Journal of Materials Science, Vol.31, No.11, 3021-3033, 1996
The Influence of Surface Kinetics in Modeling Chemical-Vapor-Deposition Processes in Porous Preforms
The isothermal chemical vapour infiltration (ICVI) process is a well known technique for the production of composites and the surface modification of porous preforms. Mathematical modelling of the process can provide a better understanding of the influence of individual process parameters on the deposition characteristics such as final porosity or deposition profiles in the pore network. The influence of different rate expressions for several binary compounds on the ICVI process is discussed. Experimental work is used to validate the importance of correct kinetic expressions in a continuous ICVI model for cylindrical pores. The predicted infiltration characteristics are compared with experimental results. The final densification and Thiele modulus, i.e. a number which is a measure for the diffusion limitations in a pore, are used for the evaluation of the presented model, and conditions are given for an optimal densification of a porous preform by the ICVI process for several binary compounds. The deposition profiles as predicted by the model calculations are in agreement with the experimentally determined deposition profiles of TIN and TiC in small tubes. Moreover, it can be concluded that the shape of the deposition profiles is determined by the heterogeneous reaction kinetics. There is only a qualitative agreement between the predicted densification and measured densification for the synthesis of TiN and TiB2 in sintered porous alumina. This mismatch can be explained in terms of a complexity of the pore network and differences in reaction kinetics. Model calculations reveal that there is a scattering for the predicted residual porosity as a function of the Thiele modulus for TIN. Moreover, this Thiele modulus can not fully account for the changes in densification at different temperatures. Given these uncertainties it is likely that a residual porosity of less than one percent can be obtained if the Thiele modulus is smaller than 1 x 10(-4). However, a CVI process with such a small Thiele modulus will not be practical, because of the concomitant long process times. Therefore, more precise conditions for the individual process parameters, i.e. concentration, reactor pressure, and temperature are deduced from the model calculations.
Keywords:CERAMIC MATERIALS;HIGH-TEMPERATURE;GAS-PHASE;INFILTRATION;COMPOSITES;CVD;DIFFUSION;SILICON;DENSIFICATION;PRESSURE