Development of a membrane-assisted fluidized bed reactor. 2. Experimental demonstration and modeling for the partial oxidation of methanol

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.