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**Flow Coal Gasifier
**

A mathematical model has been developed to simulate the Texaco downflow RAKESH GOVIND and

entrained-bed pilot-plant gasifier using coal liquefaction residues and coal-water

slurries as feedstocks. This model describes the physical and chemical processes JOGEN SHAH

occurring in an entrained coal gasifier. The gasification kinetics describes different Department of Chemical

complex reactions occurring in the gasifier and the hydrodynamics describes mass, and Nuclear Engineering

momentum and energy balances for solid and gas phases. Temperature, concen- University of Cincinnati

tration and velocity profiles along the reactor height were obtained by solving the Cincinnati, OH 45221

mass, momentum and energy balances. Parameter studies were made to provide

a better understanding of the reactor performance for various inlet feed conditions

utilizing the model.

SCOPE

Entrained-bed gasifiers are cocurrent flow reactors in which is relatively free of higher hydrocarbons particularly the tarry

pulverized or atomized hydrocarbons react with oxygen and materials.

steam to produce gaseous fuels. These reactors are becoming In this paper, a mathematical model has been developed to

popular in the processing of coal into synthetic fuels and thermal simulate the Texaco downflow entrained-bed pilot-plant gasifier

energy since they produce higher coal gasification rates and are using coal liquefaction residues as feedstocks. Results of the

easier to operate than fluidized- or fixed-bed reactors. Further, simulation have been compared with experimental data from

due to the incineration effect they produce a product gas that the gasifier.

**CONCLUSIONS AND SIGNIFICANCE
**

The Texaco downflow pilot-plant gasifier was simulated by found that oxygen-fuel ratio affects carbon conversion more

simultaneously solving the mass, momentum and energy bal- than the steam-fuel ratio. The steam-fuel ratio significantly

ances- for the solid and gas phases. Good agreement was ob- affects the gas product composition. The optimum oxygen-fuel

tained between the simulation programs and experimental re- ratio is between 0.8 and 0.9 to achieve 98-99% conversion.

sults. The gas composition leaving the gasifier and the final Depending on the oxygen-fuel ratio, the optimum steam-fuel

carbon conversion depends on three essential parameters: the ratio ranges from 0.3 to 0.6 using coal liquefaction residues as

fuel rate, the oxygen to fuel ratio, and the steam-fuelratio. It was feedstocks.

**INTRODUCTION the severe operating environment expected. In this section, com-
**

bustion and gasification reactions take place. The lower section is

As research and development continues on entrained flow re- a quench vessel. A reservoir of water is maintained in the bottom

actors, a mathematical model is necessary for gaining an insight of this vessel at all times by continuous injection of cooling water.

into the influence of design variables, feed materials, and processing Syngas leaving the top section of the gasifier passes through a

conditions on the reactor performance. Furthermore, such models water-cooled dip tube into the water reservoir in the quench vessel.

will be necessary and powerful tools in optimizing, scaling-up and Slag, most of the soot, and unreacted hydrocarbon carried with the

designing the process. syngas remain in the water and are then removed. The saturated

In an entrained flow reactor, small condensed particles (solid syngas is removed from the gas space above the reactor.

or liquid state) are dispersed into a moving gaseous medium The pulverized coal liquefaction residue is made pumpable by

thereby entraining the injected particles. This provides the largest melting and being kept at 204-260°C and then blending with 2-7%

solid-gas (or liquid-gas) reactive surface area possible and reduces aromatic solvent. The molten residue, oxygen, and steam are fed

the gas-phase diffusional resistances, so that rapid chemical reac- through a proprietary Texaco burner into the top of the pilot-plant

tions between the phases can occur. gasifier. All of the runs with coal liquefaction residues were con-

The Texaco pilot-plant gasifier, Figure 1, is a downflow en- ducted at a pressure of 24.31 X 105N/m2.

trained-bed reactor and has been described in detail in a report by For coal-water slurry runs, the coal is mixed with water and

Texaco’s Montebello Research Laboratory (Robin, 1976).The 152.4 preheated to a temperature below saturation point so that water

cm (5 ft) diameter by 609.6 cm (20 ft) long steel vessel is divided in the slurry enters the reactor as a liquid. It has been reported that

internally into two sections. The top section (330cm long) is lined the slurry can be mixed and pumped at solid loading as high as 70%,

with a special refractory material specifically designed to withstand i.e., at a water/coal ratio of 0.4 (Bissett, 1978). The operating

pressure for coal-water slurry runs is about 21.28 X 105 N/m2.

Table 1 shows the ultimate analysis of fuels used in the pilot-plant

Correspondence concerning this paper should be addressed to Rakesh Govind. runs.

AlChE Journal (Vol. 30, No. 1) January, 1984 Page 79

HfiO.37 1.200°C. 30. by the burning of the combustible volatiles.31 0. % - Feedstock Source and Run No. perhaps ex- cept for that of the char-hydrogen reactions. ANALYSISOF FEEDSTOCK USED IN TEXACO'S PILOT-PLANT TESTS* Dry Fuel Analysis.77 1.03 1. No.72 Western coal used in coal-water slurry runs 74. Hydrogen Sulphide.1. Sprouse (1980) Reaction and Goyal (1980) studied the hydrogasificationprocess rather than combustion in a different type of reactor system.20 Eastern coal used in coal-water slurry runs 72.48 H-coal residue from Wyodak coal for run W-1 78.05 6. Nitrogen and tar.53 0.exp(-A(exp(-B/T))t)) fier.70 11.65 1.OOO°C. carbon dioxide.83 0. When heated to high temperatures.73 Page 80 January. The kinetics of this thermal decomposition process is quite AW = QVMo(1 . CHd). Combustion and gasification section 3.72 5.Hp. An- Wen and Chaung (1979)used the Stoke's Law approximation for thony et al.. Sand ash. the rates of these reactions..A +C. Pyrolysis reaction which released the moisture and volatile matter in the raw fuel is usually the first to occur and REACTOR the fastest among these reactions.04 5.40 2. 1970.08 SRC-I1 vacuum flash drum bottoms 64. coal and coal liquefaction residues. The yields of volatiles and their composition depend not only on the volatile matter content of the raw fuel but also on the temperature. pressure and rate of heating during pyrolysis. char-oxygen and char- hydrogen reactions.99 9. are polymeric compounds consisting of C.07 3.54 - Exxon DSP vacuum tower bottoms 70. 6 coal for run 1-1 74. 1976): the particle instead of the solid momentum balance.S.56 P t ) TABLE1. CooCEKj char-carbon dioxide and char-hydrogen reactions are usually slow WATER and depend on the volumetric compositions.13 8. which heats the and Blake's (1979)since they did not consider the chemical reaction solid fuel rapidly to the pyrolysis temperature.74 3.56 5. char-steam. entrained-bed system.82 0.*/(l + 0. 0. H2. resulting in the evolution of gases and liquids (condensablevapors).70 16.46 11.92 0. A large amount of heat is produced in the gas Our approach is different from Kane and McCallister's (1978) phase. V* = V i f + V.05 0. char-carbon dioxide. in conjunction with reactor hydrodynamics and energy balances.c)(l .900/TC)-(V* . 1984 AlChE Journal (Vol.OOO"Cand so diffusion through the gas-film and ash-layer is the controlling factor in the gasification.. C. Based on the chemical reactions. momentum and energy balances poses and produces volatiles which consist of a mixture of com- with the reaction kinetic equations using a stirred tank in series bustible gases.V ) dt The amount and composition of the evolved products depend on the type and size of coal and the conditions prevailing in the gasi. particle collisions are unlikely to be frequent and the ash layer formed can be assumed to remain on the fuel particle during the reaction. C H N S 0 Ash CI H-coal residue from Illinois No.32 15. However. wt.OyiNa. For temperature below l.73 1.90 3. Pyrolysis and volatile combustion section 2. 1) .N&A + Volatiles A Kinetic Equations REACTOR MODEL dV. it decom- the simultaneoussolution of mass. 4SLAG Figure 1. 6 coal for run 1-2 73.37 5.96 1. at tem- peratures above 1.14 X 1@ exp(-8. the coal particles undergo major K = K Oexp(-E/RT) physical and chemical changes due to thermal decomposition. used in an Table 2 summarizes the background for the modeling of two. AV = VMo(1 . char-steam. Pyrolysis and Volatlle Combustion The input fuel. In an entrained-bed reactor. Rates of coal pyrolysis in an inert atmosphere have been inves- Ubhayankar (1977)did not consider the momentum balance.25 2.exp(-A(exp(-B/T))t)) complex and numerous mechanisms have been proposed in the literature.99 0. the operating temperatures are usually much higher than 1. Texaco downflow entrained-bed pilot-plant gasifier.37 H-coal residue from Illinois No.. (CO. It is thus unreasonableto assume that the reaction rates may be estimated by the unreacted-core shrinking model for an entrained-bed gasifier.95 16. reactor model for both the solid and the gas phases.47 7.c)(l .70 25. phase entrained-bed reactors. N. Since the particle loading in an entrained-bed gasifier is small (less than 1%of the reactor vol- ume). and tigated by many researchers (Bazioch and Hawksley.79 0. the gasifier can be divided into three sections: 1.67 1.V) - Kinetics dt In an entrained-flow reactor. The mathematical model involves H. Gasification section Major solid gas reactions involved in coal gasification are py- rolysis.K(V* .74 4. -dV _ .71 1. are controlled by gas-film diffusion and ash-layer diffusion.18 2.25 0. The kinetics of each reaction has been discussed in the following section.

+ COz COz 2Hz0 x HzO (11) (12) TOTAL VOLATLE YELD TAR a GASEOUS co YELD (assumed C6H6) Equation 4 predicts a higher pyrolysis rate than most other ex- isting data. Mechanical energy One-dimensional flow. and circumferential scale-up techniques were direction devised. steady- Chaung 0 2 . and relating included layer considered hydrogasification reaction rate Goyal (1980) Cities Service Johnson’s Continuity Mixture momentum Thermal energy One-dimensional flow. char. ‘CIS lo 1. H. relating solids. 1964): at lo3 rate.a In P t ) (8) The unreacted-core shrinking model proposed by Wen et al. volatiles. V* = V* (at 1 atm)-(l . parti- cle-particle interaction is neglected. char-HSO. Note that in Figure 2 the yield of hydrogen is independent of the prox- imate volatile matter content.Mass rate of Not considered Thermal Energy One-dimensional flow.1 5 total pressure 5 50 atm . stirred-tank plug-flow (1979) COz.* considered as surface reactions because of high operating tem- = portion of volatile yield that exceeds V i r at pressures peratures (above l. 4 is then matched with the product distribution assuming that the composition of the volatile product is independent of the rate. Wen and Texaco gasifier Devolatilization. unsteady- (1977) generation phase reactions. of relationship.’s hydropyrolysis equations for balance was used. 0 and S. just like coal. gas. balance state. char. production & state.066 for bituminous coal 0. two-phase. the ash layer formed <0. Figure 2. equation drag force balance state. plug-flow. the product distribution for the pyrolysis process is estimated. It is important to note that we have used experimental data of Loison and Chauvin (1964) for coal liquefaction residues. Product yield of coal pyrolysis (Loison and Chauvin. It has been assumed that. Chemistry of coal Differential Equation of motion.Since the system is very dilute. steady- R&D Co. Data: + YzO2 . and the data are applicable with the appropriate volatile content for the residue. axial balance unsteady-state. TABLE2.-. In an entrained-bed gasifier. plug-flow. 0 10 20 30 40 50 Further the pyrolysis reaction occurs first and is the fastest re- action. No. therefore. are used to predict the volatile product composition. unsteady- both phases balance balance state.00OoC). 1984 Page 81 . AlChE Journal (Vol. the relative compositions of the product gases are the same as obtained from Figure 2. a model for bench-scale model used both phases drag force considered hydrogasifier reactor included Vir Char-Gas Reactions = potential ultimate yield of volatiles at pressure >loo atm. most char-gas reactions can be V. (1968) is used to estimate the solid-gasreaction rates. Hence the final carbon conversion is not very sensitive to the pyrolysis Figure 2. N. since these residues are polymeric compounds of C. 1) January. Based on information on the amount of hydrogen. nonreactive flow Sprouse (1980) Rockwell Int. steady- FHP reactor particle. char-Hz. exponential model water-gas shift reaction rate expression for velocity Blake (1979) Similar reactor Not considered Continuity Multidimensional Multidimensional Multidimensional. 30. The temperature rises very quickly during the pyrolysis PROXIMATE VOLATILE OF COAL. during pyrolysis. McCallister Equation for radial. the ratio of CO/COZ and HzO/COZ obtained from Figure 2 together with the material balance on different elements. system equations for momentum mechanical turbulent model.coz Volatile Combustion co + 1/202 (9) Hz + ‘ / ~ O Z HzO + (10) >p. In this model effects a = 0. Not considered Continuitv Equation of motion Mechanical energy Multidimensional flow. dimensionless (1978) and equations are prepared. boundary devolatilization. exponential mixing plant thermal cracking.001 atm can be assumed to remain on the fuel particle during the reaction.O5O0C.Differential Stoke’s law is Thermal energy One-dimensional flow. reaction and the reaction is completed in a very short length (about (% DMMF BASIS) 10 cm) as compared to the total reactor length of 330 cm. BACKGROUND FOR MODELING OF TWO-PHASE ENTRAINED-BED REACTORS Reactor Mass Momentum Energy Author Simulated Kinetics Balance Balance Balance Comments Ubhayakar MHD power Devolatilization. equation assumed for balance state. plug-flow model constant particle size remaining solids Kane & . Experimental data by Loison and Chauvin (1964). + CH4 Hydrocarbons +0 . The volatile production rate from Eq.

= 0. The overall rate can be expressed as follows.y)H2O a C O char-steam.Field et al.710 exp(-17. CO + HzO .s) in the + ( a .O. Kdiff = 7. (1968): K s = 0.877 X 105) .500 exp(-6. designated as I' (g/cm3.HpO.PHB. Water-Gas Shift Reaction + (2/4 .Z(dp .Dutta et al. is estimated by a correlation suggested by Wen et al. C. 1) . The nature of mixing 6 between the solid and gas phases can have a significant effect on H2 + cH2S + . = PHZ .060/Tc) (31) hence. = . 30.[rz + r3 + r 4 ] for gasification section RP K. 75 exp[18. Page 82 January.967/Tc) (22) CH4 + HzO F+ CO + 3Hz (44) Kinetic Equation dCCHI dt = -KCcH4 (45) K = 312 exp(-30.OSS](Z + 2) (19) pf * (s)(gof ash) (40) for 0.NaS..N2 + ash (30) the final carbon conversion and product composition.A + ( a .1)COz (16) The gas-phase reactions occurring in the gasification section have been investigated by Singh and Saraf (1977).of ash layer diffusion..30.p .P i = PHz0 .- 1 F+ X C02 + H2 (39) Pt Kinetic Equation + 4 = (22 2)/(2 + 2) for d p I 0. Each compart- ment is treated as a stirred-tank reactor.005 cm (18) gmol + = [(ZZ + 2) .. = 247 exp(-21.005 cm < d p I0. char-hydrogen reactions per unit volume of the solids in the reactor.1/4)CO + (2/4 . (1977). The basic assumptions have been: Char-Carbon Dioxide Reaction (1) The solid-gas phases are assumed to be completely mixed.gas film.1 cm 4 = 1.HpO. 2 (2) Radial dispersion is neglected. Ash layer is assumed to remain on particle surface.Dobner (1976). unreacted core shrinking model is assumed.000/RT) in s-l (46) - Char-Steam Reaction The net rate of char consumption due to the char-oxygen. K.12 exp(-17.060)/Tc) r = R p (47) 3 .P ? ) (13) PI .713 and Wen (1978). char-carbon dioxide. No.400/(1.644 .1 cm (20) Z = 2.921)/Tc) (35) Kash =K d i d (15) Kdiff = 1.(2.N&A + aCO2 + 2aCO + -Y2 H2O A compartment-in-series approach is employed.l)~lCOz+ . = 8. A steady-state one-dimensionalmodel for the reactor system has been formulated. and Zahradnik and Grace (1974). (:1 H2O +EH~S + -62 N2 + ash (17) Kinetic Equation Rate = F.t)H2 + cH2S + -26 N2 + ash (25) reactor modeling equations discussed in the following section can be written as Kinetic Equation 3 -[rl + r~ + r 3 ] for combustion reaction - K .y + -P2 .260/(1. Char-Oxygen Reaction PI .8Tc)] (28) Model Development PI . (38) Carbon + l/+0 2 + 2(1 . Kinetic Equation (3) Due to a very dilute system. Ks = 247 exp(-21. 1984 AlChE Journal (Vol. diffusion and chemical reaction are considered.PCO (29) Ke.8Tc)] (37) 34. = Pcoz (33) Char-Hydrogen Reaction Kdiff Kash where Y=- rC (14) + Y H ~ O+ tHzS + -26 Nz + ash (34) R?J Kinetic Reaction The ash diffusion constant.2 (43) Methane-Steam Reaction K .33x (36) The specific char-gas reactions have been investigated by Wen and O' Dutta (1978). (1967). Wen and Chaung (1979).249/T) (21) T = (Tc + Tg)/2 in K F.45 x (32) Rate = 1 * (Pi .OO5)/O. Kash. interactions among particles are neglected. = exp[17.P.0 for d p > 0. C.

1975).7 5. can be written as 3E I =-AA.6 ) P g U g ) x = rE (49) 1979) 2K Solid-Phase Momentum Balance hc = A (57) dP (fPcUz)x+Ax + . 30.9 for the = 0. (58) 24 C D = . 1) January.0.5. The 1 = pyrolysis 2 = char-oxygen reaction effect of ash as a catalyst has been formally neglected although this 3 = char-steam reaction may have been accounted for indirectly when the kinetic equations 4 = char-carbon dioxide reaction were developed.The emissivity of the gas mixture is selected to be 0. the following overall heat balance is obtained. = 2.3 m long reactor results in a dispersion number ( D / U c l )equal to 0.6.15Re0. the temperature gradients within the particle are negli.T : ) RP I I C p . 1979) tween the gas and the reactor wall. ~ i P d U C i -l Combining the gas-phase and solid-phase thermal balances. potential and k = reaction kinetic energies have been neglected in comparison with thermal energy. and volatile combustion Dvrolvsis 1 1. be- Gidaspow. Reaction Section i k Solid-Phase Mass Balance -.4 L2.((1 . 6 + = CH4 HzO+CO 3Hz + ment have been investigated by Arastroopour and Gidaspow Three Reaction Sections (1979).Tc)x . and Wen (1979).f s c (50) section have been summarized in Table 3. Drag Coefficient (Rowe and Henwood. Gas Phase: (9) Due to the high temperatures in the reactor.e.2. 30%of the total heat generated by = (1 .OOO (53) Texaco entrained-bed gasifier.f ) P g u g ) z + Ax . T g + ~~c~ccpcTc)x+Ax + ~PcUcCp. Drag Force per unit Volume of Particles (Arastroopour and (2) The rate of heat exchange per unit area of reactor wall. which has been used by Wen (1979).((1 . 4 combustion and gasification 2. F . ((1 . which is about 7-10% of the heating value of the raw fuel. Solid Phase: gible). 1 = Hz + -21 0 2 HzO + The compartment-in-seriesapproach is tantamount to assuming 1 2 =co+-o2'coz plug flow for the solid and gas phases (Wen and Fan.T w ) .687)for Re < 1.Ax e F o ( T t . REACTIONS (5) The temperature of solid is uniform throughout the particle (i. j = reaction (6) Ash is assumed as inert and it remains with the particle.44 for Re I1. 7 = methane-steam reforming reaction (catalyzedby the mineral ma- glected. Eq.3 gasification 3.( f P c u c ) x = -rf (48) Gas-Phase Mass Balance Convection and Conduction Heat Transfer Coefficient (Wen. The 2 selection of 1 cm height compartments for a 3.((1 .3.c ) P t ) z + A x g c .E ) P g u g c p . ' (4) Ideal gas equation of state is assumed to hold. + ((1 . for radiation heat transfer between gas and fuel particles can be assumed to be 1.4.( C P c u z ) ~ (@L)x+Axgc Reactions occurring in the solid and gas phases for each reaction . char) (7) The frictional force between the phases and the wall is ne. the viewing factor. the final results will change if ash catalyzes the 6 = water-gas shift reaction (catalyzed by the mineral materials in combustion reactions. terials in char) (8) No particle attrition is considered.f ) P g g + fsf (51) reactions is transferred from gas phase to the reactor wall.4 P g U g C p J g AlChE Journal (Vol.OOO Because of very dilute system. is calculated by UO(Tg. momentum and energy balances for each compart. 55.Rowe and Henwood (1961).((1 .600(x/L)in O F .. Gas-Phase Momentum Balance An approximate approach followed by Wen (1979) has been followed to compute heat exchange between the gas and the reactor ((1 . No. TABLE3.3. 3 4 5 = CH4 202 + + COz 2Hz0 + -+ = C6H6 15/2 0 2 6 c O ~ 3H20 = CO + HzO + COz t Hz + The mass. Since the validity of the results depends on the 5 = char-hydrogen reaction kinetic equations.(1 Re + 0.6 (fPcuc)x+Ax . 1984 Page 83 .f ) P g U i ) x + A x .0015 which is essentially plug flow.f)PgUi)x wall. a linear correlation of the wall temperature is as- sumed. . ((1 .100 . The value of Uo selected is temperature.( f P t ) x g c = EPcg . (54) SOLUTION PROCEDURE The solid-phase thermal balance. in the zones following combustion zones.E ) P t ) x g c (1) In the combustion zones. 1961) T .

Us and solid I guessin! ralue residence t i e in the compartment (3) Calculate partial pressures for different gaseous components Use calculated partial pressure Figure 3. 6 p . A€)and the elements of the A matrix A21 =0 and vector C Page 84 January. Equations 58 and 59 are used to compute the solid and gas tem. All = CiPci peratures. predict the char composition ~ f i s t comDartment Use Runge-Kutta-Gill Method to find sold temperature for this compartment I Assume values of partial pressures Reas: for different gaseous components Tg Vi the nc 4 comp Use Root-Search and s Methods (Regula. No. The mass and momentum balances for the solid and gas phases A12 = 0 are solved simultaneously as follows: A13 =0 X = A-lC (61) A14 = pciUc5 + FAX where X = (AU. 1) . AU. Computer flow diagram for solving the model equations. 30.. respectively. 1984 AlChE Journal (Vol. furthc Falsi) to look (1) Calculate r f r o m kinetics calcul for a better Tg (2) Calculate Uc ..

350pm i = inlet conditions Specific heat = 0.67 298 Western Coal used in coal-water slurry runs 186. In our study. 62. check total heat balance.87 400 400 600 (1) Assume a value for the gas-phase temperature ( T g )in the compartment. 400pm All other runs. p=l due to lack of inlet velocity data.33 67633 298 H-coal residue from Illinois #6 (Run W-1) 86. OPERATING CONDITIONS RUNS OF TEXACO'S FOR SEVENTYPICAL PILOT-PLANT TESTS Fsed Rate Feedstock Source (Hun Number) Fuel Rate (g/s) w Fuel 4 L Fuel Fuel Feed Temperature (K) Steam Oxygen H-coal residue from Illinois #6 coal (Run 1-1) 76.66 0.9 total mol of gaseous components leaving compartments a1 = Overall heat transfer coefficient between gas and reactor wall = total mol of gaseous components entering compartments 122 kcal/hr.866 505.22 696. using Runge-Kutta-Gill method. TABLE4. 1984 Page 85 . versions were found for runs where the fuel rate is higher.18cm/cm3 Initial solid velocity = 50 cm/s (assumed) . use calculated partial pressure values as new guessing values and repeat the procedure again.P b . the inlet velocity of solids was assumed to be 50 cm/s for all the runs.55 692.28 X 105 N/m2 Diameter: 152.45 cal/g"C The partial pressures of gaseous components leaving the com. Gasifier Pressure: Coal liquefaction residue runs 24. RESULTS AND DISCUSSIONS The Texaco reactor was simulated for 27 runs using coal lique- faction residues and two runs using coal-water slurries as feedstock.22 696. Significant deviations in the gas composition and carbon con- The partial pressures of the gaseous species leaving the com. This can partment are computed using Eqs. If the total heat bal- ance satisfies the required error criteria.90 513.241 0.m2.7682 496. 1) January. 61. 1964). 47.alpout rate.79 0.4 cm (5 ft) Height: 330 cm (combustion section) Solid Phase Initial density of coal liquefaction residue = 1.Uii(I . 62. (3) Assume the values of partial pressures for gaseous compo- nents leaving the compartment.11 0. 60. Otherwise.32 X 105 N/m2 (24 atm) Coal water slurry runs 21.318 0.44 298 SRC I1 Vacuum Flash Drum Bottoms 126. No. Ff Pt 5 r:.63 and 64.314 0.78 0. For a stirred-tank reactor The gas composition leaving the gasifier and the final carbon 1 conversion depend on three essential operating parameters: the fuel V'f . use root-search method (Reg- ula-Falsi) to find a better value of Tg and repeat the procedure again. Othersise.50 0. repeat the procedure for the next compartment. Gas Phase partment are calculated using the following material balance Specific heats for gases and heats of combustion (Perry's Hand- equations.22 696. Tc. This lack of experimental data makes it difficult to exactly compare the numerical results of 2 PLt = pt 1=1 (64) the simulation program with experimental data. Parameter values for these seven typical runs are as follows. Ug and solid residence time in the compartment from Eq.30 0.0 0. If the partial pressures meet the required error criteria.70 505. Table 4 shows the operating conditions.ci)Apg Initial particle size = Wyodak coal liquefaction residue. be attributed to the error in the inlet velocity of the solids which The solution procedure shown in Figure 3 is as follows: in the experimental run was probably much higher than 50 cm/s AlChE Journal (Vol.5 0. Calculate partial pressures for gaseous components leaving the compartment from Eqs.91 400 400 600 Eastern coal used in coal-water slurry runs 133.52 0.18 0. ( 2 ) Calculate solid-phase temperature. (5) Check total heat balance using Eq."C (25 Btu/h*ftz-"F) The results of the model predictions have been summarized in Table 5 along with the reported experimental results (Robin. 30. from Eq.11 0..63 and 64. Calculate values of U.67 298 H-coal residue from Illinois #6 (Run 1-2) 81. (4) Calculate value of r from Eq.79 505. 59.67 298 Exxon DSP Vacuum Tower Bottoms 126. book) Emissivity of gas = 0. the oxygen to fuel ratio and the steam-fuel ratio.

. 1) . 1984 AlChE Journal (Vol. No. 30. TABLE5. C02 CH4 H2S N2 RUN INPUT CONDITION NO. COMPUTATIONAL RESULTS THE MODELvs TEXACOENTRAINED-BEDPILOT-PLANTGASIFIER r co H. Flow Rate Flow RateFlow Rate Flow RateFlow RateFlow Rate Carbon 4/sec 9/sec 4/sec 9/sec 9/sec 9/sec :onversion Fuel Rate O2 Steam ( V O l 9 ) (Vol 76) ( V O l % ) ( V O l X) (Vol X) (Vol % ) % (9/sec) Fzl Fuel Source Page 86 January.

66 W-3A 128.81 1.859 0.626) 220.56) (8.279 Exp ((59.198) (0.- 157.253 (37.7 132.109 1.286 (37.25 6.04) (0.44 (36.71 9.08 Model (54.84 1 (5.ooi I1.34 10.566 Exp (53.40) 196.231 0.69 0.82 135.343 I 25.77 w-4 (57.50 0.78) (0.26 7.654 86.91) (16.49 0.04 41.58) I(8.0 0.2 0.88) (0. .45 '0.21 f a.00 4. Continued co HZ C02 CH4 N2 RUN NO.8484 0.44) (36.63 42.11) 99.97 (39.511 (3.963) (8.52) (11.25 (49.62) I(31.58 6.86 0.00) W-5 W-6 W.79) (0.42 1-1 1 132.016 0.187 -Model 155.07 (54..41 176.24) 10.39) B.94 10.16) (32.64 1 I 0.06) 1 (0.85 25.75) l(8. 1) January.04 0.304) 87.038) (0.77 0.27 126.90) (4.29) . 30.52) l(0.8 AlChE Journal (Vol.82) W-38 128.18) :611:?4) (0.129 i!j?O2) (5. .844 0.91) 1312 f4G.OO) (0.744) .8) (7.6) (33.79 0.75) 146.47) (4.37) 143.4 74.43) 174.29) (12.855' 0.96 0.:3663) ii:::) w.865 17.79 Oa5 Model (37.7) (7.04) l(0.00 3.10 126.54 .264 8.54 0.5) 99 .51 8.44 10.37) (0.87 29. Model I(52.30 Model (50.092) (0.98 9.57 129.61) 167.O.475 Exp (45.087 1.38 43.91 16.34 I 0.95 1. 1984 Page 87 . INPUT CONDITION Source I( I 9/sec 9 / s e c j(vzis. vol %) (vol %) 1 r n v e r%s i o n 1 204.318 EXD (56.20) I 1 33.68 8.1 w-2 87.96) w-1 (38.921) 21 1. .310 -EXP Model Exp L' 215.81) (5.491 z 76!!87) (0.09 Model (52. Using SRC I 1 Vacuum Flash Drum Bottoms as feedstock: I I I I I I I I INPUT CONDITION I Flow Rate FlowRate FlowRate '1owRate FlowRate howRate Fuel FlowRate Carbon Rate (Wet) O2 - Fuel Steam i%T Source 9/sec 9/sec 9/sec 9/sec 9/sec 9/sec (vol 9 ) (vol %) (vol %) (vol %) (vol %) (vol %) 9/sec (vol %) - 'onversion % 167.15) (0.1 1.318 10.38) 99 135. TABLE5.02 i(54.rj vol %) (vol I) (9/sec 1 low Rate h o w Rate Flow Rate Flow Rate Flow Ratb Flow Ra'e Carbon 9 / s e c lvzis.16 10.06 23.37 45.936 32.613) 34.67 0.032 (0.03 39.10) (6.11 0.90 0.9) (. 212.00) 189. I 215.11 0.98 14. No..69 1.

tional to the particle size.64 0.44 32. reactor have been shown in Figures 4 through 8 for Run No.5 0. Large atures.093 20. Steam and COz concentration attain a particles. Continued D. increases initially and then decreases and attains a final value of ature profiles along the reactor height Both the solid and gas 19.028 0. etc. 1984 AlChE Journal (Vol.05 0.15 20. % Vol. 1) .2 cm/s. On the other hand.370 velocity based on the inlet solid density is 101 cm/s which is higher K respectively. % Vol. 2 8 $ d' 8 8. At this point in the reactor the entire oxygen gets then the inlet velocity of 50 cm/s. TABLE5.7 Westerr 186. L s + m - Y Y 0 i 8. The maximum velocity is at- Page 88 January. Solid velocity using Illinois No.87 0. the specific contact area between maximum at a height when oxygen has just been consumed.00 420W REACTOR HEGHT ( CMS.79 Model 39.03 0. namely. These two effects combine to give higher indicating significant conversion in the first 100 cm of reactor conversion for smaller (droplets) with higher inlet velocity. assumed in the simulation program. No.78 0. Figure 7 shows carbon conversion as a function of reactor height.91 0.00 380. 4 9 co.51 Model 42.55 36.00 7000 14000 21000 280. 30. concentration and velocity profiles within the Figure 8 shows solid and gas velocities along the reactor height.40 0. 1 REACTOR HElOrr (CMS. E O0. % :onvers ion % - EXP 50. 1-1 Gas velocity increases as different gases are produced. char-COz. char-steam.498 0. % Vol. faction residues) rates the particle (droplet) size becomes smaller. Product gas composition profiles for 1-1 run. reacting gases and the fuel particle (droplet)is inversely propor. Figure 5.79 13. temperatures undergo a rapid increase due to the highly exother. At higher fuel (coal lique.14 0. % Vol. The temperature. consumed and the endothermic reactions. Coal-Water Slurry Runs: COAL INPUT CONDITION co H2 C02 CH4 H2S N2 TYPE ' Coal Carbon Rate (9/sec) - O2 Coal - Water Coal Source Vol. The solid velocity increases initially since the solid terminal mic combustion reactions attaining a maximum of 2. become effective. reducing the and gas temper- since the fuel is sprayed into the reactor through nozzles.1 Figure 4.71 35.021 0. ii $ 3 12 8.427 86. particles (droplets) have greater terminal velocities and thus travel The change in gas composition over the reactor length have &n at higher velocities resulting in shorter residence time than smaller shown in Figures 5 and 6.33 8 P 8 9 - I co 0 * ? s 2.38 85.24 92. Temperature profilesfor 1-1 run. % Vol.269 and 2.00 0.00 7000 14ObO 21600 280'00 35600 42000 20.8 Eastern 133.075 0 795 97. Figure 4 shows the solid and gas temper.79 EXP 41.62 21. 6 coal.09 0. height.46 37.85 0.

5 0. 7aa.8 and 0.6 0. Effect of oxygenlfuel ratio on carbon conversion at varlous steam/ formance for various operating conditions using the model. Yelocity profiles lor 1-1 run.9 As the solid density decreases. The solid velocity de. Carbon conversion profiles for 1-1 run. 75 tained at the exit of the pyrolysis section. Figure 10 on the oxygen/fuel ratio the optimal (for maximum carbon con- shows the effect of steam/fuel ratio on carbon conversion at various version) steam/fuel ratio ranges from about 0. 1984 Page 89 . significantly but does not have a significant effect on the gas the optimum (for maximum carbon conversion)oxygen/fuel ratio product distribution. gasifier using coal liquefaction residues as feedstock.3 to 0. Figure 9 shows the effect of oxygen-fuel ratio on carbon con- version at various steam/fuel ratios feeding the coal residue from is between 0.6 for this oxygen/fuel ratios using coal liquefaction residues as feedstock. 70 creases due to the decrease in solid density caused by the reaction. 6 coal into the Texaco pilot-plant gasifier. REACTOR HEIGHT (CMSJ Figure 8.9 to achieve 98-99% conversion.On the contrary. 100 PARAMETER : 95 STEAM I FUEL h aR (OM I GM) Y =8 90 fi 85 0 i3 9 am 7 m -1 21m 28O. 8- P %- u s aa. Depending Illinois No. Product gas composition profiles for 1-1 run. the terminal velocity decreases and the solid particle follows this trend. No. Figures fuel ratios. steam/fuel ratio significantly AlChE Journal (Vol. 30. It was found that oxygen/fuel ratio affects carbon conversion more Figure 11shows that oxygen/fuel ratio affects carbon conversion than does the steam/fuel ratio. Figure 9.lm 3Moo 42om 3 0 80 REACTOR m (aa) Figure 7.8 0. It was found that for this gasifier. 1) January. 9 through 12 show the effect of oxygen-fuel and steam-fuel ratio on the final conversion and gas product distribution.7 0. 0. OXYGEN 1 FUEL (GM I GM) Parameter studies were made to understand the reactor per. 14oa) 21am 28orx) 35Mo m m (CMS) REAcTm Figure 6.

866 gig.4 0. represents the effects so 5 u) of ash layer diffusion.4 0.241 glg. since the pyrolysis f8 = drag force on solids per unit volume of particles reaction rate does not significantly affect the final carbon con.8 0. 1) .K) keeping steam/fuel ratio. Figure 12. gas composition at oxygen/fuel = 0. F. Quantitatively. and water-gas shift reactions.3 0. Effects of steamlfuel ratlo on carbon conversion and major product genlluel ratios. for 1-1 run (H-coal residue from Illinois #6 coal) the sensitivity coefficient for the char-oxygen reaction was equal to 0.5 STEAM I FUEL (GM 1 OM) STEAM/NEL (GMIGM) Figure 10.866 OM I OM 100 70 I/PARAMETERS : OXYGEN I FUEL (GM l GM) 60 0.1 0. The char-steam kinetic coefficient also affected ~ STEAM / FUEL the % carbon conversion but not to the same degree as the char- : 0. = concentration in the nth compartment variations are due to the competition among char-oxygen.7 0. the concentration of Hz and CD = drag coefficient COz increases but that of CO decreases.5 0. Effect of steamlfuel ratio on carbon conversion at various oxy.- carbon conversiun. 7c 0. The sensitivity coeffi- cient for the same run for the char-steam reaction was 0. char dP = particle diameter (cm) COz.3 0.P . = correction factor for water gas shift reaction version.2 0. char-steam.86 and a steam fuel ratio of 0.257 for an oxygen/fuel ratio of 0. the char-oxygen kinetic coefficient had a major impact on the % 100 . g. Qualitatively the analysis revealed that k! = gravity acceleration.6 0. NOTATION affects the gas product distribution.Cpc = specific heats of gas and solids respectively (cal/ centration of Hz decreases but those of CO and COZ increases. 1oa SO 0. As the oxygen/fuel increases.24. gas film diffusion and chemical reactions. Figure 12 shows the effect of steam/fuel ratio on conversion and gas product distribution at a At = cross-sectional area of reactor (cm2) fixed oxygen/fuel ratio. according to Eq. (cm/sZ) Page 90 January. No.7 0.8 I 1 0. 13.s ACKNOWLEDGMENT OXYGEN I FUEL (GM I GM ) I would like to thank Ms. Effects of oxygenlfuel ratio on carbon conversion and major product typing this paper. D = diffusivity of gas (cm2/s) A sensitivity analysis of the developed model was conducted with e = emissivity of gas the char-gas reactions kinetic coefficients only. as noted earlier. the con. The sensitivity coefficient (S) is defined as follows: K E8 A%C Conversion . ) (65) where the Coefficient K .9 O2 / FUEL : 0. defining a char-gas reaction rate as -- E rate = K(P1 . These concentration C.241 (GM / O M ) oxygen kinetic coefficient.y= %C Conversion z AK / K Pa 5 80 The sensitivity coefficient depends on the type of runs and the operating conditions selected for the gasifier. 1984 AlChE Journal (Vol. Figure 12. gas composition at steamlfuel = 0. 30. Denterlein for patiently and accurately Figure 11.081. For example.2 0. Cpg.

MERC/RI-78/2. (1972).... Wiley Eastern Ltd. B. Eng. Fund.. Hemisphere Publishing = reaction rate of kth gas involved reaction (g/cm3.. j.” Ind.” Chim. M. “Coal Devolatizationand Hydrogasif- = total pressure in reactor (atm) ication.. ticle (cm) Bissett. B. 1) January. “Combustion =(Tc + Tg)/2(K) of Pulverized Coal. Chapman and Hall = rate of char-oxygen reaction Lts. = gas-phase velocity (cm/s) Field.. Dev. Sahagian. Process Des. “Pyrolyse Rapide Du Charbon. (1960). Belt. 4 Boothroyd. and D. Meissner. Eng. G. (1971). M. and J. No.625 (1976). Chem. W. = volatile content at time t (cm3/g) Goyal. Ed. “Vertical Pneumatic Conveying Using Four Hydrodynamic Models.. “Kinetics of Thermal Decomposition of the compartment of Pulverized Coal Particles. m = total number of reactions Rowe. Flame. = total volume of compartment Howard.. “Rapid reverse reaction effect (atm) Devolatization of Pulverized Coal. H. “Kinetics of the Activated €1 = voidage of ash layer Carbon-Stream Reaction. Henwood. Eng. McCallister.. M.” AIChE j .. Chemical Reaction Engineering. “Reactivity of Coal and Char. J. Essenhigh. H. A. “Drag Forces in Hydraulic Model of 9 = total number of gaseous species Fluidized Bed. Black. and R. Morgantown Energy Research Center (April.. “Pyrolysis of Coal Particles in Pul- = distance from the top of reactor (cm) verized Fuel Flames.D.” BCURDA.” Combust.. = correction factor a = stoichiometric coefficient for carbon = convection heat transfer coefficient between gas and P = stoichiometric coefficient for hydrogen solid (cal/cm2.. 14. H. T. Jensen. C. Perry. Process Des. H. and E. B. (col/cm2-s. Flowing Gas-Solids Suspensions.237 (1970)..pg = densities of solid and gas (g/cm3) Loison. 18.” 1 = gaseous component L. Chem. B. A. . Chem.. R. 15. and G. R. = rate of char-steam reaction Carnahan. 1976).. Hawksley.. EPRI-AF-233 (Dec. 1977). E. “An Engineering Assessment of Entrainment Gasification. Hottel.K-s) Y = stoichiometric coefficient for oxygen = heat exchange between gas and reactor wall (call 6 = stoichiometric coefficient for nitrogen cms) € = stoichiometric coefficient for sulfur = heat of reaction of kth reaction (cal/g) = heat of reaction of jth reaction (cal/g) = overall kinetic constant defined by Eq. H. 123 of compartment (1979). (cm/s) Field. H. J. H. Techno]. Stewart.atms) 1 = gaseous component = ash film diffusion constant (g/cm2-atm. A.. Morgan and P. R. Eng. and R. A.. = ratio of rc/Rp in an unreacted-core-shrinking par. Eng. B. Gidaspow. = gas-phase temperature (K) 20 (1977).E.. 2. B. Leatherhead (1967).. R. 55 (1978).121 (1976). = Sensitivity coefficient defined in Eq.” Combust. “Gasificationof Residual Materialsfrom coal Liquefaction.. 24. B. Luther. D. pc. 1984 Page 91 . S. 0. (1978). = solid-phase temperature (K) Field. Chem. H y - = reaction rate of jth solid phase reaction (g/cm3-s) drocarbon Conuersion Technology. Chilton. Thesis. J. 14. and P. Dev. J. B. 55.. R. k = gas viscosity (poise) Levenspiel. B.. Sundstrom. “Mathematical Modeling of Entrained Flow Coal Gasification Reactors. Ind.. A. 1. = effective partial pressure of gas taking into account Anthony.O. Flame. (g/cm%) 91. 74 = length of each compartment (cm) (1967). = wall temperature (K) Dutta. Howard.. 6. Chicago (1980). No. Eng. CA (Jan. 521 = gas constant (1970). B.” Ind. 30. T.. Gill.” = radius of the unreacted core of an unreacted-core..” Ind. “Hydrogen Production from Coal Liquefaction Residues... Chemistry of Coal Utilization.” Fuel.” i = inlet conditions in compartment EPRI Rtp. and D.. R..” Ph. M. Chem. Kane. Illinois Inst. 65 Superscripts = surface reaction constant (g/cm2-atm-s) g = gas phase = gas diffusion constant (g/cm2. 1976). G.. “Rate of Combustion of Size-Graded Fractions of Char from = solid phase velocity (cm/s) a Low-Rate Coal Between 1200°K and 2000”K.. “Measurements of the Effect of Rank on Combustion Rates = total volatile content of coal (cm3/g) of Pulverized Coal. P.470 cp = mechanism factor of combustion reaction (1975). and H. and R. In Carbon Dioxide Atmosphere.. D. W. N. Fifth Ed. Transport Phenomena.. Quarterly Report. O.” h d . € = solid-phase volume fraction Klei. “Scaling Laws and the Differential Greek Letters Equation of an Entrained Flow Coal Gasifier. 7. A. Eng. A... B.” Ind. S.” EPRI. cr = Stefan-Boltzmann constant. A. = outside radius of an unreacted-core-shrinking par. r = rate of char consumption. A. 9. H. Chem. N.. S. Dev. Process Den. C. John Wiley & Sons (1980)..318 (1975). 16. W. shrinking particle (cm) 1978). E. 14.. A. and R.43 (1961).. = temperature correcting factor Bird. 66 Palo Alto. AlChE Journal (Vol. dimensionless Minerals at Atmospheric Pressure. Lightfoot. 2971. P.” AIChE I. Y. R.269 (1964). Hawksley. Chemical Engineers’ Handbook. Process Des. Wen. 39. 13. Applied Numerical Analysis. “The Kinetics of Gasification of Carbon Contained in Coal ticle. FE-2247-11 (Oct. Nejat Veziroglu. W. S. Howard.. “Alternative Energy Sources. Robin. “Modeling of Entrained Bed Gasification:The Issues. L. = average solid velocity between compartments 237 (1969).” Ind. H. J. 22. Chem.s) * = equilibrium conditions = equilibrium constant of water gas shift reaction = thermal conductivity of gas (cal/cmK) = total effective reactor length (cm) = total number of reactions LITERATURE CITED = total number of species = pressure correction factor Anthony..K4) Lowry. M. Deu. = rate of char-carbon dioxide reaction John Wiley & Sons (1969). = partial pressure of Zth gaseous component at the exit Badzioch.k = reactions in solid and gas phase Robin. = rate of char-hydrogen reaction Dobner.Process Des. John Wiley & Sons. and C.” Trans. Wilkes. Chauvin. D. = partial pressure of Zth gaseous component at the inlet Arastoopour.” Ed. Subscripts McGraw-Hill Ltd.

.. C. N. Gasification. Computer time reduction up to 80% is demonstrated in the examples solved. Coal Conversion Technology. and R. Process Des. 1981). C. and R. 60. Israel fications do not change considerably the convergence rate of the Newton-Raphson and Broyden’s methods while reducing the problem’s dimension.. large systems of equations tend to be the major ones being: (1)tearing requires formula manipulation sparse so that each equation usually involves a small number which is very expensive in terms of computer time. Eds.” equations. Wen. J. L. P.. Chemistry of Coal Utilization-Sup. Saraf.. Dev. Lee. 126 (1974). Marcel Dekker. 3. and H. New York (1975).313 (1977). Evans.281 (1977). and R. Grace. Press (1976). It is shown that these modi. Chap. is presented. 26. M.. SCOPE Steady-state simulation or design of chemical processes gives partitioning. Y. W. Decomposition of Systems of Nonlinear Algebraic Equations A new method for decomposing irreducible subsets. It has been proved that it is advantageous manipulation. Addison Smoot. “Mixing and Gasification of Coal in Entrained Wesley Publishing Go. Numerical experiments have shown that they in the system. Chuang. The nonlinear expres. C. Eng. (1979). and by adding number of the tear variables is equal to the number of the re- new nonlinear equations to the system. Chem. and P. John Wiley & Sons (1963). Beer Sheva. Ed. solved sequentially. and T. E. Sticker. Academic Ind. “Entrainment Coal Gasification Modeling. 16. 30. Fortunately. “Noncatalytic Heterogeneous Solid Fluid Reaction Models. Znd. Y. Department of Chemical Engineering linear expressions by new variables. . method. and (2)the of variables.Singh.” Water-Gas Shift Reactors. “Chemistry & Physicsof Entrained Coal Thring.” Fuel.. C. is also presented.. R. Fan. H. This method consists of two steps: (1) elimination of the nonlinearity from some of the equations by replacing non. “Modeling Pulverized Coal Conversion in Entrained actors. The placing nonlinear expressions by new variables. Models for Flow Systems and Chemical Re- Sprouse. and there are several algorithms available for methods are used for solution. and it either improves or does not change the to partition a system to irreducible subsets (Hernandez and convergence rate when the Newton-Raphson or Broyden’s Sargent. K. T.” Szekely. 2. Flows. 1979). in the solution of systems MORDECHAI SHACHAM of nonlinear algebraic equations. J.”lnd. Flow Systems. The simultaneous solution of such a large as explicit functions of the tear variables. Essenhigh. D. 2. S. C.1983. It has been proved that these sions for replacement are selected so that the net effect of each operations do not change the convergence rate of the Newton- replacement is reduction of the number of nonlinear equations Raphson method. and (2) formulation of a problem of smaller Ben Gurion University of the Negev dimension by tearing the linear subset of equations. and accepted Bed Pulverized Coal Gasifiers. ducible subset. February 28. and E. P. 2. Ser. 1972). “Simulation of High-Temperature Wen.. H. Zahradnik. 1) . CONCLUSIONS AND SIGNIFICANCE The proposed tearing method includes the following steps: using partial Gauss elimination in this subset to express all the 1. Lowry. In the equation-oriented flowsheeting programs This operation reduces essentially the dimension of the irre- which are currently being developed (Shacham et al. Smith. Wen. which uses Boolean matrices instead of formula manipulation. No. 1984 AlChE Journal (Vol. Dev. J. FE-2666-f. Y. Eng. Tearing of the linear subset of equations is carried out by The net effect of the tearing is reduction of the dimension of Page 92 January. This sparsity makes it possible to decompose the smaller system generated by tearing tends to be more nonlinear large system into a set of smaller problems which can then be and more difficult to solve (Mah. Wen. The operations of this step are carried out in a may slightly improve the convergence rate of Broyden’s Boolean matrix so that no formula manipulation is required. impractical. S. Chem. Ubhayaker. Y. and D. rise to the need of solving large sets of nonlinear algebraic Irreducible subsets can further be decomposed by “tearing.. Y. Gannon. 17. 34 (1968). Gas-Solid Reactions. This process (usually denoted partitioning) In this paper a new tearing method for systems of nonlinear decomposes the system into “irreducible subsets” which cannot equations is presented. An algorithm for elimination of nonlinear expressions.. W.. L... N. No. Process Des. Sohn. maining nonlinear equations. plementary Volume. No. H.” ERDA Rpt. and L. (1979).. B. “Modeling of Entrained Manuscript received February 17. This method does not require formula be further partitioned.” Adv. 56. There are several number of equations is very time-consuming and may be even difficulties in applying tearing techniques to nonlinear systems. by selecting some of the variables as “tear these may be problems containing tens of thousand of linear and variables” and expressing the additional variables in the subset nonlinear equations. Chem.. Chem. variables as explicit linear functions of the tear variables.964 (1980). Eng. D.. 9. revision received January 7 . 131.. K.1982. Some of the nonlinear equations are linearized by re. J...684 (1979).” AZChE j . 18.

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