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Volatile Reaction Products From Silicon-Based Ceramics in Combustion Environments Identified

Silicon-based ceramics and composites are prime candidates for use as components in the hot sections of advanced aircraft engines. These materials must have long-term durability in the combustion environment. Because water vapor is always present as a major product of combustion in the engine environment, its effect on the durability of silicon-based ceramics must be understood. In combustion environments, silicon-based ceramics react with water vapor to form a surface silica (SiO2) scale. This SiO2 scale, in turn, has been found to react with water vapor to form volatile hydroxides. Studies to date have focused on how water vapor reacts with high-purity silicon carbide (SiC) and SiO2 in model combustion environments.

Because the combustion environment in advanced aircraft engines is expected to contain about 10-percent water vapor at 10-atm total pressure, the durability of SiC and SiO2 in gas mixtures containing 0.1- to 1-atm water vapor is of interest. The reactions of SiC and SiO2 with water vapor were monitored by measuring weight changes of sample coupons in a 0.5-atm water vapor/0.5-atm oxygen gas mixture with thermogravimetric analysis (ref. 1). SiC initially exhibited a weight gain due to SiO2 formation:

SiC(s) + 3H2O(g) = SiO2(s) + 3H2(g)+ CO(g)
(1)

At longer durations, a weight loss attributed to the volatility of SiO2 in water vapor became apparent:

SiO2(s) + 2H2O(g) = Si(OH)4(g)
(2)

SiO2(s) + H2O(g) = SiO(OH)2(g)
(3)

By testing SiO2 (rather than SiC) in water vapor, a linear weight loss uncomplicated by the oxidation reaction (1) can be observed by thermogravimetric analysis.

graph

Weight change kinetics for SiC and SiO 2 in 0.5 atm H 2 O/0.5 atm O 2 at a temperature of 1200 °C and a velocity of 4.4 cm/sec.

The identities of the volatile species were established by using a specialized mass spectrometer that samples reactions at 1-atm total pressure (ref. 2). SiO2 samples with large surface areas were exposed to water vapor/oxygen mixtures at high temperatures. Molecules with masses corresponding to both Si(OH)4 and SiO(OH)2 were identified.

Because SiO2 is volatile in combustion environments, it no longer provides protection for SiC. Consumption of SiC thus occurs at more rapid rates in water-vapor-containing environments. The consumption rate of SiC increases with water vapor pressure as well as gas velocity. This is a concern when SiC is applied in the high-pressure, high-velocity aircraft engine environment. Current efforts are focused on coatings for SiC that prevent volatility of the surface SiO2.

References

  1. Opila, E.J.; and Hann, R.E.: Paralinear Oxidation of CVD SiC in Water Vapor. To be published in J. Am. Ceram. Soc., vol. 80, no. 1, 1997.

  2. Opila, E.J.; Fox, D.S.; and Jacobson, N.S.: Mass Spectrometric Identification of Si-O-H(g) Species From the Reaction of Silica With Water Vapor at Atmospheric Pressure. Submitted to J. Am. Ceram. Soc.


Lewis contacts: Dr. Elizabeth J. Opila, (216) 433-8904, opila@grc.nasa.gov; Dr. Nathan Jacobson, (216) 433-5498, Nathan.J.Jacobson@grc.nasa.gov; and Dennis Fox, (216) 433-3295, Dennis.S.Fox@grc.nasa.gov
Author: Dr. Elizabeth J. Opila
Headquarters program office: OA
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Last updated May 5, 1997


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