Rigorous Multicomponent Reactive Separations Modelling : Complete Consideration of Reaction-Diffusion Phenomena

This paper gives the first step of the development of a rigorous multicomponent reactive separation model. Such a model is highly essential to further the optimization of acid gases removal plants (CO2 capture, gas treating, etc.) in terms of size and energy consumption, since chemical solvents are conventionally used.Firstly, two main modelling approaches are presented: the equilibrium-based and the rate-based approaches. Secondly, an extended rate-based model with rigorous modelling methodology for diffusion-reaction phenomena is proposed. The film theory and the generalized Maxwell-Stefan equations are used in order to characterize multicomponent interactions. The complete chain of chemical reactions is taken into account. The reactions can be kinetically controlled or at chemical equilibrium, and they are considered for both liquid film and liquid bulk. Thirdly, the method of numerical resolution is described. Coupling the generalized Maxwell-Stefan equations with chemical equilibrium equations leads to a highly non-linear Differential-Algebraic Equations system known as DAE index 3. The set of equations is discretized with finite-differences as its integration by Gear method is complex. The resulting algebraic system is resolved by the Newton- Raphson method. Finally, the present model and the associated methods of numerical resolution are validated for the example of esterification of methanol. This archetype non-electrolytic system permits an interesting analysis of reaction impact on mass transfer, especially near the phase interface. The numerical resolution of the model by Newton-Raphson method gives good results in terms of calculation time and convergence. The simulations show that the impact of reactions at chemical equilibrium and that of kinetically controlled reactions with high kinetics on mass transfer is relatively similar. Moreover, the Fick’s law is less adapted for multicomponent mixtures where some abnormalities such as counter-diffusion take place

Gas Holdup in a Trayed Cold-Flow Bubble Column

An Experimental Study Was Performed to Investigate the Effect of Sieve Trays on the Time-Averaged Gas Holdup Profiles and the overall Gas Holdup in a Cold-Flow Bubble Column that Was Scaled-Down from a Commercial Unit. Γ-Ray Computed Tomography (CT) Was Used to Scan the Column at Several Axial Locations in the Presence and Absence of Trays from Which the Local Variation of the Gas Holdup Was Extracted. the overall Gas Holdup Was Also Determined using the Same Configuration by Comparing the Expanded and Static Liquid Heights. Air and Water Were Used as the Gas-Liquid System. the Superficial Gas and Liquid Velocities Were Selected to Span the Range of the Commercial System using Gas Spargers Having Multiple Lateral Distributors that Were Also Scaled-Down from the Commercial Design. to Investigate the Impact of Sparger Hole Density on the Local and overall Gas Holdup, Two Difference Sparger Designs Were Used in Which the Hole Density Per Lateral Was Varied. the Gas Hole Velocity Was Maintained Constant at Ca. 245 M/s, Which Approached that Used in the Commercial Reactor. It is Shown that the Local Gas Holdup Determined by CT is Generally Higher in the Tray Down Comer Region and Exhibits an Asymmetric Pattern When Trays Are Present. the Use of Increased Sparger Hole Density at a Constant Gas Superficial Velocity Leads to Steeper Gradient in the Gas Holdup Near the Column Centerline and a Higher overall Gas Holdup. These Findings Suggest that the Performance of Bubble Column Reactors for Various Applications is Sensitive to Both Sparger and Tray Design. © 2001 Elsevier Science Ltd. All Rights Reserved

Using Rheo-Small-Angle Neutron Scattering to Understand How Functionalised Dipeptides Form Gels

We explore the use of rheo-small-angle neutron scattering as a method to collect structural information from neutron scattering simultaneously with rheology to understand how low-molecular-weight hydrogels form and behave under shear. We examine three different gelling hydrogel systems to assess what structures are formed and how these influence the rheology. Furthermore, we probe what is happening to the network during syneresis and why the gels do not recover after an applied strain. All this information is vital when considering gels for applications such as 3D-printing and injection

The effect of solvent choice on the gelation and final hydrogel properties of Fmoc–diphenylalanine

Gels can be formed by dissolving Fmoc–diphenylalanine (Fmoc–PhePhe or FmocFF) in an organic solvent and adding water. We show here that the choice and amount of organic solvent allows the rheological properties of the gel to be tuned. The differences in properties arise from the microstructure of the fibre network formed. The organic solvent can then be removed post-gelation, without significant changes in the rheological properties. Gels formed using acetone are meta-stable and crystals of FmocFF suitable for X-ray diffraction can be collected from this gel

Application of X-ray micro-computed tomography on high-speed cavitating diesel fuel flows

The flow inside a purpose built enlarged single-orifice nozzle replica is quantified using time-averaged X-ray micro-computed tomography (micro-CT) and high-speed shadowgraphy. Results have been obtained at Reynolds and cavitation numbers similar to those of real-size injectors. Good agreement for the cavitation extent inside the orifice is found between the micro-CT and the corresponding temporal mean 2D cavitation image, as captured by the high-speed camera. However, the internal 3D structure of the developing cavitation cloud reveals a hollow vapour cloud ring formed at the hole entrance and extending only at the lower part of the hole due to the asymmetric flow entry. Moreover, the cavitation volume fraction exhibits a significant gradient along the orifice volume. The cavitation number and the needle valve lift seem to be the most influential operating parameters, while the Reynolds number seems to have only small effect for the range of values tested. Overall, the study demonstrates that use of micro-CT can be a reliable tool for cavitation in nozzle orifices operating under nominal steady-state conditions

Computational Fluid Dynamics of Catalytic Reactors

Today, the challenge in chemical and material synthesis is not only the development of new catalysts and supports to synthesize a desired product, but also the understanding of the interaction of the catalyst with the surrounding flow field. Computational Fluid Dynamics or CFD is the analysis of fluid flow, heat and mass transfer and chemical reactions by means of computer-based numerical simulations. CFD has matured into a powerful tool with a wide range of applications in industry and academia. From a reaction engineering perspective, main advantages are reduction of time and costs for reactor design and optimization, and the ability to study systems where experiments can hardly be performed, e.g., hazardous conditions or beyond normal operation limits. However, the simulation results will always remain a reflection of the uncertainty in the underlying models and physicochemical parameters so that in general a careful experimental validation is required. This chapter introduces the application of CFD simulations in heterogeneous catalysis. Catalytic reactors can be classified by the geometrical design of the catalyst material (e.g. monoliths, particles, pellets, washcoats). Approaches for modeling and numerical simulation of the various catalyst types are presented. Focus is put on the principal concepts for coupling the physical and chemical processes on different levels of details, and on illustrative applications. Models for surface reaction kinetics and turbulence are described and an overview on available numerical methods and computational tools is provided

ADVANCED DIAGNOSTIC TECHNIQUES FOR THREE-PHASE SLURRY BUBBLE COLUMN REACTORS (SBCR)

This report summarizes the accomplishment made during the first year of this cooperative research effort between Washington University, Ohio State University and Air Products and Chemicals. A technical review of the variables affecting the SBCR performance, some aspects of bubble dynamics and hydrodynamics properties and physical properties of FT waxes and catalyst have been performed. The needed experimental facilities and measurement techniques have been evaluated and prepared. Exxon Norpar 14 has been suggested as a solvent to be used that mimics at room temperature and pressure up to 200 psi the hydrodynamics of FT waxes. A new correlation has been developed and tested to predict gas-liquid mass transfer coefficient at high pressure operation based on high pressure gas holdup and atmospheric data of gas-liquid mass transfer coefficient