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EXPERIMENTAL STUDIES OF NUCLEATION PHENOMENA WITHIN THERMAL BOUNDARY LAYERS—INFLUENCE ON CHEMICAL VAPOR DEPOSITION RATE PROCESSES
Authors:Baishen Liang  Alessandro Gomez  Jose L Castillo  Daniel E Rosner
Affiliation:  a Yale University, Chemical Engineering Department, High Temperature Chemical Reaction Engineering Laboratory, New Haven, CT
Abstract:In carrying out partial vapor condensations using actively cooled surfaces it is known that 'mist' formation can occur within thermal boundary layers (Rosner and Epstein, 1968), dramatically modifying total deposition fluxes. Using a combination of flash-evaporation (Rosner and Liang, 1986) and laser probing techniques, we report new experimental results on binary alkali salt (K2SO4 + Na2SO4) deposition from combustion gases showing that the deposition rate of potassium sulfate first increases with the addition of sodium sulfate until the concentration of Na2SO4 reaches a (target surface temperature dependent) 'threshold' value. Further increases in the concentration of Na2SO4 dramatically decrease the total deposition rate of K2SO4, implying that potassium sulfate-containing microdroplets are formed within the thermal boundary layer, which, despite their thermophoretic drift toward the target, are not collected as effectively as the 'parent' K2SO4-vapor species. Laser light scattering measurements clearly reveal that suspended particles exist near the deposition surface under these conditions. Our experimental results on mass transfer rate and light scattering are consistent with those predicted using laminar boundary layer theory (Castillo and Rosner, 1989b) coupling both binary salt vapor deposition with particle vapor scavenging and deposition. Comparisons of our observed mist onset conditions (implying critical supersaturations near unity) with those expected using homogeneous nucleation theory suggest that the binary alkali sulfate mist nucleation mechanism is, instead, heterogeneous, even in our relatively 'clean' combustion products. Because of the; well-known vapor pressure reduction phenomenon associated here with the formation of non-ideal solutions, binary systems are shown to provide convenient 'vehicles' to investigate BL mist formation onset conditions and CVD-rate consequences without requiring the more extreme surface coolings characteristic of unary condensible vapor systems. An understanding of this dramatic phenomenon, obtained via such laboratory experiments and calculations, will allow its inclusion in future deposition rate calculations of engineering importance.
Keywords:Condensation  Nucleation  Vapor deposition  Convective mass  transfer  Alkali salts  Thermophoresis
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