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A Comparative Study of Various Size Distribution Measurement Systems

Andreas M. Neumann*, Herman J. M. Kramer**
(Received: 31 July 2001)

Abstract One of the major product specifications of a crystalline material is the crystal size distribution (CSD). In order to monitor and control the CSD in an industrial crystallization process, on-line sensors are required. Over the years, a number of techniques to measure the CSD have been established. In this paper, three instruments operated in an on-line fashion and an offline method are compared. The instruments were the OPUS, a HELOS/VARIO (both manufactured by Sympatec) and a Malvern 2600c (manufactured by Malvern). They were implemented on an 1100-l evaporative draft tube baffle (DTB) crystallizer producing ammonium sulfate crystals from aqueous solution. Samples from this crystallizer were also analyzed offline by wet sieving. The results show reasonably good agreement between the different on-line techniques and the wet sieving technique concerning the shape of the distribution. However, there is a discrepancy regarding the absolute values, which can be explained by the fact that the techniques used are based on different measuring principles.

Keywords: crystal size distribution, on-line technique, comparative study

1 Introduction
The crystal size distribution (CSD) is one of the most important product requirements in industrial crystallization. The shape of the CSD determines to a large extent the behavior of the product in downstream handling processes such as solid-liquid separation and conveying. For instance, an excess of fine crystals will typically result in poor filterability and a higher tendency for caking or give rise to large losses in air dryers. Operational problems in industrial crystallizers often cause temporary changes in the CSD of the crystals produced and in some cases can result in open loop unstable behavior. Monitoring of the CSD of the crystal suspension is therefore of major importance and a prerequisite for optimization and/or control of the product quality in an industrial crystallizer. In industrial practice, monitoring of the CSD is mostly realized by
* Dr. Dipl.-Ing. A. M. Neumann, Akzo Nobel Chemicals bv, Chemicals Research Arnhem, CPT-S, P.O. Box 9300, 6800 SB Arnhem (The Netherlands). ** Dr. ir. H. J. M. Kramer, Laboratory for Process Equipment, Delft University of Technology, Leeghwaterstraat 44, 2628 CA Delft (The Netherlands). E-mail: h.j.m.kramer@wbmt.tudelft.nl
WILEY-VCH Verlag GmbH, 69469 Weinheim, Germany, 2002

taking (dry) samples from the crystallizer followed by a CSD analysis in the laboratory (Coulter Counter, sieving, laser diffraction, etc.). It has recently been shown, however, that possibilities exist for on-line measurements [1] and even in-line measurements of the CSD [2]. The particle size determined by a given analyzer is strongly dependent on the measurement principle of the particular piece of equipment. For a spherical particle, the diameter or radius is an accurate single number index of size, thus making it possible to describe and measure unambiguously its size, even if different analyzers using different particle size indices are utilized. Strictly, this is not applicable for instruments measuring chord length. The more the particle shape deviates from that of a sphere, the more the size information obtained by one analyzer deviates from that of another. Hence the interpretation and intercorrelation of data (for various reasons, e.g. consistency of quality control, assessment of kinetic data, etc.) obtained from analyzers/methods exploiting different physical principles becomes a difficult task requiring a fundamental understanding of the underlying principles employed for sizing. It may even be difficult to correlate data from the same type of analyzer, e.g. due to different deconvolution algorithms employed to reconstruct the CSD [3 6].
0934-0866/02/1901/0017 $ 17.50+.50/0

18 In this study, two measurement methods were applied in an on-line fashion and their results were compared with those from an off-line sieve analysis. The first technique, laser diffraction, is nowadays one of the most widely applied techniques for measuring the CSD. When this technique is employed for the purpose of on-line Techset CSD measurements in industrial crystallizers, however, a number of disadvantages become evident. The most critical one is related to the fact that the use of this technique is restricted to a solid concentration of approximately 1.5 vol.%, whereas the product concentration in industrial crystallizers is generally an order of magnitude higher. This requires dilution of the product to the appropriate concentration, which involves a complex procedure. The second method used is based on the principle of measuring the attenuation of ultrasonic waves propagating through the slurry to be measured. One of the main advantages of this technique is that it can measure the CSD at much higher slurry concentrations (of the order of 40 vol.%). For this study, a Malvern 2600c (equipped with a 1000 mm Fourier lens) and a HELOS/VARIO (equipped with a 2000 mm Fourier lens), both laser diffraction measurement systems, and the ultrasonic instrument, OPUS, were implemented on an 1100-l draft tube baffle (DTB) crystallizer. In addition, solid samples were taken from the crystallizer, analyzed by wet sieving and compared with the results obtained from the on-line techniques.

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Fig. 1: Implementation of the measuring devices on the DTB crystallizer.

2 Experimental
An 1100-l draft tube baffle (DTB) crystallizer was used to evaluate the different measurement techniques. The crystallizer was operated continuously in an evaporative mode at a constant temperature of 50 8C, producing ammonium sulfate crystals from aqueous solution. Neumann et al. [7] gave a detailed description of the crystallizer and the experiments performed. In this paper only one of the experiments performed is considered. 2.1 Implementation of the Measuring Devices The measuring devices under evaluation were implemented on the crystallizer as depicted in Figure 1. The OPUS was situated in the product loop of the crystallizer whereas the Malvern and HELOS were placed, in series, in a separate measuring loop. After passing through the OPUS a small stream of product was continuously removed from the product line (stream 1) by means of an impeller pump (stream 2). At regular time intervals (2 min), the positions of the pneumatic valves (marked with asterisks in Figure 1) were switched and part of the product stream was injected for approximately 20 s into a

dilution stream of saturated crystal-free mother liquid. The diluted product sample was then transported through the optical cells of the Malvern and HELOS device (stream 3). By using this dilution technique, the original product solid concentration (11 vol.%) was lowered to a solid concentration of approximately 1.5 vol.%, the maximum solid concentration which avoids multiple scattering and thus permits an accurate measurement using the laser diffraction measurement systems. The solid samples were taken at various moments in time from the product stream 2 as depicted in Figure 1. 2.2 Specifications of the Measurement Systems The OPUS system, manufactured by Sympatec, Germany, consists of an ultrasonic sensor, a measuring and evaluation unit and a computer system. A schematic drawing of the OPUS sensor is given in Figure 2. The

Fig. 2: Schematic drawing of the OPUS sensor.

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19 optical flow cell (window diameter 42 mm, pathlength 3.5 mm), also manufactured by Sympatec, was placed between the transmitting unit and the receiver unit. Each measurement lasted for 10 s with a time resolution of 100 ms and a background measurement was performed prior to each measurement. 2.3 Solid Sampling A total of 13 solid samples, marked by consecutive numbers in Figure 3, were taken at various moments in time. The dynamic trend of the median crystal size (L50), that is depicted in Figure 3, was measured using the Malvern instrument. This trend can typically be observed during the start-up phase of such crystallizer types and is attributed to a combination of relative low rates of attrition/secondary nucleation and an efficient dissolution of small crystals [9, 10]. The product samples were filtered on a Buchner filter using a blue band filter cloth and subsequently washed with pure ethanol. Each of the solid samples consisted of up to six individual samples taken consecutively at time intervals of 2 min. This procedure was chosen for the following reasons: (1) wet sieving analysis requires a fairly large amount (approximately 10 g) of crystalline material, and owing to experimental limitations (size of the filter), this amount cannot be obtained in a single filtration step; (2) one filtration step, consisting of taking a sample, filtration and washing of the sample with ethanol and discharging the filter, takes approximately 90 s. This time, in combination with the fact that no filtration step can be carried out during a measuring cycle of the Malvern and HELOS (every 2 min), results in a delay of about 2 min between each sampling step. The CSD of a solid sample is

measuring principle is based on measuring the extinction of ultrasonic waves (at a wide range of frequencies) propagating through the slurry that is pumped through the gap (width d) between the receiver and emitter unit of the sensor. In order to derive a CSD from the extinction measurements, an extinction function is required, which describes the interaction of the suspension with the sound waves as a function of the wavenumber s. This function cannot be calculated but has to be determined experimentally by an independent method of particle size analysis, generally laser diffraction. The manufacturer provides this function using solid samples of the crystalline material produced in the crystallizer. For the OPUS device the following settings were used: (1) the size range was set to 10 2500 mm using a set of 31 frequencies corresponding to 31 size classes; (2) the gap width d was set to 7 mm; (3) the boundaries specifying the part of the extinction function used were given by 0.015 < s < 100; (4) the CSD was determined from the average of 15 measuring cycles, i.e. the set of frequencies traversed the slurry 15 times (measurement time < 60 s); (5) a so-called background measurement (also averaged over 15 measuring cycles) of the crystal-free mother liquid was performed once at the start of the experiment and was subtracted from the later performed measurements. The Malvern measurement system consists of a Malvern 2600c laser diffraction instrument, which is linked to an Olivetti M24 PC on which a software package called ROMA is installed [8]. The diffraction instrument is equipped with a Fourier lens having a focal distance of 1000 mm. A custommade optical flow cell (window diameter 40 mm, pathlength 3 mm) through which the slurry to be measured is pumped is mounted between the transmitting unit (laser and beam expander) and the receiver unit (lens and detector). The measuring domain and the number of size classes used for discretization of the size domain, both of which can be set in the ROMA software, were 25.15 2515 mm and 20 size classes, respectively. Each measurement using this instrument consisted of 1000 sweeps (one sweep is one detector reading) with a read-out delay of approximately 10 ms. The average and standard deviation for each measurement were stored locally and transferred to the host computer. Then, the background measurement (1000 sweeps) of the crystal-free mother liquid, which was obtained prior to each measurement was subtracted. The HELOS measurement system consists of a HELOS/ VARIO laser diffraction instrument and a computer system, both manufactured by Sympatec, Germany. The diffraction device is equipped with a Fourier lens having a focal distance of 2000 mm and the corresponding measuring range is 18 3500 mm. Thirty-one size classes were used for discretization of the size domain. A similar

Fig. 3: Trend of L50 as function of time. Circled numbers mark the times at which solid samples are taken from stream 2.

20 therefore a combination of several individual samples (up to six) and therefore needs to be compared with about five or six measurements with the OPUS, HELOS and Malvern instrument. The solid samples were analyzed by wet sieving in 2-propanol by the Particle Characterization Group of Bayer, Leverkusen, Germany. For this purpose 10 sieves with apertures varying from 100 to 2000 mm were used.

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by each of the on-line devices during one solid sampling period is almost negligible, only one of the distributions is depicted for each measuring device. (2) For the on-line systems the trend in time of the measured quantities L10, L50 and L90 are compared. 3.1 Laser Diffraction Measurement Systems The size distributions measured by the laser diffraction measurement systems are depicted in Figure 4. The modal values of the distributions for both systems are in good agreement; however, the maximum values differ slightly, owing to small differences in the width of the peaks. In addition, deviations are visible with respect to the relative amplitude of the peaks in the bimodal distributions (Figure 4(b) and (c)) but a slight deviation in the upper size range is also visible in Figure 4(d). These differences become more apparent if the trends of the L10, L50 and L90 are compared (Figure 5). The median crystal size, L50, is in good mutual agreement, but L10 and L90 deviate, in particular L90. Nevertheless, both instru-

3 Results and Discussion

The results are presented in two ways. (1) From the large number of recorded measurements and samples taken, four different moments in time were selected (corresponding to numbers 2, 3, 6 and 13 in Figure 3). The corresponding size distributions obtained by the individual measurement systems are presented as volume percentage per ln(mm) (ordinate) vs. crystal size L (abscissa) on a logarithmic scale. According to Allen [11], this presentation is preferred for data manipulation. Since the difference between the distributions measured

Fig. 4: Laser diffraction measurement systems: (a) sample 2, (b) sample 3, (c) sample 6 and (d) sample 13.

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21 collecting lens might also have contributed to the observed deviation. Merkus et al. [3], Etzler and Sanderson [4], Etzler and Deanne [5] and Kaye et al. [6] published similar observations. They also performed comparative studies using various laser diffraction instruments and powders ranging in size up to 300 mm. They observed considerable variations in the calculated particle size between instruments from different manufacturers. These differences were attributed to differences in the physical instrumentation and the deconvolution algorithms. Wang and Shen [12] studied the influence of misalignment on the measuring results. They concluded on the basis of numerical calculations made for monodisperse particle systems that misalignment may have severe effects on the final results of the measurements.

3.2 Laser Diffraction vs. Ultrasonic Attenuation Comparison between the OPUS and HELOS results revealed that the OPUS gives a narrower distribution for the monomodal cases (Figure 6(a) and (d)). This narrowing of the distribution is also observed in the results of the sieve experiments (see the following sections). For the bimodal distributions that are shown in Figure 6(b) and (c), a clearer separation between the two peaks is also visible as opposed to the laser diffraction instrument. The same diagnosis is made if the L10, L50 and L90 trends are compared (Figure 7). Nevertheless, the overall trends in time for both systems are in mutual agreement. For the interpretation of the observed results, the following points should be taken into account: 1. The manufacturer has to calibrate the OPUS instrument against the HELOS instrument for each application. An empirical calibration procedure is used to determine the extinction function, which is needed to reconstruct the CSD from the attenuation measurements by off-line comparison between OPUS and HELOS CSD measurements using solid samples obtained from the crystallizer. Problems can easily arise when the samples used for calibration do not cover the whole size range that is of interest for the on-line measurements. In addition, changes in the shape, size and surface properties of the crystals induced by sampling, drying, transport and re-suspension steps in the calibration procedure can also induce large errors in the calibration procedure. 2. Low sensitivity of the OPUS instrument. This phenomenon is shown more clearly in Figure 8, where the trend of the volume fraction of crystals between 100

Fig. 5: Laser diffraction systems: L10, L50 and L90 as a function of time.

ments show the same overall trends in time. The observed differences may result from the following factors:

1. Different inversion methods: For the HELOS system the exact deconvolution algorithm used in the deduction of the size distribution data from the measured energy distribution of the diffraction pattern is not known, although it is assumed that some kind of Phillips-Twomey algorithm is used. The ROMA software uses a weighted non-negative least-squares method with an additional Phillips-Twomey smoothing (g 0.01). 2. Different transmitting and receiver units: The HELOS has a more modern detector, optical system and an automated focusing unit. Owing to the age of the Malvern instrument, possible misalignment of the optical system, drifting of the laser and/or flaws in the

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Fig. 6: Laser diffraction vs. ultrasonic spectroscopy: (a) sample 2, (b) sample 3, (c) sample 6 and (d) sample 13.

and 180 mm determined by the OPUS and HELOS system is plotted for this particular experiment. The comparison reveals that only above a certain threshold value does the amount of crystals fit that of the laser diffraction instrument. 3. Since the OPUS sensor is situated in the product loop, only one background measurement is performed at the start of the experiment. Possible changes in the composition of the crystal-free mother liquor or drift in the instrument or electronics may therefore also contribute to the observed differences. In the light of these possible error sources, the results for the OPUS instrument are remarkably good. However, the lower sensitivity of the instrument for small fractions is a limitation to the use of the instrument for on-line monitoring and control. Product specifications are often expressed in terms of small fractions below or above a certain size range. As shown above, the OPUS instrument seems not very suitable to determine such small fractions.

3.3 Laser Diffraction vs. Sieving Comparisons of the CSD obtained from the laser diffraction measurement systems and those from sieving reveal a difference in the modal value of the distributions; the distribution measured by wet sieving is in all cases shifted to smaller crystal sizes (Figure 9). Also, the width of the peaks is smaller, which is in line with the OPUS results; in the case of the bimodal distributions, however, the peaks are similarly resolved, as opposed to the OPUS. The observed differences between laser diffraction and sieving are related to the different physical principles employed by these techniques: 1. In order to pass the rectangular aperture of a sieve, the crystals need to have two dimensions smaller than the aperture (Figure 10). For non-spherical crystals the measured crystal diameter does not correspond to the equivalent volume diameter of a sphere. Thus the measured sieve diameter deviates from the sphere diameter that is measured by the laser diffraction

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23 sulfate crystals produced in the 1100-l DTB crystallizer is not cubic, as can be seen in Figure 11. The aspect ratio of the crystals, approximated by a tablet, in the direction of L1, L2 and L3 is about 1 : 0.7 : 1.2. Hence it is expected that the measured sieve diameter of the crystals will be smaller than the equivalent volume diameter. The above-mentioned aspect ratio is used to correct the sieve distribution for the shape of the crystals. Figure 12 shows the effect of this correction on the size distribution. The Figure clearly shows a better agreement of the distributions for the sieve and laser diffraction measurements after correction. However, the observed differences between the width of the peaks remain. In the case of laser diffraction, the broader distribution observed is explained by the smoothing effects that are introduced by the Phillips-Twomey inversion method. The remaining discrepancies are attributed: (1) to imperfections of the screen separation and of the sieve apertures, (2) to variations in crystal shape (the corners of larger crystal become more and more rounded-off in the course of the experiment) and (3) to some extent to the low number of sieve apertures used for discretization of the size domain. A sizedependent shape factor (aspect ratio) could further reduce the deviations. 2. The crystal size measured by the forward light scattering technique is related to the projected area of the crystals. For spherical crystals this projected area is independent of the orientation of the crystals in the laser beam. For non-spherical crystals, however, there is a dependence of the projected area on the orientation of the crystal, although the equivalent volume diameter does not change. The forward light scattering technique thus measures an average diameter over all dimensions of the crystal if a random orientation of the crystal in the laser beam is assumed. This brings about two consequences: (a) crystals of identical shape and size show a distribution in size; (b) crystal shapes, which differ strongly from a spherical shape, cause the appearance of tails in the volume distribution, either in the small crystal size classes (flakes or tablets) or in the large crystal size classes (elongated shapes). Another aspect to be considered is the fact that most commercial laser diffraction systems still mainly use a scatter matrix for spherical particles for reconstructing the size distribution from the measured diffraction pattern. Heffels et al. [14] showed that a large deviation can be expected for the crystal size distribution by volume, obtained with a scatter matrix for spherical particles in the case of flakes or elongated particles. For cubes the difference is negligible. Since the shape of ammonium sulfate crystals differs from a cube, the scattering matrix is

Fig. 7: Laser diffraction vs. ultrasonic spectroscopy: L10, L50 and L90 as function of time.

Fig. 8: Volume fraction of crystals in a certain size domain measured by the OPUS and HELOS system.

instruments. Crystals differing in shape (flakes, tablets and needles) but having the same equivalent mesh size will also show a distribution in equivalent volume diameters [13]. The shape of the ammonium

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Fig. 9: Laser diffraction vs. sieving: (a) sample 2, (b) sample 3, (c) sample 6 and (d) sample 13.

Fig. 10: Crystal passing through the aperture of the sieve.

array detector. The volume distribution is derived from the raw data of the Malvern instrument using the Phillips-Twomey inversion method with a smoothing factor g 0.01. As an alternative, the Chahine iterative scheme is used to reconstructed the CSD. No significant differences in the results between the two methods were found. The crystal size distribution by volume, obtained with a scatter matrix for spherical crystals and the distribution obtained with the scatter matrix for the correct crystal shape is depicted in Figure 13 for samples 2 and 3. The reconstructed size distribution for crystals and for spheres is almost identical, hence the shape effect on the measurements using the laser diffraction instruments can be neglected.

adapted to the shape of the crystals using the generalized Fraunhofer theory for arbitrary sharpedged particles. A detailed description of this method was given by Heffels et al. [14]. The shape of the ammonium sulfate crystals is once again approximated by a tablet with L1 L, L2 0.7 L and L3 1.2 L. The scatter matrices are calculated using the dimensions of the Malvern 2600c semi-ring photodiode-

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Fig. 11: SEM photographs of ammonium sulfate product crystals: (a) sample 3 and (b) sample 13.

Fig. 12: Laser diffraction vs. sieving with correction for shape of crystals: (a) sample 2 and (b) sample 3.

Fig. 13: Volume distribution calculated for spherical particles and for the actual crystal shape, which is approximated by a tablet, using laser diffraction: (a) sample 2 and (b) sample 3.

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4 Conclusions
A study has been presented in which several on-line CSD measurement systems were analyzed and compared with the classical wet sieving analysis technique. The two laser diffraction instruments deliver comparable results. They can be brought into reasonably good agreement with the wet sieving results when the latter are corrected for the shape of the crystals. The width of the distribution, however, remains broader in case of the laser diffraction results, which is due to smoothing effects introduced by the Phillips-Twomey inversion method. The deconvolution of the laser diffraction data appears not to be sensitive to the shape of the crystals, at least not for the plate-like crystals used in this study. The observed deviations between the two laser diffraction instruments are attributed to differences in the instrumentation and the deconvolution algorithms. Nevertheless, the observed trend of the quartiles (L10, L50, L90) is in good agreement. The size distributions obtained with the ultrasonic instrument appear to be less sensitive for crystal fractions with a low solid concentration. The calibration of the system appears to be of crucial importance. The overall trend in the quartiles (L10, L50, L90) is in good agreement with laser diffraction. As regards the CSD data required for model development and validation, it can be concluded that those obtained by laser diffraction are the most suitable. Regarding data acquisition, the laser diffraction technique employed in combination with the dilution technique, although suitable for the laboratory or pilot-plant scale, is not suitable for industrial applications. On the other hand, the acoustic instrument is robust and tolerant to the rigors of industrial environments, making the technique ideal for on-line (and with its latest release for in-line) applications in production processes. However, one has to realize that the lower sensitivity of the instrument for small fractions also forms a limitation for the use of the instrument for on-line monitoring and control since product specifications are often expressed in terms of small fractions below or above a certain size range.

6 Symbols and Abbreviations

CSD DTB HELOS L L10 L50 L90 OPUS s d g Crystal Size Distribution Draft Tube Baffle HElium-neon Laser Optical diffraction Spectrometer crystal size [mm] 10% quartile [mm] median of the crystal size distribution [mm] 90% quartile [mm] On-line Particle size analysis with UltraSonic extinction wavenumber [ ] gap width between emitter and receiver of the OPUS sensor [mm] smoothing factor or Lagrange factor [ ]

7 References
[1] R. A. Eek, A. Boxman, Sj. Dijkstra: Observability and Controllability of Industrial Crystallizers, in O. H. Bosgra, P. M. J. van den Hof (eds): Selected Topics in Identification Modelling and Control. Delft University Press, Delft 1992, pp. 47 54. [2] R. J. Farrell: Modeling Issues in Crystallization Processes. Proceedings of the International Symposium on Industrial Crystallization, Tokyo 1998, pp. 92 101. [3] H. G. Merkus, O. Bischof, S. Drescher, B. Scarlett: Precision and accuracy in particle sizing. Round-robin results from sedimentation, laser diffraction and electrical sensing zone using BCR 67 and 69. Proceedings of the 6th European Symposium on Particle Characterization, Nuernberg 1995. [4] F. M. Etzler, M. S. Sanderson: Particle size analysis: a comparative study of various methods. Part. Part. Syst. Charact. 12 (1995) 217 224. [5] F. M. Etzler, R. Deanne: Particle size analysis: Comparison of various methods II. Part. Part. Syst. Charact. 14 (1997) 278 282. [6] B. H. Kaye, D. Alliet, L. Switzer, C. Turbitt-Daoust: The effect of shape on intermethod correlation of techniques for characterizing the size distribution of powder. Part 1: Correlating the size distribution measured by sieving, image analysis, and diffractometer methods. Part. Part. Syst. Charact. 14 (1997) 219 224. [7] A. M. Neumann, S. B. Bermingham, H. J. M. Kramer, G. M. van Rosmalen: Modeling Industrial Crystallizers of Different Scale and Type. Presented at the 14th Symposium on Industrial Crystallization, Cambridge 1999. [8] A. Boxman: Ph.D. Thesis, Delft University of Technology, 1992. [9] R. O. Meadhra, H. J. M. Kramer, G. M. van Rosmalen: Model for secondary nucleation in a suspension crystallizer. AIChE J. 42 (1996) 973 982. [10] C. Gahn, A. Mersmann: Brittle fracture in crystallization processes, Part B. Growth of fragments and scale-up of suspension crystallizers. Chem. Eng. Sci. 54 (1999) 1283 1292. [11] T. Allen: Powder Sampling and Particle Size Measurement. Particle Size Measurement, Vol. 1, 5th ed. Chapman & Hall, London 1997.

5 Acknowledgements
The authors acknowledge Philippe Massard for finding the ins and outs of the OPUS system, Martin Wei for getting the solid samples analyzed and Ma Zhenhua for programming. Prof. Brian Scarlett is gratefully acknowledged for fruitful discussions and the Dutch Foundation of Technology (STW), Akzo Nobel, BASF, Bayer, Dow Chemicals, DSM, DuPont de Nemours and Purac Biochem for supporting the UNIAK III research program.

Part. Part. Syst. Charact. 19 (2002) 17 27 [12] N. Wang, J. Shen: A study of the influence of misalignment on measuring results for laser particle analyzers. Part. Part. Syst. Charact. 15 (1998) 122 126. [13] B. Scarlett: Characterization of Particles and Powders, in R. J. Brook (ed): Material Science and Technology, a Comprehensive Treatment. Vol. 17A, Processing of Ceramics, Part 1. VCH, Weinheim 1996.

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[14] C. M. G. Heffels, P. J. T. Verheijen, D. Heitzmann, B. Scarlett: Correction of the effect of particle shape on the size distribution measured with a laser diffraction instrument. Part. Part. Syst. Charact. 13 (1996) 271 279.