4th World Congress on Industrial Process Tomography, Aizu, Japan

3d Imaging of Reactive Distillation Packings with a New High Energy X-Ray Tomograph
D. Toye 1, J.B. Abdullah 2, M. Crine 1 and P. Marchot 1
1

Laboratory of Chemical Engineering, University of Lige, Sart-Tilman, B6, B4000 Lige, Belgium, Pierre.Marchot@ulg.ac.be 2 Malaysian Institute of Nuclear Technology Research (MINT), Bangi, 43000 Kajang, Malaysia

ABSTRACT
We describe a new, high energy (420 kV), large scale (0.45 m diam, 4 m high), X ray tomograph developed to investigate gas and liquid flow through fixed bed like absorption, distillation and reactive distillation columns. First results obtained with this setup on test objects such as a cylindrical container filled with water or a large diameter structured metallic packing are presented. 2D and 3D images of a 0.10 m diameter KATAPAK-SP, a reactive distillation packing, are also presented. Keywords: image reconstruction, reactive distillation, structured packings, X-ray tomography.

INTRODUCTION

The design of reactive distillation columns is far more complex than that of separated conventional distillation columns and chemical reactors. The introduction of separation and reaction zones in one single apparatus leads to complex interactions between hydrodynamics, vapour-liquid equilibrium, vapour-liquid mass transfer, internal diffusion and chemical kinetics. Various catalyst packing configurations based on a regular alternation of zones with weak permeability (catalytic zones) and of high permeability (gas liquid transfer zones) have been reported in the literature. These sandwich structures allow to postpone the flooding beyond usual operating flow rates and offer interesting new potentialities. In these types of packings, the solid catalyst particles are generally maintained in baskets constituted by metallic gauzes. They are separated by open channels or by portions of more classical structured packings. Baskets and channels may be packed together following many configurations allowing to adjust to the particular catalytic process. A few years ago, we developed large scale X-ray tomography at 160 kV to obtain, in a non intrusive way, images of the gas liquid flow patterns in fixed beds filled with plastic packings (Toye, 1998, Marchot, 2001). The selection of plastic materials was imposed because of the low energy of the rays, unable to cross metallic sheets. However, since most of the new structured and reactive distillation packings use stainless steel and since there is still a strong interest in fundamental studies in that field (Adler, 2000, Olujic, 2003, Schmit, 2004), we decided to build a new facility operating at higher energy.

MECHANICAL DESCRIPTION OF THE NEW X-RAY SETUP

The generator is a Baltograph CSD450 constant potential generator manufactured by Balteau NDT, Belgium. It is constituted by two identical high tension units, insulated by gaseous SF6, working 180 out of phase. It may be operated between 30 and 420 kV. The X-ray source (labelled S on figure 1) is an oil cooled, bipolar TSD420/3 tube (Comet and Balteau), producing a 40 aperture fan beam. Its minimum focus size is 0.8x0.8 mm following norm IEC336 EN12543. Its nominal intensity is 2 mA whereas its maximum value is 6.5 mA. A lead collimator produces a 1 mm thick fan beam. The detector (D) is an X-Scan 0.4f2-512-HE manufactured by Detection Technology (Finland). It is constituted by a linear array of 1280 photodiodes each coupled with a CdWO4 scintillator. The detector is 512 mm long with a 0.4 mm pixel pitch, 0.3 mm pixel width and a 0.6 mm pixel height. The integration time may be set from 0.67 to 10 ms and its dynamic range is 12 bits. The detector is operated with a frame grabber board ITI PC-DIG installed in a PC.

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The mechanical rig designed by PROACTIS Belgium, is constituted by two parts, a source-detector arm (A) and a rotating table (R) on which the object to be scanned is fixed. The arm is a very rigid metallic structure on which are embedded the source and the detector. This arm may be rotated by a fixed angle, around a vertical axis located at O, by an electrical jack, in such a way that the object lays out of the fan beam, this allows an easy calibration of the detectors. This arm is embedded to a carriage (C) which slides following two vertical high precision machined rails (R). The carriage vertical displacement is obtained with a great accuracy by a helicoidal screw (V) rotated a synchronous motor equipped with frequency variator. On figure 1, C represent the upper position of this carriage. This rig allows a vertical movement up to 3780 mm keeping verticality and horizontality errors within 1 mm. The high voltage cables, following a baffle (D), crosses a 0.6 m thick concrete wall (W) which surrounds the whole setup ensuring the radio protection of the laboratory. This cable is connected to the source (S) via a folding cable channel (B). Its position, when the carriage is in (C), is represented in (B). The column to be scanned is fitted on the lower turn table (R), the rotation is obtained by a synchronous motor equipped with frequency variator which is supervised by the data acquisition system. Objects up to 0.45 m diameter may be scanned. An upper freely rotating device is provided at the top (R) to guide the movement of the column.

Figure 1: X-ray setup. A : arm; B, B : cable channel lower and upper positions; C, C : carriage lower and upper positions; D : detector bank; E : baffle; O : arm rotation vertical axis; R, R rotating table; R : rails; S : X-ray source ; V : helicoidal screw; W : 0.6 m concrete wall.

Figure 2 illustrates the setup when it was installed outside the radio protected laboratory, a small room, inside which it is impossible to get a global view of the setup. On this picture there are no electrical connections nor detector. More views are available at www.ulg.ac.be/bioreact/

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Figure 2: Picture of the manipulator outside of the lab

DESCRIPTION OF THE CONTROL SYSTEM

The high voltage generators and the oil and water cooling devices are located outside the radio protected lab. All electrical commands including security checks are gathered into a system console. The operator interacts with the tomograph through three system interfaces. The first, called Balteau RC6, is used to set the focal spot size, voltage and current intensity of the source. It computes also the length of the preheating of the source as a function of its past utilisations, 22 min minimum. The second interface is a touch screen interface of a programmable logic controller (Hitachi EH-150 Series PLC). This controller manages the security checks concerning the x-ray, the vertical position of the arm, the rotation of the object and the data acquisition process. From the number of equiangular positions at which attenuations must be recorded, the controller computes the corresponding angles and compares them to the indications delivered by an angular coder which follows the rotation of the table. When angles match, the controller sends a signal to an external trigger which commands the frame grabber. The tomograph may be operated also in radiographic mode reading multiple attenuation lines at a fixed angular position. The third interface is the usual screen and keyboard of a rack mounted PC in which the frame grabber board, the external electronic trigger and the data storage of the attenuations are contained. It is connected to the University intranet, since reconstructions are performed in another building.

OPERATION OF THE TOMOGRAPH

1. When the installation is powered on, the security chain is checked by the programmable logic controller. 2. The X-ray source is pre-heated. 3. The vertical position coder is initialised. The x-ray source parameters (voltage, current intensity, focus spot size) are chosen as a function of the density of the object to be imaged. The detector integration time is entered from the PC keyboard. Its value is selected between 0.67 and 6.67 ms to obtain a good signal to noise ratio. 4. Instructions for detector calibration are entered from the PC keyboard The arm supporting the source and the detector is rotated around a vertical axis to allow a calibration with no object between the source and the detector. Offset and gain values are set for each of the photodiodes. The arm is then reset to its measuring position. 5. The measurement mode is selected : tomographic mode or radiographic mode.

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6. In tomographic mode, the number of equiangular positions at which attenuations are recorded is set between 480 and 12800. The resulting rotation time over 360 (from 45 s to 180 s) is computed by the controller. 7. In radiographic mode, the number of measured projections is set between 480 and 12800. The acquisition frequency is imposed by the detector integration time. 8. In both cases, attenuation data are stored in a rack mounted PC. Characteristics of the experimental run (date, name, settings,) are copied into of the first 2560 bytes of the hexadecimal file which is produced. 9. Data files are transferred to another building via the University intranet, since reconstructions are performed on another PC.

RECONSTRUCTION

Reconstruction of the object cross sections are obtained by the classical linear back projection algorithm adapted to the fan beam geometry implemented in the Fourier domain. In order to get a user friendly software, in this first step of the work, we interfaced the time consuming interpolation routine written in Fortran with Matlab 6.5. This provides a very convenient way to work and to visualize projection data as well to post-process the reconstructed images. 3D reconstruction are performed by stacking 2D reconstructed sections, box-filtering and computing the isosurfaces (i.e. surfaces of equal x-ray attenuation) of the resulting 3D matrix.

FIRST RESULTS

Presently, we are testing the setup with various solid objects (physical phantoms). Gas liquid measurements will be performed later, when these preliminary tests will have been completed. We present some reconstructed sections without tricky filtering. All the images are realised at 320 kV and 4mA with an integration time of 4 ms. Figure 3 shows a reconstructed section of a Pyrex glass cylindrical container filled with water. The vessel is 0.10 m external diameter and the wall is 2 mm thick. Scales are in 0.4 mm width pixels. Two arcs of circle are observed resulting from poor detector normalisation which is a difficulty that should be fixed soon.

Figure 3: Water filled 10 cm pyrex container

Figure 4a shows a picture of Montz-Pak, a metallic structured packing. On figure 4b, that shows a 2D reconstructed section, scales are in 0.4 mm width pixels. The packing is 0.38 m diameter, it is composed of 0.2 mm thick stainless steel corrugated sheets that are not perforated but embossed. There is no wall wiper but nails are used to tightened the sheets together.

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(a)

(b)

Figure 4: Montz-Pak metallic structured packing (diam.: 0.38 m)

(a)

(b)

(c)

(d)

Figure 5: Katapak-SP (Sulzer) (diam.:0.10 m)

Figure 5a shows a picture of Katapak-SP (Sulzer) a reactive distillation packing. Two 2D sections are reconstructed at two heights (5b, 5c) (scales are in 0.4 mm width pixels). The packing is 0.10 m diameter, it is composed of 0.2 mm thick stainless steel corrugated sheets with 4 mm holes, their surfaces are 1 mm embossed. Between these sheets, catalyst baskets (figure 5c) with wire mesh walls, are filled by 3 mm polypropylene spheres, they are closed by metallic clips. At some heights,

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baskets and sheets are tightened together by metallic wire mesh wall wipers. At these heights (5b), the catalyst baskets are empty and reduce to a thick vertical wire mesh. All these details are clearly visible on the sections. Figure 5d presents a 3D reconstruction of a very small part of this packing showing the texture of the embossed metallic sheets and some of their holes. Originally, the baskets were filled by a ion exchange catalyst that we replaced by plastic spheres.

CONCLUSIONS

These first results with a high energy X-ray tomography are extremely encouraging. They evidence the possibility of the method in investigating complex reactive distillation metallic packings. The absence of artefacts in reconstructing thick sections of water is particularly remarkable. Some problems remain to be fixed, especially in detector calibration procedure and possibly in some geometrical constants which are not yet optimised for the device. Finally, we consider the main challenge we met, i.e. having four engineering teams of different disciplines working together, and we are looking for new exciting results to come.

REFERENCES

ADLER, S., BEAVER, E., BRYAN, P., ROBINSON, S., WATSON, J., (2000), Vision 2020 Separations Roadmap, American Institute of Chemical Engineers, New York. OLUJIC, Z, FREY, G., JANSEN, H., KAIBEL, B., RIETFORT, T., ZICH, E., (2003), Distillation column internals related process intensification developments, Proceedings of the Sixth Italian Conference on Chemical and Process Engineering, June 2003, Pisa ( Italy) in Chemical Engineering Transactions, 3, pp. 367-372. TOYE, D., MARCHOT, P., CRINE, M., PELSSER, A-M., L'HOMME, G., (1998), Local measurements of void fraction and liquid holdup in packed columns using X-ray computed tomography, Chem. Eng. Process., 37 pp. 511-520. MARCHOT, P., TOYE, D., CRINE, M., L'HOMME, G., PELSSER, A-M., OLUJIC, Z., (2001), 3D Images of liquid distribution on Mellapak 250Y structured packing by X-ray tomography, AIChE J., 47 pp 1249-1480. SCHMIT, C.E., ELDRIGE, R.B., (2004), Investigation of X-ray imaging of vapor-liquid contactors. I. Studies involving stationary object and a simple flow system, Chem. Eng. Sci., 59, pp. 1255-1266.

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