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Thermal Decomposition Kinetics of Kerosene-Based Rocket Propellants

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Thermal Decomposition Kinetics of Kerosene-Based Rocket Propellants : Energy Fuels 2009, 23, 5523–5528 DOI:10.1021/ef900577k Published on Web 09/09/2009 Thermal Decomposition Kinetics of Kerosene-Based Rocket Propellants. 2. RP-2 with Three Additives† Jason A. Widegren and Thomas J. Bruno* Thermophysical Properties Division, National Institute of Standards and Technology, 325 Broadway, Boulder, Colorado 80305-3328 Received June 5, 2009. Revised Manuscript Received August 12, 2009 The thermal decomposition of RP-2 with three potential stabilizing additives was investigated. The additives were 1,2,3,4-tetrahydroquinoline (THQ), 1,2,3,4-tetrahydronaphthalene (tetralin), and the additive package that is used to make JP-8 þ 100 (herein referred to as the “þ100 additive”). For mixtures of RP-2 with THQ and tetralin, the concentration of additive was 5% by mass. The mixture of RP-2 with the þ100 additive contained only 256 mg/L of the additive (the same concentration used to make JP-8þ100). Decomposition reactions were performed at 375, 400, 425, and 450 °C in stainless steel reactors. At each temperature, the extent of decomposition as a function of time was determined by analyzing the thermally stressed liquid phase by gas chromatography. The results with each additive were compared to the decomposition of neat RP-2 under the same conditions. The addition of 5% THQ slowed the rate of decomposition by approximately an order of magnitude. The addition of 5% tetralin slowed the rate of decomposition by approximately 50%. At the low concentration tested, the þ100 additive did not significantly change the thermal stability of the RP-2. Introduction parameter for specifying its performance.1,2 The thermal stability of the kerosene-based rocket propellant RP-1 has Kerosene-based rocket propellant serves the dual roles - been studied extensively.1 7 The thermal stability of a rela- of fuel and coolant in modern rocket engines.1,2 Prior to tively new rocket propellant, RP-2, has been the subject combustion, the rocket propellant circulates through cha- of fewer studies.3,7,8 The specification for RP-2, along nnels in the wall of the thrust chamber. Thus, the fuel carries with an updated specification for RP-1, was published in heat away from the wall and maintains a safe wall tempera- 2005 as MTL-DTL-25576D. The primary differences between ture. This process, commonly referred to as regenerative the specifications for RP-1 and RP-2 are that the allowed cooling, exposes the fuel to high temperatures. For this sulfur content is much lower in RP-2 (0.1 mg/kg, compared reason, the thermal stability of the fuel is a key design to 30 mg/kg in RP-1), the allowed olefin concentration of is lower in RP-2 (1 vol %, compared to 2 vol % for RP-1), † Contribution of the United States government; not subject to copyright in and the use of the red dye is currently not allowed in RP-2. All the United States. three of these differences were intended to increase the thermal *To whom correspondence should be addressed. Tel.: (303) 497-5158. stability of RP-2. Fax: (303) 497-5927. E-mail: [email protected]. (1) Edwards, T. Liquid fuels and propellants for aerospace propul- A potential approach for further improvements in the sion: 1903-2003. J. Propul. Power 2003, 19, 1089–1107. thermal stability of RP-2 is to use stabilizing additives. (2) Irvine, S. A.; Schoettmer, A. K.; Bates, R. W.; Meyer, M. L. The use of additives has a long history with kerosene-based History of sulfur content effects on the thermal stability of RP-1 under 1,9 heated conditions. 40th AIAA/ASME/SAE/ASEE Joint Propulsion jet fuels. Much of the work on jet fuels has focused on Conference & Exhibit, Fort Lauderdale, FL, July 11-14, 2004; AIAA Paper additives that are “hydrogen donors”, such as 1,2,3,4-tetra- 2004-3879. hydroquinoline (THQ),10-13 1,2,3,4-tetrahydronaphthalene (3) Brown, S. P.; Frederick, R. A. Laboratory-scale thermal stability experiments on RP-1 and RP-2. J. Propul. Power 2008, 24, 206–212. (4) Wohlwend, K.; Maurice, L. Q.; Edwards, T.; Striebich, R. C.; (8) Widegren, J. A.; Bruno, T. J. Thermal Decomposition Kinetics of Vangsness, M.; Hill, A. S. Thermal stability of energetic hydrocarbon Kerosene-based Rocket Propellants. 1. Comparison of RP-1 and RP-2. fuels for use in combined cycle engines. J. Propul. Power 2001, 17, 1258– Energy Fuels, submitted for publication. 1262. (9) Coleman, M. M.; Schobert, H. H.; Song, C. S. A New Generation (5) Bates, R. W.; Edwards, T.; Meyer, M. L. Heat Transfer of Jet Fuels. Chem. Br. 1993, 29, 760–762. and Deposition Behavior of Hydrocarbon Rocket Fuels. 41st Aero- (10) Yoon, E. M.; Selvaraj, L.; Song, C. S.; Stallman, J. B.; Coleman, space Sciences Meeting and Exhibit, Reno, NV, 2003; AIAA Paper 2003- M. M. High-temperature stabilizers for jet fuels and similar hydrocar- 123. bon mixtures. 1. Comparative studies of hydrogen donors. Energy Fuels (6) Stiegemeier, B.; Meyer, M. L.; Taghavi, R. A. Thermal Stability 1996, 10, 806–811. and Heat Transfer Investigation of Five Hydrocarbon Fuels: JP-7, (11) Yoon, E. M.; Selvaraj, L.; Eser, S.; Coleman, M. M. High- JP-8, JP-8þ100, JP-10, RP-1. 38th AIAA/ASME/SAE/ASEE Joint temperature stabilizers for jet fuels and similar hydrocarbon mixtures. Propulsion Conference & Exhibit, Indianapolis, IN, 2002; AIAA Paper 2. Kinetic studies. Energy Fuels 1996, 10, 812–815. 2002-3873. (12) Coleman, M. M.; Selvaraj, L.; Sobkowiak, M.; Yoon, E. Poten- (7) MacDonald, M. E.; Davidson, D. F.; Hanson, R. K. Decom- tial Stabilizers for Jet Fuels Subjected to Thermal Stress above 400 °C. position Rate Measurements of RP-1, RP-2, n-Dodecane, and Energy Fuels 1992, 6, 535–539. RP-1 with Fuel Stabilizers. 44th AIAA/ASME/SAE/ASEE Joint (13) Corporan, E.; Minus, D. K. Assessment of radical stabilizing Propulsion Conference & Exhibit, Hartford, CT, July 21-23, 2008; AIAA additives for JP-8 fuel. 34th AIAA/ASME/SAE/ASEE Joint Propulsion Paper 2008-4766. Conference & Exhibit, Cleveland, OH, July 13-15, 1998; AIAA Paper 98-3996. This article not subject to U.S. Copyright. Published 2009 by the American Chemical Society 5523 pubs.acs.org/EF : Energy Fuels 2009, 23, 5523–5528 DOI:10.1021/ef900577k Widegren and Bruno (tetralin),10,12-18 decahydronaphthalene (decalin),13,17,18 and benzyl alcohol.12,13,19-21 In related work, a major research effort initiated by the U.S. Air Force culminated in the formulation of the stabilizing additive package used to make JP-8 þ 100 (herein referred to as the “þ100 additive”). The þ100 additive contains three components: an antioxidant (hydrogen donor), a metal deactivator, and a dispersant (surfactant).1 The use of such stabilizing additives has been suggested2 for rocket propellants, but little work has been done.1,7 The goal of this study is to extend the work on jet fuel stabilizers to find an additive that will significantly improve the thermal stability of RP-2. Herein, we report the thermal decomposition of RP-2 with three potential stabilizing addi- Figure 1. Apparatus used to thermally stress and decompose RP-1 tives: THQ, tetralin, and the þ100 additive. We observed and RP-2. changes in thermal stability by monitoring the formation of light, liquid-phase decomposition products in the thermally Apparatus. The apparatus used for the decomposition reac- stressed fuel. Decomposition reactions were performed at 375, tions is shown in Figure 1. Two thermostatted blocks of 304 ° stainless steel (AISI designation) were used to control the 400, 425, and 450 C in stainless steel ampule reactors. At each reaction temperature. Each block was supported in the center temperature, the extent of decomposition as a function of time of an insulated box on carbon rods, which were chosen for their was determined by analyzing the thermally stressed liquid low thermal conductivity. A proportional-integral-derivative phase by gas chromatography. In addition to this quantitative (PID) controller used feedback from a platinum resistance assessment of thermal stability, we also made qualitative thermometer to maintain the temperature within 1 °C of the observations about the color of the thermally stressed fuel set value. As many as six stainless steel ampule reactors could be and the formation of a pressurized vapor phase in the sealed placed into tight-fitting holes in each of the two thermostatted reactors. blocks. Each reactor consisted of a tubular cell with a high- pressure valve. Each cell was made from a 5.6 cm length of Experimental Section ultrahigh-pressure 316 L stainless steel tubing (0.64 cm external diameter and 0.16 cm internal diameter) that was sealed on one Chemicals. Reagent-grade acetone, toluene, and dodecane end with a 316 L stainless steel plug welded by a clean tungsten- were used as solvents in this work. They were obtained from inert-gas (TIG) process. The other end of each cell was con- commercial sources and used as received. All had stated nected to a valve with a 3.5 cm length of narrow-diameter purities of no less than 99%, which is consistent with our 316 stainless steel tubing (0.16 cm external diameter and own routine analyses of such solvents by gas chromatography. 0.08 cm internal diameter) that was TIG-welded to the larger The THQ (98% purity) and tetralin (99.5% purity) were diameter tube. The valves were appropriate for high tempera- also obtained from commercial sources and used as received. ture in that the seats were stainless steel, and the packings were The þ100 additive was obtained from the Fuels Branch of flexible graphite.
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