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Euler-Euler modeling

Berlin Institute of Technology

School of Process Sciences and Engineering

Department of Energy Engineering

Chair for Energy Process Engineering and Conversion Technologies for Renewable Energies

Fasanenstr. 89, 10623 Berlin, Germany

Abstract

In this article we present an application of reactive multiphase modeling with an EulerEuler model to the pyrolysis

of wood and the gasification of the emerged woodchar in a bubbling fluidized bed reactor. In addition to the gas

phase, which is as usual modeled as a continuum, the dispersed phases wood and woodchar are treated as independent

continuous solid phases. Woody particles are assumed to have a single fixed diameter while woodchar is classified in

two seperate phases with different diameters. We present computational results which have been run to a statistically

steady state. We compare results for some main gas components and the temperature at the outlet of the reactor with

experimental data from a labscale fluidized bed reactor.

Proceedings of the European Combustion Meeting 2009

600

42

1100

50

scale fluidized bed reactors using a relatively detailed gasification model for each individual particle. In a recent

study [16] used only 20 reactive coal, 2000 inert sand particles and simulation times of 2 s in their Euler-Lagrange

simulation of a bubbling fluidized bed.

134

Euler-Euler models allow a

realistic description of the time

dependent processes in non-reproduct

acting and reacting fluidized

gas

outlet

beds. Sofisticated closure models based on the kinetic theory

of granular flow allow realistic predictions of unsteady fluid

mechanical phenomena of particulate flows [1]. Compared

to Euler-Lagrange and Direct

Numerical Simulation models

continuum models are computationally less demanding and

allow the calculation of larger

reactors. Therefore they are

95

fuel

very useful tools for simulatinlet

ing fluidized beds. One of most

severe difficulties associated

with Euler-Euler models are the

complicated closure models deair

scribing the momentum and enFigure 1: Bubbling ergy transfer between multiple

continuous phases. Although

fluidized bed reactor.

they are limited to smaller systems, the more physical modeling approach of Euler-Lagrange methods are useful to

improve closure models for continuum models.

In this work we present an Euler-Euler model with

one gaseuos and three solid phases for the simulation

of reactive gassolid flow in dense fluidized beds. The

model takes into account detailed gas phase chemistry,

pyrolysis models, and heterogeneous gasification reac 50

Introduction

Over the last years the impact of utilizing fossil fuels

on the environment (e.g. green house effect) and their

limited availability became a more addressed problem in

the scientific community and in ecopolitical discussions.

While it is well known that charcoal was one of the most

popular combustibles since the medieval times, there still

is a lack of fundamental understanding of the complex

phenomena taking place during pyrolysis and gasification of biogenic energy resources such as wood. This

might be connected to the fact that measuring physical

important variables in a reactive solidgas flow is still a

challenge. As an example, even for nonreacting dense

gase solid flow it is still an unsolved problem to simultaneously measure the velocities of the gas phase and

the particulate phase on timescales of the particle collison dynamics. Therefore the ability to simulate reactive

multiphase fluidized beds is an important issue to investigate fundamental physical questions and to increase the

efficiency of biomass conversion as wood and charcoal.

Since fluidized bed reactors has been widely used in industry for conversion of coal there is of course quite some

experience with pyrolysis and gasification in these kind

of reactors.

There are numerous models which intend to simulate

fluidized beds reactors on different scales of accuracy.

The simpler models such as zone/cell models and equilibrium models are suitable for design optimisation of

industrial size gasifiers, the more comprehensive models

such as Euler-Euler [9, 1, 13] are more targeted towards

fundamental investigations of the chemical and fluid mechanical aspects of fluidized beds.

Euler-Euler or continuum models models are comprehensive models suitable for fundamental investigations of

the chemical and fluid mechanical aspects of fluidized

beds. The advantage of applicability to real industrial

systems is partly caused by neglecting information on individual particle level With current and foreseeable computer resources it does not seem feasible to perform other

tions. Different models for pyrolysis and gasification reactions from the literature have been implemented. We

apply the method for the numerical simulation of wood

gasification and compare the results against experimental

data of a laboratory scale bubbling fluidized bed reactor.

Reasonable agreement between the numerical results and

measurements have been found for the exhaust gas compositions and the temperature.

where sm , sm , and v sm are the void fraction, the density, and the velocity of the solid phase m, respectively.

Here, w sml denotes the mass transfer term between solid

phases m and l (e.g. the conversion of fresh wood into

charcoal) and w smg is the mass transfer term between

solid phase m and P

the gas phase component . With (1)

we have w s = m w smg . The momentum balance

for solid phase m can be written as

Mathematical model

Gas Phase. The gas phase in the EulerEuler model is

treated as a continuum, which can be described by the

volume averaged Navier-Stokes equations.

The species mass balance equations in the gas phase

can we written as

t

Nm

X

sm psm + sm

I ml + I mg + m mg . (6)

l=1

l6=m

where psm and sm are the pressure and the stress tensor of the solid phase m and I mg , I ml denote momentum

exchange terms between solid phase m and the gas phase

and the solid phase l. To close the system of mass and

momentum balance equations we solve an energy equation in temperature form for each solid phase m:

Tsm

+ v sm Tsm =

sm m cpm

t

q sm gm (Tm Tg ) Hsm .

g g Y

+ (g g Yu g ) = g w ,g + g w ,s . (1)

t

where Y denotes the massfraction of species in the

gasphase, w ,g is the net producton rate of species due

to gas phase chemical reactions, and w ,s is the mass exchange term between the solid phase and the gas phase.

Summing up equation 1 gives the global mass balance

for the gaseous phase in conservative form:

XX

g g

+ (g g u g ) =

g w ,s 0,

t

s

(2)

the following simple kinetic mechanism for syngas has

been used:

and the gas phase velocity, respectively.

The gas phase momentum equation is given by

g g u g

t

CO

2 CO

2 H2

CH4

+ (g g ug ug ) + g p

+ g ( g ) + g g g = I gs .

(3)

Nm

X

gm (Tsm Tg ) Hg .

well as the fixed mass-fractions of the products are taken

from [6]. Primary pyrolysis is followed by secondary

cracking of tar. In this study we consider two different

models for the secondary pyrolysis. In the first model of

[3] for beech wood, tar reacts to gas phase components

and inert tar:

(4)

The second pyrolysis model of [14] has been developed

for spruce wood. Primary and secondary pyrolysis in this

model can be summarised as follows:

the particulate phases are treated as a set of multiple continuous solid phases each having their own constant diameter. For solid phase m we solve a mass balance equation

[4]

[5]

[11]

[5]

between gas phase and solid phase m gm , the temperature of the solid phase Tsm ,and the heat of reaction Hg .

H2

+ CO2

2 CO2

2 H2 O

CO

+ 2 H2 O

of solid biomass gaseous components like wood gases

and tar and solid component char:

m=1

sm sm

+ (sm smv sm )

t

X

X

= sm

w sml + sm

w smg ,

The kinetic parameters for all reactions are from the cited

literature.

(modeled as a Newtonian fluid), the gravitational force,

and the momentum exchange between the gas phase and

solid phases, respectively.

The energy equation is solved in form of a non-conservative temperature equation:

Tg

g g cpg

+ v g Tg = q g v

t

+

+ H2 O

+ O2

+ O2

+ 1.5 O2

tar1 H2 O, CO, CO2 , H2 , CH4 , C2 H4 ,

C2 H 6 , C3 H 6

tar2 H2 O, CO, CO2 , H2 , CH4 , C2 H4 ,

(5)

2

C2 H 6 , C3 H 6 .

(7)

900

inlet

150 mm

325 mm

500 mm

700 mm

900 mm

800

temperature [C]

700

600

500

400

300

200

100

0

20

40

60

80

100

time [min]

120

140

160

180

complete run of the reactor at different heights.

Figure 3: Experimental data of the exhaust gas composition sampled from 19 different experiments with different

wood charges.

88 min operating time are due to an interrupted fuel supply. Between t=100 min and t=120 min the reactor runs

at almost steady state conditions. We use the data from

this time window to compare with numerical simulations.

After 120 min of operating time several tests were performed leading to the unsteady temperature data seen in

Figure 2.

Heterogeneous reactions. Heterogeneous reactions of solid

Figure 3 shows minimum, mean, and maximal meachar with species in the gas phase are modeled using the

sured exhaust gas concentrations. The concentrations are

following overall reactions:

sampled values of timeaveraged data from 18 different

C + O2

CO2

[15]

experiments with different charges and types of wood.

C + CO2 2 CO

[2], [8]

Usually, the exhaust gas concentrations of CO are higher

C + H2 O CO

+ H2

[7], [8]

then those of CO2 as can be seen from Figure 3. HowC + 2 H2 CH4

[7]

ever, among the 18 different experiments their were also

Rate expressions and kinetic parameters are taken from two case with higher CO2 than CO concentrations. The

the cited literature.

huge variance of wood properties (density, water content,

structure, etc.) leads to big uncertainties in the modeling

Results and Discussion

of wood gasification and should be kept in mind when

Experimental Setup. The experimental data in this study comparing numerical results against experimental data.

were taken from a laboratory scale bubbling fluidized bed

reactor at the Institute of Energy Engineering at Berlin Computational Setup. The reactor shown in Figure 1

University of Technology. Figure 1 shows the reactor and has been discretised in the two-dimensional Euler-Euler

its dimensions. The freeboard area and the bubbling bed model with a grid spacing of 1 cm in radial and axial dizone have inner diameters of 134 mm and 95 mm, respec- rection. Due to the residence time of the wood particles

tively. The reactor is operated at atmospheric pressure. in the fuel supply the temperature of the wood entering

The bed material consists of pure wood and is fed in the the reactor has been assumed to be 150 C. The gas comlower part of the reactor with a feeding rate of 2 kg/h. position entering the reactor through the fuel supply with

Preheated air with a velocity of 0.25 m/s at a tempera- a velocity of 4.5 cm/s has been set to be 100% H2 O at

ture of 400 C enters the reactor from the bottom over the T = 150 C. This massflow corresponds to complete drywhole diameter of the reactor. Six thermocouples inside ing of wood in the fuel supply. Inflow conditions for the

the reactor at heights 5, 150, 325, 500, 700, and 900 mm air are taken from the experiments. Three solid phases

above the air intake are monitoring the temperature inside have been used in the continuum model: spherical wood

3

the reactor. Product gases concentrations at the exit of particles (diameter 3 mm, density 6.5 g/cm , water content

10%,

volume

fraction

0.35,

molar

mass

128 g/mol),

the reactor are analysed with a combination of gas chroand

two

classes

of

spherical

char

particles

(diameter

1

matography and laser mass spectroscopy, see [12] for de3

and

2

mm,

density

0.35

g/cm

,

volume

fraction

0.35,

and

tails.

Figure 2 shows experimental temperature data over molar mass 12 g/mol) with carbon being the only contime at different heights above the inlet in the reactor for stituent. The walls of the reactor are modeled isothermal

a complete experiment. The reactor was started with a with a temperature of Tw = 600 K.

Figure 4 and 5 show the spatially averaged outlet tembed of pure charcoal and a pure heated nitrogen mass

perature

and volume fractions of H2 , CO, CO2 and H2 O

flow below the fluidization velocity to heat up the sysover

time

for the first secondary pyrolysis model. Both

tem. After the heating period of approximately 60 min

temperature

and volume fractions become statistically stathe reactor has been operated with heated air entering the

reactor with a velocity of 0.25 m/s and a temperature of tionary after a few seconds and show therefore that the

400 C. The temperature peaks seen in Figure 2 at about approximated initial conditions of the simulation are close

3

The introduction of an inert tar species is quite questionable since at higher temperature or longer hold-up time

one would expect to crack all the tar which evolves from

the primary pyrolysis but for this work we accepted this

components to be consistent with the used literature.

520

to the steady values. The model seems to have some difficulties to predict the experimental values shown in figure

3. Especially the CO concentration is to low copared to

the experimental data - a problem which is investigated

in recent simulation at the department. The concentration

of the species shown in figure 5 depend on various term.

Using different approaches for the main gasification reaction which result in the formation of water and carbon

monoxide shows mostly higher rates and, as these reaction are endothermic, higher cooling rate too. At the end

the bed would become coulder, less C02 and more CO

would evolve. Examples for different gasification kinetics are given in [8] and [10] where both of them using

kinitics which depend on the grade of conversion. This

problem is currently under investigation.

Figure 6 and 7 show again middled outlet temperature

and volumefractions of H2 , CO, CO2 and H2 O for the

second secondary pyrolysis approach. The result are similar but more Water evolves and even less carbon monoxide. The Temperature of the outlet gas is almost equal for

both models.

To show the strong connection of fluidmechanics and

chemistry we show the snapshots given in figure in 8. The

left picture in figure 8 shows bubbles rising in the bed

while both of the right pictures show a high concentration of CO2 in the bubble but a low concentration of CO.

The CO2 essentially evolves only from the wood and in

the very lowest part directly above the inlet, since only

there is oxygen. The bubble transport the CO2 through

the bed and constricts the CO2 to react with the charcoal

of the fluidized bed. Therefore less carbon monoxide is

in bubble.

Temperature [C]

500

300

350

400

450

200

250

time [s]

300

350

400

450

Temperature [C]

mole fraction []

450

500

mole fraction []

H2

CO

CO2

H2O

0.1

50

100

150

200

250

time [s]

300

350

400

450

500

References

[1] K. Agrawal, P. N. Loezos, M. Syamlal, and S. Sundaresan. The role of meso-scale structures in rapid

gas-solid flows. J. of Fluid Mechanics, 445:151

185, 2001.

0.05

150

400

Acknowledgements We gratefully acknowledge the Deutsche Bundestiftung Umwelt (DBU) for financial support

of this work and York Neubauer for the provision of the

experimental data shown in this article.

H2O

100

350

500

CO

CO2

50

300

Conclusions We have presented an EulerEuler modeling approach of wood gasification in a dense fluidized

bed. We have shown two different models for the secondary pyrolyis in a complex simulation of a polydispers fluidized bed reactor with homogeneous and heterogeneous reaction. The necessary time to simulate the

shown results was in the order of one week on two processor cores of an AMD Opteron running at 2.4 GHz clock

speed. Parallelization is done by are shared memory approach. Results given in this article agree partially well

with shown experimental data. In an upcoming publication we will present results of more pyrolysis and gasification models and a systematic investigation of the influences of grid resolution and boundary conditions.

0.1

0

0

250

H2

0.15

200

0.15

0

0

0.2

150

0.05

420

250

time [s]

100

0.2

440

200

50

460

150

time [s]

480

100

440

400

500

50

460

420

520

400

0

480

500

[2] M. J. Biggs and P. K. Agarwal. The CO/CO2 product ratio for a porous char particle within an incipiently fluidized bed: A numerical study. Chemical

Engineering Science, 52(6):941952, 1997.

[3] M. L. Boroson, J. Howard, J. P. Longwell, and W. A.

Peters. Product yields and kinetics from vapor phase

of biomass char gasification with carbon and steam.

Fuel, 84:885892, 2005.

[9] D. Lathouwers and J. Bellan. Modelling of dense

gas-solid reactive mixtures applied to biomass pyrolysis in a fluidized bed. Int. J. of Multiphase Flow,

27:21552187, 2001.

[10] F.. Mermoud, S. Salvador, L. Van de Steene, and

F. Golfier. Influence of the pyrolyis heating rate on

the steam gasification rate of large wood char particles. Fuel, 85:14731482, 2006.

[11] T. Mitani and F. A. Williams. Studies of cellular flames in hydrogen-oxygen-nitrogen mixtures.

Combustion and Flame, 39:169190, 1980.

[12] Y. Neubauer and F. Behrendt. Application of laser

mass spectrometry for a fast and detailed online tar

analysis in biomass gasification. In 15th European

Biomass Conference & Exhibition, pages 850854,

Berlin, May 2007.

[13] T. J. OBrien, M. Syamlal, and C. Guenther. Computational fluid dynamics simulations of chemically

reactive fluidized bed processes. In 3rd Int. Conf. on

CFD in the Minerals and Process Industries, pages

469474. CSIRO, Melbourne, Australia, December

2003.

[14] J. Rath and G. Staudinger. Cracking reactions of

tar from pyrolysis of spruce wood. Fuel, 80:1379

1389, 2003.

[15] I. B. Ross and J. F. Davidson. The combustion of

carbon particles in a fluidized bed. Chemical Engineering Research and Design, 60a:108114, 1982.

Figure 8: Snapshots of the volumefraction of the gas, volumefraction of CO and CO2 (from left to right)- pyrolysis

model 2, dark stays for higher gas, C02 and CO fractions

of coal combustion in a bubbling fluidized bed. Part

II: coal combustion at the particle level. Chemical

Engineering Science, 59:42054215, 2004.

35:120128, 1989.

[4] M. L. De Souza-Santoz. Comprehensive modelling

and simulation of fluidized bed boilers and gasifiers.

Fuel, 68(12):15071521, 1989.

[5] F. L. Dryer. High Temperature Oxidation of CO

and CH4 in a Turbulent Flow Reactor. PhD thesis, Princeton University, Aerospace and Mechanical Sciences Department, Princeton, New Jersey,

USA, 1972.

[6] M. Gronli and M. Melaaen. Mathematical model for

wood pyrolysis-comparison of experimental measurements with model predictions. Energy & Fuels,

14:791800, 2000.

[7] M. L. Hobbs, P. T. Radulovic, and L. D. Smoot.

Modeling fixed-bed coal gasifiers. AIChE Journal,

38(5):681702, 1992.

5

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