Mechanism and kinetics of the catalytic CO-H2 reaction: An approach by chemical transients and surface relaxation spectroscopy

The aim of this paper is to demonstrate the importance of providing time-resolved information in catalysis research. Two truly in situ methods will be presented and compared for their merits and drawbacks: chemical transient kinetics (CTK) and pulsed field desorption mass spectrometry (PFDMS). The presentation will be given by way of example choosing the syngas (CO/H2) reaction over cobalt-based catalysts as a catalytic process. Despite numerous efforts in the past, the mechanism of this reaction is still under debate. In CTK the reaction is studied on a metal-supported catalyst under flow conditions in a pressure range extending from atmospheric pressure down to 100 Pa. Sudden changes in the partial pressures of the reactants then allow following the relaxation to either steady-state conditions ("transients") or cleanoff ("back transients"). In PFDMS short field pulses of several volts per nanometer are applied to a model catalyst which resembles a single metal particle grain (a "tip"). These pulses intervene during the ongoing reaction under flow conditions at pressures ranging from 10(-1) to 10(-5) Pa and cause field desorption of adsorbed species. This method is particularly suited to detect reaction intermediates in a time-dependent manner since the repetition frequency of the pulses can be systematically varied. It is shown that both methods lead to complementary results. While CTK allows conclusions on the mechanism of CO hydrogenation by following the time-dependent formation of hydrocarbon species, PFDMS provides insight into the initial steps leading to adsorbed CxHy species. A quantitative assessment of the CTK data allows the demonstration that the catalyst under working conditions is in an oxidized rather than metallic state. The initial steps to oxidation are also traced by PFDMS. Most importantly, however, CTK results allow formulation of a reaction mechanism that is common for both hydrocarbon and oxygenate formation and is based on the occurrence of a formate-type species as the most abundant surface intermediate.     

Robust formation of morphogen gradients

We discuss the formation of graded morphogen profiles in a cell layer by nonlinear transport phenomena, important for patterning developing organisms. We focus on a process termed transcytosis, where morphogen transport results from the binding of ligands to receptors on the cell surface, incorporation into the cell, and subsequent externalization. Starting from a microscopic model, we derive effective transport equations. We show that, in contrast to morphogen transport by extracellular diffusion, transcytosis leads to robust ligand profiles which are insensitive to the rate of ligand production.     

Investigation of the interaction of evaporated aluminum with vapor deposited Teflon AF films via X-ray photoelectron spectroscopy

The interfacial bonding and mixing between evaporated aluminum and a vapor deposited Teflon AF (abbreviated to AF) film have been investigated with X-ray photoelectron spectroscopy. Graphite carbon (C–C), and aluminum carbide (Al–C), oxide (Al–O–C) and fluoride (Al–F) are formed when aluminum atoms are deposited on to the AF film. With increasing deposition of aluminum, the concentrations of these newly formed components increase gradually. Moreover, in situ annealing results in remarkable increases in the C–C, Al–C, Al–O–C and Al–F configurations and a decrease in metallic aluminum. No significant diffusion of aluminum into the AF film was observed during the annealing. The Al compounds form a layer at the Al/AF interface that acts as an adhesion promoter and diffusion barrier. Received: 21 October 2002 / Accepted: 22 October 2002 / Published online: 15 January 2003 RID="*" ID="*"Corresponding author. Fax: +49-431/880-6229, E-mail: sjding@yahoo.com     

Synthesis of isobutyl-C-galactoside (IBCG) as an isopropylthiogalactoside (IPTG) substitute for increased induction of protein expression

[reaction: see text] Addition of isopropyl-beta-d-thiogalactopyranoside (IPTG) to bacterial cultures is often used to induce expression of plasmid-based genes for the production of recombinant proteins under control of the lac promoter, but a simple method to circumvent the inherent instability of this compound has not been addressed experimentally. Herein we report the first synthesis of isobutyl-C-galactoside (IBCG), the C-glycoside analogue of IPTG, and show that IBCG is superior to IPTG in inducing protein expression over long induction times.     

Driven Diffusive Systems of Active Filament Bundles

The cytoskeleton is an important subsystem of cells that is involved for example in cell division and locomotion. It consists of filaments that are cross-linked by molecular motors that can induce relative sliding between filaments and generate stresses in the network. In order to study the effects of fluctuations on the dynamics of such a system we introduce here a new class of driven diffusive systems mimicking the dynamics of active filament bundles where the filaments are aligned with respect to a common axis. After introducing the model class we first analyze an exactly solvable case and find condensation. For the general case we perform a mean-field analysis and study the behavior on large length scales by coarse-graining. We determine conditions for condensation and establish a relation between the hopping rates and the tension generated in the bundle.