ࡱ> uwpqrst'` hbjbj"9"9 .j@S@SC~ ' ' ' '4>'<g5''''''''4444444$6h849(''((4''!5+++(''4+(4++VN3@4'z' ʊҀ 'K**3 4750g53xC9u+dC94C94'>',+'$('''44+ '''g5((((DF&F&z TOWARD THE UNIFICATION OF COMBUSTION NEW VERSION ABSTRACT The same overall kinetic expression has been found to hold for both premixed and diffusion ignitions, within the estimated maximum error, in the hot gas ignition system. This is so, even though diffusion ignitions are a few hundred degrees C below those of premixed. The criterion of ignition occurs when the enthalpy derivative with respect to radius turns positive. For premixed ignitions, this corresponds to a positive temperature derivative. An overall kinetic expression can describe flame spreading, the presence of a cold wall, total combustion, unusual glows, and probably, cool flames as well. This represents a step toward unifying combustion, which may have an impact on mechanism studies. A single overall kinetic expression has been found adequate to describe both premixed and diffusion ignitions using a hot gas as the ignition source1,2,3. The rate expression for ignition is of the form wf = AMfe-E/RTCfCoD = AMfe-E/RT(P/RT)(C+D)YfCYOD (1) where A = frequency factor Cf = molar fuel concentration Co = molar oxygen concentration C = fuel power C + D = total order of reaction D = oxygen power E = activation energy Mf = molecular weight of fuel P = total pressure R = gas constant T = absolute temperature (K) Wf = fuel mass rate of production (gm/cc sec) Yf = fuel mole fraction and Yo = oxygen mole fraction For premixed experiments, the hot gas (centered in a mixing chamber for vertical flow, as shown in Figure 1) used was nitrogen and the nearly stagnant peripheral gas was a fuel-air mixture; for diffusion experiments, the hot gas used was air with 21% oxygen and the nearly stagnant peripheral gas was pure fuel.  The centered, inner gas was heated by a ceramic tube furnace (which was wound with platinum wire) before entering the mixing chamber. An annular water jacket around the top of the furnace kept the fuel cold, thereby preventing cracking. Ignition was approached by regulating the ceramic tube furnace power with a transformer. Altogether five furnaces of differing inside tube diameters were used. An exhaust system was constructed to fit above the mixing chamber to remove all gases flowing inside. The fuels studied were methane, ethane, and ethylene. Concentration ranged from 0.8 to 1.5 stoichiometric. Reynolds numbers of the hot gas were in the order of 200, indicating boundary layer flow coming out of the ceramic furnace. Studying hydrogen as a fuel would probably work, but would have to be done extra carefully to prevent an explosion in and above the mixing chamber. Therefore, one could start with very lean, premixed conditions and gradually work into rich, premixed and diffusion ignitions. The principal measurements in an ignition experiment are the ignition temperature (measured at the base of the hot gas jet to the mixing chamber with a horizontal, platinum 10% rhodium thermocouple coated with silica), ignition distance (determined with high-speed movies of the flame spreading through an observation window), hot gas velocity, and concentrations (using rotameters). The horizontal thermocouple wire ran through a ceramic holder in the mixing chamber. Outside the chamber, a stainless steel jacket surrounded the ceramic holder. An o ring was used to bolt the stainless steel jacket to the chamber to prevent leakage. Two penlight beams were shined through the mixing chamber and were filmed by the movie camera to serve as a frame of reference in determining ignition distance in the free gas stream. To obtain the ignition temperature, the horizontal thermocouple was connected to a potentiometer using appropriate extension wire. Ignition temperatures were corrected for radiation, based on intermediate heat transfer to a sphere and a cylinder6. This correction is presented in Figure 2.  The partial differential equations describing the blending of hot and cold gases with reaction in cylindrical coordinates was solved numerically by Goh and Ma5 (working under Spalding8). Their computer program was modified considerably to fit the experimental data. (Part of the modification was to all heat capacity, viscosity, thermal conductivity, and diffusivity to vary with temperature and, when appropriate, with composition). The criterion of ignition of the program for both diffusion and premixed flames in cylindrical coordinates is dH/dr = + (2) where H is the total enthalpy. (Actually, the program used stagnation enthalpy, enthalpy plus kinetic energy, for this criterion. For practical purposes, the kinetic term is negligible.) The heat of reaction was taken to be that of complete fuel combustion to carbon dioxide and water vapor. In the case of premixed ignitions, dT/dr = +. (3) For computer premixed ignitions, both the enthalpy and the temperature derivatives were positive at the same ignition distance. This temperature derivative is a form of the familiar Semenov equation. [In a derivation of this equation by Glassman4, dT/dt goes positive in a batch (non-flow) reactor. This occurs at time, t, when the energy of reaction becomes greater than the heat loss.] Obviously, then, changes in enthalpy with radius involve concentrations more-so in diffusion ignitions than in those of premixed. This is in contrast to previous kinetic mechanism theory about diffusion ignition being controlled by free radicals, rather than simply enthalpy changes. Therefore, with the same overall kinetics explaining both premixed and diffusion phenomena, there might be some rethinking about the kinetic mechanism similarities. The sign changes in equations (2) and (3) first occur at a distance above the jet base of the heated tube to the mixing chamber. More generally, the derivatives in these two equations should be partials. In order to verify the computer program, mixing experiments were performed under conditions of no reaction. Radial temperature and concentration profiles were obtained experimentally around 10 cm above the jet base in the mixing chamber. To obtain these profiles, a traversing mechanism mounted at the top of the chamber was used to hold a thermocouple connected to a potentiometer and a quartz probe with a throat diameter of around 75 microns. A water jacket was used to keep the thermocouple and quartz probe vertical in the mixing chamber. Bottled gas samples obtained through the quartz probe and tygon tubing were analyzed on the gas chromatograph. All work was done at atmospheric pressure. For ignition experiments in the free gas stream, the traversing mechanism was removed from the mixing chamber. The principal computer variable turned out to be the initial computer profiles of temperature, fuel concentration, and oxygen concentration. Theoretical studies5,7 have used a very thin initial mixing zone between the hot and cold gases. Experiments here indicated a broader initial mixing zone. An excellent fit was achieved with a ramp function for the initial computer profiles of concentrations and temperature. This ramp starts with the hot gas extending to the inside furnace radius and ends with the cold gas at the inside furnace radius. With so many computer and experimental variables, the problem of correlating results was encountered. It was found that for premixed ignitions, a plot of Log (ucl/z) + (C + D) log (T/P) vs. 1/T (4) where ucl = center line velocity (cm/sec) and z = Ignition distance (cm), at constant concentration, yielded a straight line for both computations and experimentation with a slope of E/R. The total order, (C + D), was taken from combustion literature, particularly shock tube results.2 Values of A were computed using the reaction rate given in equation (1) to fit experimental ignition data. Equation (4) was derived using a plug flow model (one-dimensional flow in a tube). In this model, ignition takes place within the tube. (It is not feasible to run experiments like this. For one thing, the fuel would crack at high temperatures; for another, the heated fuel-air would be subject to explosion.) The center line velocity, ucl, was calculated to be 1.71 times the average velocity. This calculation was made to correspond to flat initial temperature profiles used experimentally. Center line velocities for the five furnaces used in this study range from 430 to 3700 cm/sec. The fuel power, C, was computer to be slightly positive for lean mixtures and negative for rich mixtures. Since the effect of concentration of premixed ignitions is small, an overall fit was obtained using C = 0 for stoichiometric mixtures. Values of the frequency factor constant, A/R(C+D), are given in Table I. These values were then used to determine ignition distances for diffusion flames. TABLE I COMPUTED KINETIC PARAMETERS (Premixed Stoichiometric Fit) Fuel Methane Ethane Ethylene Molecular Weight, Mf 16.04 30.07 28.05 Total Order (C + D) 1.1 1.7 1.8 Frequency Factor Constant 2.9 x 107 4.7 x 1010 1.4 x 1010 A/R(C+D) Activation Energy, E 50,430 44,930 41,460 Fuel Power, C 0 0 0 Premixed Temp. Range, K 1650-1850 1160-1400 1140-1420 Maximum Error in A 3.3 3.1 3.2 The maximum error factor in A (to be either multiplied or divided) was estimated from possible errors in measurements, estimations and even computations, all multiplied together. The ignition distance error, for instance, was estimated using 95% confidence limits on a series of ten repeated ethylene stoichiometric ignitions using a movie camera. It should be mentioned that the maximum error in A is expected to be much greater than any actual one. Actual error may even be below 10% total, as indicated in the consistency of the results, such as having the stoichiometric concentrations with the strongest ignition strength (see Figure 4 below). The fit of methane mixing data under mixing conditions with no chemical reaction is shown in Figure 3. The initial temperature and concentration computer profiles were taken to be ramp functions, as discussed above.  The overall kinetics are still valid in the presence of a cold wall. In fact, a water jacket perpendicular to the vertical hot gas flow can be used to determine the ignition distance with considerable accuracy. As a result of this, future overall kinetic studies can be carried out quite easily using only one furnace with a water jacket to measure ignition distance. The data for premixed ethane ignitions, both in free gas stream and using the vertical water jacket, is given in Table II. This data is plotted in Figure 4 using the relationship given in Equation 4 with a log to the base 10. As calculated from the slope of the lines, the activation energy is 44,930, the same value given in Table I. Also, the results from ethane experiments using the vertical water jacket as a cold wall lines up perfectly with those taken in the free gas stream. Similar results were obtained for methane and ethylene. TABLE II ETHANE PREMIXED DATA In the Free Gas Stream Mole Frac- Fur- T T ucl z 104/T log ucl/z + % in tion nace (C+D) log(T/P) Air Stoich. # C cm/sec cm K 5.67 1.0 1 860.3 29.8 447 21.77 8.60 6.523 6.71 1.2 1 863.4 30.4 448 21.77 8.57 6.527 8.27 1.5 1 865.6 30.9 449 24.47 8.55 6.480 5.13 0.9 1 871.8 31.3 452 27.47 8.55 6.433 5.67 1.0 4 1044.3 39.2 2780 11.57 7.37 7.695 6.71 1.2 4 1059.6 40.8 2815 11.73 7.28 7.715 8.27 1.5 4 1079.3 43.9 2860 15.47 7.17 7.613 5.67 1.0 2 918.6 35.1 592 10.42 8.15 7.005 6.71 1.2 2 927.6 36.0 597 11.43 8.08 6.975 Using the Vertical Water Jacket 5.67 1.0 1 941.5 41.6 483 6.61 7.96 7.131 5.67 1.0 1 912.3 36.8 469 9.47 8.18 6.943 5.67 1.0 1 897.1 35.0 463 12.03 8.29 6.824  Diffusion ignitions were checked by computations using the maximum error factor in A (3.3 for methane, as listed in Table I). The computed results for methane using the Equation 4 relationship were somewhat curved. This is to be expected, as ignition for diffusion flames occurs somewhat away from the center line. Figure 5 was obtained using an Apple IIE Pc. Since the original computations for one ignition point would take so long on a PC (over 40 hours estimated), the iterations were cut by a factor of 25. This had the effect of lengthening the ignition distances. A temperature correction curve for this PC iteration discrepancy is given in Figure 5. This correction is still within the maximum error envelope, which is, most likely, much larger than any actual one (discussed above).  Computations indicate that premixed ignitions occur at high temperatures and low fuel and oxygen concentrations, whereas diffusion ignitions occur at low temperatures and high fuel concentrations. In general, the distances for premixed ignitions for a given furnace rose as the flammability limits were approached and the flames formed after ignition were less uniform. The hot gas jet broke down experimentally at a certain distance above the jet base (somewhat over 25 cm using the largest furnace (#1), with an inside tube diameter of 5/8 inch. This breakdown therefore explains the flammability limits in the hot gas system. If the gases are left on following ignition in the premixed case, the flame settles on glass beads at the base of the mixing chamber. In the diffusion case, the flame spreads after igniting and goes out before reaching the glass beads. Then, it ignites at the same place it did before and keeps repeating the same sequence. This unusual phenomena occurs because the flame can only spread within the flammability limits of the fuel. In a theoretical work, Marble and Adamson7 used a simple overall kinetic expression to study ignition and the post-ignition zone. Since the computations discussed here also predict flame spreading, which followed ignition experimentally, it is believed that the overall kinetic parameters (given in Table I) will hold for combustion as well. (In other words, flame spreading can be thought of as a continuous, moving ignition.) Modifications might have to be made for the accumulation of stable combustion productsnamely, carbon dioxide and water vapor. Unusual combustion phenomena, such as pre-ignition glows and probably, cool flames, could also be taken into accounts with an overall kinetic model. What makes these phenomena unusual is the way that fuel and oxygen (or air) flow through the reactor, and the way that temperatures, concentrations, reactor geometry, and total pressure vary. In this hot gas system, premixed ethane and ethylene exhibit glows within a few degrees of their ignition temperature. Because the overall kinetics appear to be able to account for ignition, flame spreading, combustion, unusual glows, and, probably, cool flames, it appears that the mechanism of combustion [or, at least, the rate determining step(s)] must be the same for all these situations, even in the presence of a cold wall. This represents a unification of combustion. It may even extend to other gaseous reactions besides combustions, and possibly into other solids and liquids as well. One way of studying the mechanism is by taking the spectra of pre-ignition glows in the hot gas system, which is very stable for this purposeon the order of hours, if necessary. With some seriously expected difficulties, the computer program used here could be revised to account for a mechanism of ignition. REFERENCES 1. Fink, Zachary and Marcel Vanpee, Overall Kinetics of Hot Gas Ignition, Combustion Science and Technology, 11, 1975, 229-38 Fink, Zachary, The Overall Kinetics of Hot Gas Ignition (Ph.D. Thesis), 1971. Fink, Zachary with Marcel Vanpee, :Kinetics of Ignition by Hot Gases (Presented at the 15th International Symposium on Combustion, Tokyo), 1974. Glassman, Irvin. Combustion, Orlando: Academic Press, Inc., 1987, 299. Goh, S.Y. and A.S.C. Ma, A Theoretical Investigation into the Ignition of Explosive Environment by a Hot, Laminar, Round, Inert Gas Jet, TWF/TN132, 1967. Kaskan, W.E. The Dependence of Flame Temperature on Mass Burning Velocity, 6th International Symposium on Combustion, 134-43. $234=>   $ % ) * J K : ; k l jh^Uh^ hH*hh*S hDDHH* hDDHH*hDDHhlhhh5CJ aJ h5CJ$aJ$hh:~5>*CJ$aJ$h*S 5>*CJ$aJ$hh5>*CJ$aJ$:34=>   % F i {   6 g gd^gdlgd$a$gdhFhi\~^<=>?B!./78(ij $%`a,. L"""U#V#$$Žιι hk(H* hk(H*hk(h,o:hSeh6s h H*h<h hH*jQhe;Uhe; h3)H*h3)h^hbhWhE^_^_=@Aef{ij-gdl-.!!+","V#W#T$U$$$ %!%P%Q%z%{%&&''))*gd]gdl$-%/%P%Q%T%y%z% &O&P&&&((.*3*******++&+'+<+=+@+p+s+++++++++++++++!,$,[,^,,,,,?-ƺڶڶڭکڭڭڭڊhe;hvG hZ:hZ: hnThW hnTH*hnThWhZ: hZ:H*hhZ:h5CJaJhDDHhH*hZ:h5CJ aJ h] hH* hH*hh hk(hk( hk(H*hk(6********++=+p++++!,[,,--////k1l13gd$a$gdgd]?-\-k-----3.S.//////j1k1111 2428222333333334d4444444444r55 66l6s666żё𑃑h9 h|LH* h|LH*h|LhvnhnT>* hvn>*hvnhvn>*hvn5CJaJhvn5CJ aJ hvG5CJ aJ hvnhvn5CJ aJ hvnh 'nhvGj he;Uhe; hnTh]hnTh^h&h]3333333334566y66/777<888K9L9l9m99%::gd]gdvngdnT & Fgdvn$a$gdvn6"7)76777K9L9l9m9k:::::::=;;,<======^>b>@AABB3F4FFGGGGyHHHHHHHHHºƶƲƲ垚h5CJ aJ hZ:h5CJ aJ h] h.hvnhh^ h.H*h.hnTjNh&Uh&h$hvGh 'nj3(h 'nU hvnhhhvnhvnhvn>* hvnh|Lh9h|L0::::::;;===Y>u>v>(@)@AA D DEEGGHHHIh^hgdZ:$a$gdgd]HIMInIoIpIrIII+J-JFJbJcJvJJ9KBKKKKKKhShahchehhhhhhhҽҶ hlhlhUhlhl>*H* hl>*hlhZ:hZ:H* hZ:>* hZ:hZ:hZ:hZ:>*hZ:hZ:5CJ aJ !IIIIIcJdJJJJKKKKKthuhhgdl & Fgdl & FgdZ:gdZ:Marble, F.E. and T.C Adamson. Ignition and Combustion in a Laminar Mixing zone, Jet Propulsion, 24, 1954, 85-94. Patanker, S.V. and D.B. 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