In order to model the complex hydrodynamic phenomena prevailing in industrial scale gas-solid bubbling fluidised bed reactors and especially the macro-scale emulsion phase circulation patterns induced by bubble-bubble interactions and bubble coalescence, a discrete bubble model (DBM) has been developed. In the DBM, the (larger) bubbles are modelled as discrete elements and are tracked individually during their rise through the emulsion phase, which is considered as a continuum. The DBM, originally developed for the description of gas-liquid flows, has been adapted to cope with bubbles with a diameter larger than the size of an Eulerian cell, which is required in view of the large bubble size distribution at higher gas flow rates. Moreover, a new drag model for a single bubble rising in a fluidised bed derived from empirical correlations has been implemented, as well as a simple model to account for bubble coalescence and break-up. The strong advantage of the DBM compared to other models previously reported in the literature for the description of large-scale fluidised beds is that it fully accounts for the two-way coupling between the bubbles and the emulsion phase, which enables direct computation of the emulsion phase velocity profiles. Comparison of the results of simulations ignoring bubble coalescence and simulations taking bubble coalescence properly into account demonstrated the significant effect of bubble coalescence on the large-scale circulation patterns prevailing in bubbling fluidised beds. The simulation results for the lateral profiles of the visible bubble flow rate have been compared qualitatively with experimental results reported by Werther [1974. Influence of the bed diameter on the hydrodynamics of gas fluidized beds. A.I.Ch.E. Symposium Series 70(141), [53][54][55][56][57][58][59][60][61][62]. The effect of the superficial gas velocity on the velocity and porosity profiles has been studied. In general, it can be concluded that the DBM is able to capture the salient features of the hydrodynamics of bubbling fluidised beds. However, further research is required to improve the closure equations for the bubble behaviour, bubble-bubble interactions and bubble coalescence and break-up to enable a complete quantitative description. ᭧

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A small laboratory-scale membrane-assisted fluidized bed reactor (MAFBR) was constructed in order to experimentally demonstrate the reactor concept for the partial oxidation of methanol to formaldehyde. Methanol conversion and product selectivities were measured at various overall fluidization velocities, reactor temperatures, methanol and oxygen overall feed concentrations, ratios of gas fed via membranes relative to gas fed via the bottom distributor, and aspect ratios of the fluidized bed. High methanol conversions and high selectivities to formaldehyde were achieved with safe reactor operation (isothermal reactor conditions) at very high methanol inlet concentrations, much higher than currently employed in industrial processes. It was experimentally demonstrated that with distributive feeding of oxygen in a MAFBR the overall formaldehyde yield and throughput could be increased without a pronounced and undesirable conversion of formaldehyde to carbon monoxide. Furthermore, a one-dimensional two-phase phenomenological reactor model has been developed with which the experimentally observed conversion and selectivity as a function of the operating conditions could be well described.

A small laboratory-scale membrane-assisted fluidized bed reactor (MAFBR) was constructed in order to experimentally demonstrate the benefits of this reactor concept, especially the enhanced bubble-to-emulsion phase mass transfer and the reduced overall axial gas phase back-mixing, due to the presence of the membranes and permeation of gas through the membranes. With steady-state tracer gas injection experiments, it was demonstrated that the experimental reactor exhibited approximately plug flow behavior for all the operating conditions investigated in this work as a result of the elimination of macroscale circulation patterns due to the presence of the membranes and, even more importantly, the permeation of gas through the membranes. With an ultrasound technique, the gas residence time distribution (RTD) of the MAFBR was measured over a wide range of fluidization velocities for two different bed heights. Interpretation of the RTD measurements with a phenomenological two-phase reactor model extending the bubble assemblage model proposed by Kato and Wen (Kato, K.; Wen, C. Chem. Eng. Sci. 1969, 24, 1351 showed that the average bubble diameter is significantly decreased for higher ratios of gas permeated through the membranes relative to the total gas flow rate.