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PubMed2002

Optimal design of radioactive particle tracking experiments for flow mapping in opaque multiphase reactors.

In the past decade, radioactive particle tracking techniques have emerged in the field of chemical engineering and have become increasingly popular for non-invasive flow mapping of the hydrodynamics in multiphase reactors. Based on gamma-ray sensitization of an array of scintillation detectors, the Computer Automated Radioactive Particle Tracking (CARPT) technique measures flow fields by monitoring the actual motion path of a single discrete radioactive flow follower which has the physical properties of the phase whose motion is being followed. A limitation to the accuracy of CARPT lies in the error associated with the reconstruction of the tracer particle position which affects the space-resolution capability of the technique. It is of interest, therefore, to minimize this error by choosing wisely the best hardware and an optimal configuration of CARPT detectors' array. Such choices are currently based on experience, without firm scientific basis. In this paper, through theoretical modeling and simulation, we describe how the accuracy of a radioactive particle tracking setup may be assessed a priori. Through an example of a proposed implementation of CARPT on a gas-solids riser, we demonstrate how this knowledge can be used for choosing the hardware required for the experiment. Finally, we show how the optimal arrangement of detectors can be effected for maximum accuracy for a given amount of monetary investment for the experiment.

Journal Article↗
PubMed2000

Epoxide electrophiles as activity-dependent cysteine protease profiling and discovery tools.

BACKGROUND: Analysis of global changes in gene transcription and translation by systems-based genomics and proteomics approaches provides only indirect information about protein function. In many cases, enzymatic activity fails to correlate with transcription or translation levels. Therefore, a direct method for broadly determining activities of an entire class of enzymes on a genome-wide scale would be of great utility. RESULTS: We have engineered chemical probes that can be used to broadly track activity of cysteine proteases. The structure of the general cysteine protease inhibitor E-64 was used as a scaffold. Analogs were synthesized by varying the core peptide recognition portion while adding affinity tags (biotin and radio-iodine) at distal sites. The resulting probes containing a P2 leucine residue (DCG-03 and DCG-04) targeted the same broad set of cysteine proteases as E-64 and were used to profile these proteases during the progression of a normal skin cell to a carcinoma. A library of DCG-04 derivatives was constructed in which the leucine residue was replaced with all natural amino acids. This library was used to obtain inhibitor activity profiles for multiple protease targets in crude cellular extracts. Finally, the affinity tag of DCG-04 allowed purification of modified proteases and identification by mass spectrometry. CONCLUSIONS: We have created a simple and flexible method for functionally identifying cysteine proteases while simultaneously tracking their relative activity levels in crude protein mixtures. These probes were used to determine relative activities of multiple proteases throughout a defined model system for cancer progression. Furthermore, information obtained from libraries of affinity probes provides a rapid method for obtaining detailed functional information without the need for prior purification/identification of targets.

Affinity Labels↗
PubMed2003

Single excitation multiple image RARE (SEMI-RARE): ultra-fast imaging of static and flowing systems.

This paper describes the development and application of a new rapid, full k-space acquisition imaging pulse sequence based on the rapid acquisition with relaxation enhancement (RARE) methodology. We have termed this pulse sequence single excitation multiple image RARE (SEMI-RARE). We demonstrate the application of SEMI-RARE to the visualisation of a static liquid phantom and it is shown that up to 120 images can be acquired from a single excitation. By exploiting the inherent relaxation and diffusion contrast within the series of images, the SEMI-RARE provides an ultra-fast method for characterising the spatial distribution of chemical species and phases within complex systems. The pulse sequence is then applied to the study of single- and two-phase flow in a single narrow tube of inner diameter 2.9mm. In particular, it is shown that 8 two-dimensional slice-selective images for two-phase bubble-train flow in a single tube can be acquired from a single excitation at effective echo-times of 37, 109, 181, 253, 325, 397, 469, and 541ms. The visualisation enables the determination of gas/liquid bubble sizes and velocities during two-phase flow. We also report the first direct evidence, obtained from magnetic resonance measurements, of liquid re-circulation zones associated with bubble-train flow. The robustness of the SEMI-RARE technique makes it an attractive fast imaging technique for the study of multi-phase flow phenomena, which are often characterised by large variations in magnetic susceptibility, and are of widespread interest in chemical engineering.

Journal Article↗
PubMed2004

Enhancement of the knowledge on the ultrasonic reactor behaviour by an interdisciplinary approach.

Our work is a step to a better understanding of high frequency ultrasonic reactors behaviour. Using finite elements calculations, it was demonstrated that localization of chemical and physical effects can be well correlated with mechanical behaviour of ultrasound emitter. This complementary approach enables us to propose a full interpretation of the sonochemical reactor behaviour. A major reason of scientific interest on ultrasound is the well-known enhancement of chemical or physical phenomena. This is so important that "Enhancement" is probably the most used word in the title of related publications. To fully understand experimental results, present work demonstrates that ultrasound needs also to significantly enhance a very difficult knowledge transfer operation that might be named interdisciplinary co-working. Hence, ultrasound is now used and studied in many different fields of science such as acoustic, chemistry, medical imaging, disease treatment (lithotripsy), non-destructive testing. Each one has his own vocabulary, approach, and method to describe the phenomenon. In this work four different methodologies were involved to study of the same effect but using a chemical, chemical engineering, physical and mechanical approach respectively. All these viewpoints were then brought together in order to explain new original results.

Journal Article↗
PubMed1999

Cross-linked enzyme crystals.

The active site of cross-linked enzyme crystals can be further modified by chemical means, yielding a new type of chemically engineered enzyme. In the past year, the characteristics of cross-linked protein crystals as microporous materials have been studied and used as stationary phases in chromatographic separations.

Biotransformation↗
PubMed1995

Artificial cells with emphasis on bioencapsulation in biotechnology.

The most common use of artificial cells is for bioencapsulation of biologically active materials. Each artificial cell can contain combinations of materials. The permeability, composition and shape of an artificial cell membrane can be varied using different types of synthetic or biological materials. These possible variations in contents and membranes allow for large variations in the properties and functions of artificial cells. Artificial cells containing adsorbents have been a routine form of treatment in hemoperfusion for patients. This includes acute poisoning, high blood aluminum and iron, and supplement to dialysis in kidney failure. Artificial red blood cell substitutes based on modified hemoglobin are already in Phase I and Phase II clinical trials in patients. Artificial cell encapsulated cell cultures are being studied for the treatment of diabetes, liver failure, gene therapy and other conditions. Research on artificial cells containing enzymes includes their use for treatment in hereditary enzyme deficiency diseases and other diseases. Recent demonstration of extensive enterorecirculation of amino acids in the intestine has allowed oral administration to deplete specific amino acids. One example is phenylketonuria, an inborn error or metabolism resulting in high systemic phenylalanine levels. Preliminary clinical studies in patients using bioencapsulation of cells or enzymes have started. Artificial cells containing complex enzyme systems convert wastes like urea and ammonia into essential amino acids. Artificial cells are being used for the production of monoclonal antibodies, interferon and other biotechnological products. Other areas of biotechnological uses include drug delivery, and other areas of biotechnology, chemical engineering and medicine.

Aluminum↗
PubMed2002

Origins, current status, and future challenges of green chemistry.

Over the course of the past decade, green chemistry has demonstrated how fundamental scientific methodologies can protect human health and the environment in an economically beneficial manner. Significant progress is being made in several key research areas, such as catalysis, the design of safer chemicals and environmentally benign solvents, and the development of renewable feedstocks. Current and future chemists are being trained to design products and processes with an increased awareness for environmental impact. Outreach activities within the green chemistry community highlight the potential for chemistry to solve many of the global environmental challenges we now face. The origins and basis of green chemistry chart a course for achieving environmental and economic prosperity inherent in a sustainable world.

Chemical Engineering↗
PubMedDate not supplied

A cysteine-linkable, short cleavable photoprobe with dual functionality to explore protein-protein interfaces.

We developed a bifunctional photoprobe with dual functionality, that can be specifically tethered to cysteinyl residues of peptides and proteins through a short cleavable disulfide bond. Thus, an aryldiazonium moiety is positioned at approximately 8.5 A from the modified cysteinyl alpha-carbon, leading to one of the shortest cleavable linkages. In a sodium azide-containing buffer, the aryldiazonium moiety is transformed into an aryl azide. Therefore, with one bifunctional photoprobe two types of photogenerated species can be obtained: a hydrophilic and positively charged arylcation or a hydrophobic nitrene. We coupled the aryldiazonium probe, in a site-directed manner, to a nicotinic acetylcholine receptor competitive antagonist, obtained by chemical engineering of an analogue of a snake alpha-neurotoxin. In this molecule, Arg33, which is known to interact with the receptor, was replaced by a cysteine residue, where the photoprobe could be attached. Under inactinic light, this novel photosensitive snake toxin behaved as a reversible ligand on the Torpedo acetylcholine receptor. However, when irradiated at 391 nm, it generated a highly reactive arylcation which labeled mostly the receptor alpha-subunit, confirming the location of the tip of the second toxic loop near this receptor subunit. Finally, we showed that reduction of the disulfide bond, linking the ligand to the photocoupled receptor, allowed introduction of radioactivity on the labeled residue(s), opening the way to further characterization and avoiding the synthesis of a radioactive bifunctional photoprobe.

Animals↗
PubMed2004

Highly efficient liquid-phase photooxidation of an azo dye methyl orange over novel nanostructured porous titanate-based fiber of self-supported radially aligned H2Ti8O17 x 1.5H2O nanorods.

Novel nanostructured porous fibers of self-supported, radially aligned H2Ti8O17 x 1.5H2O nanorods were prepared from layered H2Ti4O9 x 1.2H2O tetratitanate fibers by novel solvothermal reaction in glycerine at 150-250 degrees C. The H2Ti8O17 x 1.5H2O fibers with diameters of 0.5-1.5 microm and lengths of 10-20 microm consist of multi-scale nanopores and nanostructures. They also are of high crystallinity, large surface area of 127 m2 g(-1), and stable phase up to 350 degrees C. Photocatalytic activity of the H2Ti8O17 x 1.5H2O fibers was evaluated in aqueous photooxidation of an azo dye methyl orange in the presence of UV irradiation and 02, using P-25 as the standard sample. Both the photocatalytic activity and the dispersity-agglomeration property of H2Ti8O17 x 1.5H2O fibers are pH-controllable. Highly photooxidative activity, superior to that of P-25, occurs at pH 6.0-11.0 due to certain distinguishable material characteristics and to large amounts of adsorbed reactants of surface active OH* free radicals, surface hydroxyl OH, O2*-, O*OH, and methyl orange. The agglomeration of H2Ti8O17 x 1.5H2O fibers becomes more serious from pH 2.0 to pH 5.0 and from pH 6.0 to pH 11.0. Well-dispersed H2Ti8O17 x 1.5H2O fibers occur at pH 6.0. Both the total photodegradation of waste chemicals and the entire sedimentation of H2Ti8O17 x 1.5H2O fibers can be timed to end simultaneously at suitable pH value. The photocatalyst-free reaction solution is then easily removed, and the fresh wastewater is added again. Standard unit operation processes of chemical engineering are used to design a continuous, low-cost, large-scale, liquid-phase photocatalysis technique based on the H2Ti8O17 x 1.5H2O fibers.

Azo Compounds↗
PubMed2003

Do Aviram-Ratner diodes rectify?

We present state-of-the-art first principles calculations for the IV characteristics of a donor-insulator-acceptor (DsigmaA) type molecular diode anchored with thiolate bonds to two gold electrodes. We find very poor diode characteristics of the device, and the origin of this is analyzed in terms of the bias-dependent electronic structure. At zero bias, the highest occupied molecular orbital (HOMO) is confined to the D part, and the lowest unoccupied molecular orbital (LUMO) is confined to the A part, while at 3.8 V the two states align, and this gives rise to an increasing current. The latter is a potential mechanism for rectification and may in some cases lead to favorable diode characteristics. We identify the origin of the vanishing rectification for the investigated molecule, and on the basis of this we suggest parameters which are important for successful chemical engineering of DsigmaA rectifiers.

Journal Article↗
PubMed2005

Quantitative description of the relation between protein net charge and protein adsorption to air-water interfaces.

In this study a set of chemically engineered variants of ovalbumin was produced to study the effects of electrostatic charge on the adsorption kinetics and resulting surface pressure at the air-water interface. The modification itself was based on the coupling of succinic anhydride to lysine residues on the protein surface. After purification of the modified proteins, five homogeneous batches were obtained with increasing degrees of modification and zeta-potentials ranging from -19 to -26 mV (-17 mV for native ovalbumin). These batches showed no changes in secondary, tertiary, or quaternary structure compared to the native protein. However, the rate of adsorption as measured with ellipsometry was found to decrease with increasing net charge, even at the initial stages of adsorption. This indicates an energy barrier to adsorption. With the use of a model based on the random sequential adsorption model, the energy barrier for adsorption was calculated and found to increase from 4.7 kT to 6.1 kT when the protein net charge was increased from -12 to -26. A second effect was that the increased electrostatic repulsion resulted in a larger apparent size of the adsorbed proteins, which went from 19 to 31 nm2 (native and highest modification, respectively), corresponding to similar interaction energies at saturation. The interaction energy was found to determine not only the saturation surface load but also the surface pressure as a function of the surface load. This work shows that, in order to describe the functionality of proteins at interfaces, they can be described as hard colloidal particles. Further, it is shown that the build-up of protein surface layers can be described by the coulombic interactions, exposed protein hydrophobicity, and size.

Adsorption↗
PubMed2006

Effect of pore packing defects in 2-d ordered mesoporous carbons on ionic transport.

Ordered mesoporous materials show great importance in energy, environmental, and chemical engineering. The diffusion of guest species in mesoporous networks plays an important role in these applications, especially for energy storage, such as supercapacitors based on ordered mesoporous carbons (OMCs). The ion diffusion behavior in two different 2-D hexagonal OMCs was investigated by using cyclic voltametry and electrochemical impedance spectroscopy. In addition, transmission electron microscopy, small-angle X-ray diffraction, and nitrogen cryosorption methods were used to study the pore structure variations of these two OMCs. It was found that, for the OMC with defective pore channels (termed as pore packing defects), the gravimetric capacitance was greatly decayed when the voltage scan rate was increased. The experimental results suggest that, for the ion diffusion in 2-D hexagonal OMCs with similar mesopore size distribution, the pore packing defect is a dominant dynamic factor.

Journal Article↗
PubMed2000

A new method for yeast recovery in batch ethanol fermentations: filter aid filtration followed by separation of yeast from filter aid using hydrocyclones.

In the Melle-Boinot process for alcohol production, centrifuges are normally used for yeast recovery at the end of a batch fermentation. Centrifuges are expensive equipment and represent an impressive part of the equipment costs in alcohol industries. In the present work, an alternative method for yeast recovery using less expensive equipment was studied. Instead of using centrifuges, yeast was separated from the fermented broth by filter aid filtration, followed by separation of yeast from the filter aid using hydrocyclones. A stainless steel plate-and-frame filter of filtration area 1.14 m2 and two 30 mm hydrocyclones, which followed the Bradley and Rietema recommended proportions, were used in this work. The filter aid was perlite. Tests of direct separation of yeast from the fermented broth using the Bradley hydrocyclone proved to be completely unfeasible, since the maximal reduced total efficiency obtained was only 1%. When the hydrocyclones were used to separate perlite from the resuspended filtration cake, the perlite total separation efficiency obtained in the underflow was as high as 95% when using the Bradley hydrocyclone with an underflow diameter of 3 mm. To show the feasibility of the proposed new method of yeast recovery, a complete cycle of experiments, which included fermentation, yeast separation, and new fermentation using the recycled cells, was performed with good results.

Centrifugation↗
PubMed2000

Stress transmission through a model system of cohesionless elastic grains

Understanding the mechanical properties of granular materials is important for applications in civil and chemical engineering, geophysical sciences and the food industry, as well as for the control or prevention of avalanches and landslides. Unlike continuous media, granular materials lack cohesion, and cannot resist tensile stresses. Current descriptions of the mechanical properties of collections of cohesionless grains have relied either on elasto-plastic models classically used in civil engineering, or on a recent model involving hyperbolic equations. The former models suggest that collections of elastic grains submitted to a compressive load will behave elastically. Here we present the results of an experiment on a two-dimensional model system--made of discrete square cells submitted to a point load--in which the region in which the stress is confined is photoelastically visualized as a parabola. These results, which can be interpreted within a statistical framework, demonstrate that the collective response of the pile contradicts the standard elastic predictions and supports a diffusive description of stress transmission. We expect that these findings will be applicable to problems in soil mechanics, such as the behaviour of cohesionless soils or sand piles.

Journal Article↗
PubMed2005

Silencing of microRNAs in vivo with 'antagomirs'.

MicroRNAs (miRNAs) are an abundant class of non-coding RNAs that are believed to be important in many biological processes through regulation of gene expression. The precise molecular function of miRNAs in mammals is largely unknown and a better understanding will require loss-of-function studies in vivo. Here we show that a novel class of chemically engineered oligonucleotides, termed 'antagomirs', are efficient and specific silencers of endogenous miRNAs in mice. Intravenous administration of antagomirs against miR-16, miR-122, miR-192 and miR-194 resulted in a marked reduction of corresponding miRNA levels in liver, lung, kidney, heart, intestine, fat, skin, bone marrow, muscle, ovaries and adrenals. The silencing of endogenous miRNAs by this novel method is specific, efficient and long-lasting. The biological significance of silencing miRNAs with the use of antagomirs was studied for miR-122, an abundant liver-specific miRNA. Gene expression and bioinformatic analysis of messenger RNA from antagomir-treated animals revealed that the 3' untranslated regions of upregulated genes are strongly enriched in miR-122 recognition motifs, whereas downregulated genes are depleted in these motifs. Analysis of the functional annotation of downregulated genes specifically predicted that cholesterol biosynthesis genes would be affected by miR-122, and plasma cholesterol measurements showed reduced levels in antagomir-122-treated mice. Our findings show that antagomirs are powerful tools to silence specific miRNAs in vivo and may represent a therapeutic strategy for silencing miRNAs in disease.

3' Untranslated Regions↗
PubMed2006

Recent progress on nanovehicles.

Nanovehicles are a new class of molecular machines consisting of a molecular scale chassis, axles, and wheels, that can roll across solid surfaces with structurally defined directions making them of interest to synthetic chemists, surface scientists, chemical engineers, and the general car enthusiast. In this tutorial review, following a brief introduction to the development of nanomachines, our recent progress on the nanovehicle project is presented including the design, synthesis, and testing of a series of nanocars, nanotrucks, and motorized nanocars.

Journal Article↗
PubMed2002

Effect of different solvents and crosslinkers on cytocompatibility of Type II collagen scaffolds for chondrocyte seeding.

Type II collagen extracted from porcine costal cartilage was evaluated as scaffolds for cartilage tissue engineering. Chemical crosslinkers were employed to improve the mechanical properties and the resistance toward degradation. Films and porous scaffolds were prepared from collagen solutions dissolved in 3% acetic acid (designated A) or in deionized water (designated W) and crosslinked by an epoxy (designated E) or by a carbodiimide (designated C). Immortalized rat chondrocytes and rabbit chondrocytes were used to assess cytocompatibility of crosslinked collagen matrices. Cell adhesion rate onto the films made by different preparations ranked in the order of WE > or = WC > AC > or = AE. Cell proliferation ranked in the order of AC > WC > AE > or = WE. Cells maintained round morphology only on AC and WC films. In 3-D seeding, AC scaffolds also were found to be the most cytocompatible. WC scaffolds, however, had better dimensional stability. It was concluded that Type II collagen scaffolds, when prepared by using deionized water as the solvent and carbodiimide as the crosslinker, could promote chondrocyte growth and matrix production.

Animals↗
PubMed2005

Effect of long retention time in the settler on phosphorus removal from communal wastewater.

GOALS: The objective of the paper is to illustrate the solution of a chronic problem occurring in a wastewater treatment facility with a capacity of 12,000 inhabitant equivalent. A drastic phosphorus concentration increase (two or three times higher than the Hungarian limit of 1 mg/l) was observed in the wastewater treatment facility for a long time (12-24 h) with changing time periods indicating malfunctioning in the operation of the facility. METHODS: Computer-aided simulation technique was used to develop a solution for the treatment of the problem using a software developed by the Department of Environmental and Chemical Engineering, University of Veszprém, Hungary. RESULTS AND DISCUSSION: The simulation studies show that if the nightly inflow is less than 200 m3/h at least for two hours, the system doesn't then receive enough fresh nutrients which can cause a deficiency in the nutrient uptake of the PAOs in the anaerobic zones. This can result in the fact that the PAOs accumulate less phosphorus into the aerobic zones. CONCLUSION: Long retention time (10 h) is the reason for the problem, namely--under special conditions--the phosphorus in the sludge of the settling tank of the wastewater treatment plant. The problem was caused by phosphorus dissolution from the sludge of the settling tank during the undesirably long retention time.

Computer Simulation↗