance.     

STOCHASTIC FINITE-ELEMENT ANALYSIS OF COUPLED HEAT AND MASS TRANSFER PROBLEMS WITH RANDOM FIELD PARAMETERS

A first-order perturbation algorithm for the computation of mean values and variances of transient temperature and moisture fields during coupled heat and mass transfer problems with random field parameters has been developed and implemented. The algorithm is based on the Galerkin finite-element discretization of Luikov's heat and mass transfer equations for capillary porous bodies and is computationally less demanding than the Monte Carlo method. The algorithm has been programmed in MATLAB and applied to a published test case of a drying process for soybean kernels. The simulations indicate that the stochastic fluctuations of the thermophysical properties and the process conditions may cause a considerable level of uncertainty in the predicted temperatures and moisture contents inside the product.     

Application of Thermodynamic and Kinetic Model for Converter Steelmaking to Optimize Manganese Yield in Crude Steel

A thermodynamic and kinetic model of the converter steelmaking process was developed allowing the analysis of the influence of the technological parameters, such as the amount and addition time of a charge material on the chemical composition of the crude steel. The process of the manganese ore addition to the converter to increase the final content of manganese in the crude steel was simulated. The optimal technological parameters for the enhancement of manganese yield were determined.     

Deriving control parameter settings from process models to control capsule fillers integrated into continuous manufacturing

The aim of this work was to investigate the mean fill weight control of a continuous capsule-filling process, whether it is possible to derive controller settings from an appendant process model. To that end, a system composed out of fully automated capsule filler and an online gravimetric scale was used to control the filled weight. This setup allows to examine challenges associated with continuous manufacturing processes, such as variations in the amount of active pharmaceutical ingredient (API) in the mixture due to fluctuations of the feeders or due to altered excipient batch qualities. Two types of controllers were investigated: a feedback control and a combination of feedback and feedforward control. Although both of those are common in the industry, determining the optimal parameter settings remains an issue. In this study, we developed a method to derive the control parameters based on process models in order to obtain optimal control for each filled product. Determined via rapid automated process development (RAPD), this method is an effective and fast way of determining control parameters. The method allowed us to optimize the weight control for three pharmaceutical excipients. By conducting experiments, we verified the feasibility of the proposed method and studied the dynamics of the controlled system. Our work provides important basic data on how capsule filler can be implemented into continuous manufacturing systems.     

Eine Formel verändert die Welt

The capacity formula for the Additive White Gaussian Noise (AWGN-) channel is taken for an example to demonstrate the extreme importance of Information Theory of C.E. Shannon for the transition from the Industrial Age to the Information Age. Exemplarily, typical ways of finding basic theorems in Information Theory are shown by means of two mathematical concepts. Simple relationships between information and energy as well as fundamental existence/nonexistence bounds for analogous and digital communication schemes are derived from the capacity formula. General comments on the importance of fundamental theories for the progress in technologies and on the rule of humanities in this process conclude the paper.     

Enhanced expoxidation activity of Ti-mesoporous catalysts containing organic–inorganic porewall

Surfactant templated Ti-containing organic–organic mesoporous catalysts which were synthesized from one step co-condensation of the precursors, showed enhanced liquid phase cyclohexene epoxidation activity and greater deactivation resistance than the parent Ti-MCM-41, with tert-butyl hydroperoxide as oxidant. The order of reactivity observed was Ti-MCM-41-phenylene > Ti-MCM-41-biphenylene > Ti-MCM-41-ethylene > Ti-MCM-41. In the presence of water, the Ti-MCM-41-phenylene catalyst showed up to 3.5-fold enhancement in activity over Ti-MCM-41. The enhancement in catalytic activity was attributed to improvement in surface hydrophobic characteristic from the incorporation of organic functionalities.