A single-pellet, moment technique is presented for evaluating reaction rate constants, effective diffusivities, and adsorption equilibrium constants for gas-solid noncatalytic reactions. Experimental pulseresponse data for the reaction of SO, with activated soda at 473 K were obtained to illustrate the method. The results show that intraparticle diffusion is the controlling mechanism for this reaction. The value of the Thiele modulus for axial transport was found to be 8.6 for a cylindrical pellet of porosity 0.56, tortuosity 2.3, and length 3 x lo-' m.
SCOPEEffective diffusivities of reactant and products, adsorption equilibrium and reaction rate constants are essential for the design of fluid-solid, noncatalytic reactors. The single-pellet, moment technique has been shown to be a valuable tool for evaluating effective diffusivities and adsorption parameters in porous solids Smith, 1975, 1976). One of the objectives of this work was to extend the application of the technique to reaction systems. The experimental procedure consists of introducing a pulse of reactive gas to one end face of a porous, cylindrical pellet of solid reactant and measuring the concentration vs. time re-sponse peak leaving the other end face. Moments of these response peaks are then equated with model equations for the moments in order to evaluate the rate and equilibrium parameters.A gas-solid reaction that also has some potential for removal of SO, from flue gases is the SO,-sodium carbonate system. When sodium bicarbonate is heated to about 473 K, a porous activated soda is produced that reacts rapidly with SO, (Marecek et al., 1970;T. Dogu, 1984). Pulse-response data were measured for this system to illustrate the method and to obtain values for reaction rate and diffusion parameters.
CONCLUSIONS AND SIGNIFICANCEThis work has demonstrated that gas-solid reaction rate constants together with effective diffusivities and adsorption equilibrium constants of reactant and products can be determined by the single-pellet, moment technique. Such results were obtained for the gas-solid reaction of SO, with activated soda at 473 K. The value of the Thiele modulus, determined from the first moment of the response curve of the product gas (CO,), was 8.6 for a pellet of porosity 0.56 and length 3 x lo-' m. The tortuosity factor of the pellet evaluated from inert tracer runs was 2.3. The adsorption equilibrium constant and effective diffusivity of CO, (in helium) were p,K, = 0.14 and D, = 0.22 x The effective diffusivity of the reactant gas (SO,) rn'ls.was evaluated from the ratio of zeroth moment of the product (CO,) response, in the reaction runs and the CO, response for the adsorption runs. The result, D," = 0.23 x m2/s, is larger than expected for pore-volume diffusion. Assuming that the discrepancy is due to surface diffusion of SO,, this mechanism could contribute about 20% to the total diffusive flux in the pellet.By carrying out the pulse-response experiments for two pellets of different lengths but with the same porosity, dead volume effect...