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**Interpretation of residence time distribution data
**

A. D. Martin*

North West Water Ltd, Dawson House, Liverpool Road, Warrington WA5 3LW, UK

Received 26 November 1998; received in revised form 15 November 1999; accepted 27 March 2000

Abstract

`Tracera or Residence time distribution (RTD) studies are commonly exploited as a means of developing an understanding of the

`mixinga status of vessels of various types. The e!ort involved in the setting up of such plant studies can be considerable and the

execution of the experiment its self is often a test of endurance. In the past full interpretation of the results has not been easy and as

a consequence super"cial treatments have been employed. This paper presents an alternative method for interpreting RTD data,

which is relatively easy to use and addresses some of the weaknesses of more conventional methods. An extention to the `tanks in

seriesa concept is presented (ETIS) and united with the `reactor networka formulation. The suitability and appropriateness of the

model is discussed and compared with the `closeda dispersion model 2000 Published by Elsevier Science Ltd. All rights reserved.

Keywords: Residence time; Tanks in series; `Closeda system; Networks; Comparison; Case studies

1. Introduction

Diagnosis of the operational ills and the characterisa-

tion of new equipment at both pilot and full scale are

common activities in the process industries. An impor-

tant component in the diagnosis or characterisation pro-

cess is an understanding of the vessel hydrodynamics,

which at a global or `black boxa level may be gained

from the interpretation of the vessel residence time distri-

bution (RTD). One of the many drivers for the character-

isation arises from the need to simulate process responses

to unusual operating conditions. Many reactor models

encoded within dynamic simulation packages such as

STOAT'` GPSX'` and SPEEDUP'` are capable of

using information regarding the RTD of the vessel under

consideration to improve the "delity of the model. Typi-

cally these models employ parameters such as the Peclet

number (Pe), the dispersion number (N

"

) or the number

of tanks in series (n

2

) in conjunction with the mean

residence time (¹

0

) to describe deviations from the ideal

continuous stirred tank reactor (CSTR) or the plug-#ow

reactor (PFR). The reactor models avoid the necessity of

employing complex computational #uid dynamics by

restricting their consideration to a single characteristic

* Now at: Environmental Technology Centre, Department of Chem-

ical Engineering, OMIST, Manchester M60 1QD, UK. Tel.: #44-161-

200-4340.

E-mail address: Alaistair.martin@OMIST.ac.uk (A. D. Martin).

length. These models are consequently one dimensional

in form.

2. One-dimensional models

There have been many models of this type designed to

interpret deviations from the two ideal extremes. The

entire family of models may be said to describe dispersed

plug-#ow reactors (DPFR). The magnitude of the disper-

sion as quanti"ed by N

"

increases from zero in the PFR

to in"nity in the CSTR. The `opena and `closeda disper-

sion models fall into this family as does the tanks in series

(TIS) model.

The **open++ dispersion model considers the axial

motion of a #uid element to be made up of two compo-

nents:

1. The convective component arising from the bulk

motion of the #uid.

2. The di!usive component arising from the random

motion of the element in response to the decay of

turbulent eddies.

This concept is expressed mathematically by the con-

ventional `di!usion with bulk #owa equation (Eq. (1)).

cC

c0

"

D

u¸

c`C

cz`

!

cC

cz

, (1)

0009-2509/00/$- see front matter 2000 Published by Elsevier Science Ltd. All rights reserved.

PII: S 0 0 0 9 - 2 5 0 9 ( 0 0 ) 0 0 1 0 8 - 1

where the dimensionless group

D

u¸

"N

"

"

1

Pe

(2)

and

0"

t

¹

0

"

Q

0

t

<

0

"

ut

¸

(3)

The `opena boundary conditions from which this model

draws its name de"ne the #ow condition at the reactor

inlet and outlet. The `opena condition is physically

achieved when the #ow is undisturbed at the inlet and the

outlet. In 1957 Levenspiel and Smith published the ana-

lytical solution to Eq. (1) for the `opena boundary condi-

tions (Levenspiel & Smith, 1957). This solution is shown

in Eq. (4).

E(0)"

C

C

B

"

1

2

Pe

0

e

.C'¹F'

`

"F

(4)

Where C

B

is the concentration that would have been

obtained had the `dyea been evenly dispersed through-

out the vessel under study.

With mean and variance

0M

"

"1#

2

Pe

, (5)

o`

"

"

2

Pe

#

8

Pe`

, (6)

It can be seen that the mean of this distribution is

a function of the dispersion and at high dispersion (low

Pe) the mean is substantially '1. This result appears to

be inconsistent with the mass balance but may be ex-

plained by the di!usion of `dyea upstream of the injec-

tion point. Thus, the pulse injected at the inlet is not the

same as the pulse which would have been measured at

the inlet. Casual observation of the inlet to and exit from

a high-dispersion reactor would also con#ict with the

assumed `opena boundary conditions. The rigorous

mathematical de"nition of the `opena boundary condi-

tions makes this model more di$cult to use than the

tanks in series formulation as the user is often left in some

doubt as to the degree to which the `opena condition is

achieved in the system under investigation.

The **closed++ dispersion model treats the system in

exactly the same fashion as the `opena dispersion model.

Eq. (1) is solved with the `closeda boundary conditions.

The `closeda boundary conditions relate to the physical

situation in which the #ow approaches the inlet to the

reactor in idealised plug #ow (Pe"R), transforms to

dispersed #ow within the reactor and returns to idealised

plug #ow at the exit. This situation is very closely ap-

proximated in many real reactors even those which are

themselves low dispersion devices. Thomas and McKee

(1944) published the analytical solution with `closeda

boundary conditions in 1944. Their solution, published

in a dimensional form, is reproduced here in non-dimen-

sional form (Eq. (7)) to maintain consistency with Leven-

spiel and Smith's `opena solution (Eq. (4)). Yagi and

Miyauchi reproduced the Thomas and McKee solution

in 1953 with an alternative condensation of the terms

(Yagi & Miyauchi, 1953).

E(0)"

C

C

B

"2

L¯`

L¯¹

Pe:

L

e.C`

¦

¹F'?

`

L >¹'`

¦

Pe(:`

L

#1)#4

:

L

cos

Pe

2

:

L

#sin

Pe

2

:

L

, (7)

where :

L

is given by the positive roots of Eq. (8).

tan

Pe

2

:

L

"

2:

L

(:`

L

!1)

. (8)

Levenspeil (1972) published expressions for the mean and

variance of the `closeda system RTD though did not

report the analytical solution for the RTD itself. Leven-

spiel's mean and variance can be shown to be equal to

those of Eq. (7) thus con"rming their association. These

results are shown below Eq. (9) for the mean,

0M

!

"4

L¯`

L¯¹

K

L

Pe`(:

L

#1)`

L¯`

L¯¹

K

L

Pe(:

L

#1)

"1 (9)

and Eq. (10) for the variance.

o`

!

"32

L¯`

L¯¹

K

L

Pe`(:

L

#1)`

L¯"

L¯¹

K

L

Pe(:

L

#1)

!1

"

2

Pe

1!

(1!e.C)

Pe

, (10)

where K

L

is given by Eq. (11)

K

L

"

2Pe:

L

Pe(:`

L

#1)#4

. (11)

Satisfactory enumeration of Eq. (7) becomes increasingly

di$cult at higher values of Pe. This di$culty derives

from the relative magnitudes of the early terms in the

series with respect to the later terms and the "nal sum.

When 0"0 the series itself is non-convergent with suc-

cessive terms oscillating as the following.

lim

L"

(S

L

)"2(!1)'L¹'e.C`. (12)

At a practical upper limit of Pe"33 a conventional

double precision summation will yield a residual of less

than 0.00005 at 0"0.001 but will require some 300 terms

to achieve this.

5908 A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917

Fig. 1. Exit age distributions of the tanks in series model for 1 and

2 tanks in series.

Fig. 2. Comparison of the tanks in series model with the closed disper-

sion model with a common variance of 0.5.

The tanks in series model seeks to describe the #ow in

a reactor system by considering it to be discretised into of

a strand of equal-sized hypothetical CSTRs. Each hypo-

thetical CSTR is independent of those preceding or fol-

lowing it. The number of tanks in series n

2

describes the

dispersion with n

2

"1 representing in"nite dispersion

and being equivalent to Pe"0. Integration of a simple

dynamic mass balance around the strand of reactors

readily yields the system RTD (Eq. (13)). Eq. (13) is also

the de"nition of the Erlang distribution.

E(0)"

C

C

B

"

nL2

2

(n

2

!1)!

0'L2¹'eL2F. (13)

With mean and variance

0M

2

"1, (14)

o`

2

"

1

n

2

. (15)

Conceptually, the development of this model is easy to

follow. It also has the advantage that the precise de"ni-

tion of the inlet and exit boundary conditions is not

required. Similarly concerns regarding the method of

`dyea injection and measurement do not arise. Phys-

ically, this model is at its best when the number of tanks

in series is low and concerns over the appropriateness of

either `opena or `closeda boundary conditions are at

their height. This model however has a signi"cant draw-

back when n

2

is small due to the integer constraint.

Fig. 1 shows that the E curve for n

2

"1 di!ers very

signi"cantly from that resulting from n

2

"2. Many real

CSTRs exhibit RTDs which lie in this range and are

therefore only characterised very approximately by the

tanks in series model. Frequently in the interpretation of

RTD data n

2

has been related to Pe or N

"

via the

variances of the RTDs (Eqs. (10) and (15)). This is tanta-

mount to assuming that the tanks in series model and the

`closeda dispersion model are equivalent. Elgeti (1996)

develops an alternative relationship between the two

RTD forms by following the progress of an arbitrary

reaction and expanding the dispersion equation in

Taylor series. This analysis leads to the following equiva-

lence relationship for Pe:

Pe"2(n

2

!1). (16)

Kramers and Alberda (1953) also proposed this equiva-

lence. Fig. 2 shows quite clearly that for the variance

equivalence, n

2

"2 and Pe"2.557, respectively,

the RTDs are quite di!erent. A plot generated for the

`Kramers, Alberda and Elgetia equivalence shows very

similar behaviour though the co-location of the peaks is

slightly poorer than illustrated in Fig. 2. The `closeda

dispersion model exhibits a considerably higher peak

value than the tanks in series model. This di!erence

reaches a maximum at n

2

"2, Pe"2.557. The `closeda

dispersion model can also be seen to exhibit a region with

a positive second derivative at 0(1 which is absent from

the tanks in series model. At values of n

2

'15,

Pe'28.97 the di!erence between the two maxima is less

than 5% and is likely to be di$cult to resolve experi-

mentally. Thus for practical purposes the two models are

su$ciently similar to be regarded as the same. The tanks

in series and `closeda dispersion models however di!er

signi"cantly from the `opena dispersion model under the

same conditions.

3. Extended tanks in series

If the tanks in series model is merely regarded as

a residence time distribution function, whose form de-

pends solely on the value of the parameter n

2

, and is

freed from the arti"cial need to have a physical manifes-

tation, it becomes possible to address the quantisation

issue arising in the analysis of high-dispersion systems.

Simply introducing the concept of a non-integer number

of hypothetical tanks in series will achieve the desired

result. The exit age distribution or E curve of the

A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917 5909

Fig. 3. Thread and knot concept for the tractor network model.

extended tanks in series (ETIS) model is given by a subset

of the gamma distribution family (Eq. (17)).

E(0)"

nL2

2

I(n

2

)

0L2¹eL2F. (17)

When n

2

is integer it is identically equal to the Erlang

distribution (Eq. (11)). As with the Erlang distribution the

mean and variance are given by Eqs. (14) and (15). The

ETIS model removes the problem of quantisation which

occurs as n

2

tends to 1 in the tanks in series model.

4. Reactor network structure

The models described in the previous sections are all

one dimensional in their nature and are consequently

unable to describe gross structure in the #ow within

a reactor. To describe such large scale structures in the

#ow pattern it is necessary to introduce appropriate

large-scale structure to the model. Many model struc-

tures have been proposed to describe a range of physical

#ow con"gurations (Levenspeil, 1972; Monteith

& Stephenson, 1981; Smith, Elliot & James, 1993). To

date the fundamental building blocks or `threadsa of

these reactor networks have been limited to either ideal

CSTRs or ideal PFRs. Algebraic expressions for the

C and E curves of some of the simple con"gurations have

been derived (Levenspeil, 1972; Monteith & Stephenson,

1981). The technique for generating the model RTD for

the majority and the more complex networks involves

the numerical integration of the dynamic CSTR mass

balance Eq. (18) (Smith et al., 1993).

dC

dt

"

(C

G

!C)

¹

(18)

Clearly to describe real DPFRs using simple CSTR or

PFR building blocks requires large numbers of the fun-

damental unit and the numerical integration of reactor

network models becomes inordinately cumbersome as

the extent of the network grows. The use of the CSTR as

the basic building block also constrains the network

description to integer values of n

2

. Employing the ETIS

model to characterise the basic building block signi"-

cantly reduces the complexity of network required whilst

simultaneously relaxing the integer n

2

constraint. To-

gether these advantages dramatically improve the tracta-

bility of the data analysis problem. The reactor network

structure is developed further in the following sections to

facilitate the description of `reala vessels exhibiting com-

plex composite dispersion behaviour with bypassing and

stagnant zones.

The network dexnition: The reactor network structure is

constructed from two component types.

1. Threads,

2. Knots.

These components serve to de"ne the volume elements

of the reactor and their connectivity, respectively. The

`threadsa receive #ow from an up stream or source

`knota and discharge to a down stream or sink `knota.

The characteristics of the `threadsa are de"ned by the

#ow through the thread its hypothetical volume and exit

age distribution (Q, <, E). The `knotsa receive #ows from

source `threadsa and distribute the summed #ow to the

sink `threadsa and are de"ned as zero-volume blender

splitters. The `knotsa are characterised by a single-#ow

split fraction parameter ( f

Q

). A number of assumptions

are implicit in this basic de"nition of the network.

1. Individual `threadsa are assumed to be fully seg-

regated from each other.

2. The exit age distribution of an individual `threada is

given by the convolution of the composite E curve

passed by the source `knota.

3. The composite E curve passed at any `knota is given

by the linear #ow weighted sum of the E curves of the

contributing `threadsa.

4. There is no dispersion through `knotsa.

Assumptions 1 and 4 are likely to be the most conten-

tious, particularly when considering reaction kinetics in

conjunction with the RTD. They are however critical to

the formulation of a manageable problem. Clearly within

the context of assumption 4 the choice of model for the

characterisation of dispersion is restricted to the `closeda

dispersion model, the TIS model and the ETIS model.

Despite the reservations expressed above the ETIS model

is used to illustrate the concept of the network.

Fig. 3 shows a network of three `threadsa connected

together in to two #ow paths or `strandsa by three

`knotsa. This type of network is a common result of

interpreting the RTD of a large shallow packed bed

reactor. This type of network di!ers from those employed

by previous authors (Levenspeil, 1972; Monteith

& Stephenson, 1981; Smith et al., 1993) in that all

`threadsa accommodate dispersed #ow.

5. Experimental data interpretation

Data Gathering. There are four general types of experi-

mental protocol for the conduct of `dye tracera

5910 A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917

experiments. The classical experimental technique in-

volves the injection of a Dirac function pulse of `dyea

followed by the measurement of its concentration as it

emerges in the outlet stream over an extended period of

time. This method produces a readily interpretable result

and maximises the potential for resolving the detailed

structure of the experimental exit age distribution.

A common alternative technique employs a `stepa input.

This technique generates the reactor F curve, which may

be di!erentiated to yield the E curve. Direct di!erenti-

ation of experimental data results in the ampli"cation of

noise arising from sampling and analytical methods.

Curve "tting to the integrated form or F curve may also

lead to poorer estimates of the parameters. This arises

because detailed features are less distinctive on the

F curve than on the E curve. A third experimental proto-

col involves the injection of a `blocka input. This method

is considerably inferior to the two previous methods. The

experimental exit age distribution obtained from this

technique is a hybrid lying between the classical E and

F curves. The duration of the `blocka tends to produce

a broad peak and damp out the detailed structure, which

would have been revealed by a function pulse input.

A "nal technique involves the analysis of a natural ran-

dom signal in the input stream. This technique has the

advantage of not altering the process stream but su!ers

from the same disadvantages as the `blocka input tech-

nique. The AWWA guide (Teefy, 1996) o!ers advice on

the conduct of `dye tracera tests in water and waste-

water treatment plants particularly with respect to the

selection of suitable `dyesa.

Data processing. Historically the interpretation of

experimental RTD data has been rather super"cial

(Tomlinson & Chambers, 1979). Often this interpretation

has been limited to extraction of the mean and variance

of the data set (Eqs. (19) and (20)).

¹

C

tM

C

"

C

L

t

L

At

L

C

L

At

L

, (19)

o`

C

C

L

t`

L

At

L

C

L

At

L

!tM`

C

. (20)

The sequential nature of the data gathering guarantees

the collection of biased data sets. So whilst for randomly

gathered data fairly modest sample sizes are su$cient to

obtain good estimates of the population mean and vari-

ance this is not the case for RTD data. It can be seen that

Eq. (19) is acutely `tail sensitivea, thus early truncation of

the data set leads to serious under estimation of the

population mean or achieved mean residence time. To

overcome this problem protracted measurement periods

are usually prescribed. Typical measurement periods are

chosen to be of the order of 3}5 times the mean residence

time with the need for longer periods coinciding with

highly disperse systems. Furthermore tM

F

is an estimate of

the mean of the RTD. It is therefore only an estimate of

the mean residence time when the `closeda dispersion,

TIS or ETIS models are appropriate.

The estimates obtained from Eqs. (19) and (20) have

often been related to the dispersion number (N

"

) or the

number of tanks in series (n

2

) via Eqs. (10) and (15) with

little regard to the overall shape of the RTD. A number of

additional empirical relationships have also been de"ned

to characterise the dispersion in reactors:

p

&

"

t

¹"

tM

, (21)

I

+

"

t

""

t

¹"

, (22)

I

"1!

t

K

tM

. (23)

Smith et al. (1993) examined these indices and found

them to be mutually inconsistent when used to describe

their data. These indices may be consistently related to

the variance of the RTD only in circumstances when the

distribution is symmetrical, i.e. very low dispersion or

plug #ow. This situation rarely coincides with the occa-

sions when the departure from plug #ow is important.

6. Selected case studies

The ETIS model has been used in the following case

studies to provide the quanti"cation of the dispersion

within an individual `threada. This has been done be-

cause of the ease of application and despite concerns

regarding strict validity at intermediate values of Pe. The

curve-"tting process has been conducted on Microsoft

EXCEL 97 using the built in SOLVER and mathemat-

ical functions. The built in functions were also supple-

mented with visual basic for applications (VBA) code

developed by the author.

Simulated very large CSTR. The reactor under study

consisted of a nominal 1500 m` cuboid vessel with

a multi-ported inlet manifold located at the bottom of the

vessel and an outlet weir located on the opposite wall.

Fig. 4 shows a schematic elevation of the vessel which

was nominally 19.5 m in the axial direction by 19.5 m

wide by 4 m deep. The inlet manifold directed the feed

#ow across the #oor of the reactor underneath a grid of

aeration equipment. The process feed rate was

0.0523 m`/s. The reactor was simulated using a commer-

cial CFD package and an `experimentala RTD

generated using a particle tracing technique. Several ap-

proximations were made in the construction of the CFD

model of this reactor:

1. The vessel was assumed to be semi-in"nite (normal to

the direction of #ow).

2. The feed manifold was modelled by a continuous

axially pointing slot at the foot of the feed wall.

A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917 5911

Fig. 4. Schematic vertical section through the simulated very large

CSTR.

Fig. 5. Early period exit age distribution for the simulated very large

CSTR showing contributions from the component threads.

Fig. 6. Complete exit age distribution for the simulated very large

CSTR.

Fig. 7. Reactor network to model the exit age distribution of the

simulated very large CSTR.

3. A 300 mm wide #ow section with `periodica boundary

conditions was assumed to be su$ciently large to

model the expected #ow structure.

Preliminary inspection of the early period results

(Fig. 5) shows clearly a delay of approximately 20 min

before a signi"cant concentration of `dyea is found in the

exit. The delay is followed by a steady increase to a max-

imum at approximately 100 min elapsed time. These gen-

eral characteristics suggest a candidate framework

capable of describing the exit age distribution and

E curve. Additional threads are added to the network by

analysis of the residual after attempting to "t the model

to the data. The analysis of the residual must be under-

taken with some care as the degrees of freedom are

successively reduced with the addition of each new

thread. Equally, the inherent noise in the data arising

from measurement errors must be considered. The solid

line in Figs. 5 and 6 presents the E curve generated as

a result of this process. The broken lines show the #ow

weighted E curves of the individual threads. Fig. 7 illus-

trates the "nal network structure synthesised to describe

the data.

The theoretical hydraulic residence time of this vessel

T

0

is 484 min and the mean of the "tted residence time

distribution ¹

0

is found to be 509 min. The estimate of

¹

0

obtained from the `experimentala data set tMis found

to be 476 min. The data set from which this estimate is

made extends to 1620 min or 3.4 residence times. The "ve

`threada model proposed in Fig. 7 satisfactorily describes

the `experimentala data. The dominant #ow strand

consists of a plug-#ow `threada and a large CSTR

`threada. Together these account for the vast majority of

the vessel volume. Two small additional `threadsa are

required to describe the small by-pass #ow around the

large CSTR volume. The "fth `threada describes the

`deada volume. This technique is unable to order con-

secutive `threadsa. However, with knowledge of the reac-

tor geometry a considered assignment may be made. In

this instance the plug #ow section is placed "rst and its

characteristics are attributed to the region de"ned by the

decaying feed `jeta underneath the aeration grid. From

Fig. 7 it can be seen that `threadsa 1 and 4 are very

similar in character. This suggests that thread 4 is a por-

tion of the feed `jeta which by-passes the well-mixed

region. This may be considered to be a portion of the

#uid that travels the full length of the reactor underneath

the aeration grid and then ascends the end wall to the exit

weir. Such a #ow strand would have failed to interact

with the air bubbles in the reactor and would therefore

remain un-converted. A similar argument may be ad-

vanced to describe `threada 3. Together `threadsa 3 and

5 represent 5% of the #ow through the vessel. Thus,

based on the above argument this reactor would be

unlikely to achieve greater than 95% conversion.

The mean of the `experimentala data tM is remarkably

close to the value of T

0

. This situation is di$cult to

5912 A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917

Fig. 8. Schematic vertical section through the packed bed reactor.

Fig. 9. Exit age distribution for the packed bed reactor.

Fig. 10. Reactor network to model the exit age distribution of the

packed bed reactor.

support given the truncation of the data set at 3.4 resi-

dence times. Integration of the complex model E curve

over 1620 min (3.4 residence times) reveals an expected

98% `dyea recovery. It also provides an estimate of the

mean based on a truncated portion of the E curve. This

estimate is found to be 473 min which is in close agree-

ment with tM. On the basis of these consistency checks

509 min estimated from the consideration of the whole of

the "tted distribution is likely to be reliable. Practically,

neither ¹

0

'T

0

nor negative dead volume fraction

(`threada 5) can be supported and may be indicative of an

error in either the #ow or volume speci"cation of the

model region. Such errors may arise from the numerical

handling of symmetrical or periodic boundary condi-

tions. The CFD model also predicts a signi"cant fraction

of the vessel to exhibit an occluded volume exceeding

5%. This is attributed to the presence of bubbles. The

expected e!ect is to reduce the value of ¹

0

relative to

T

0

since the reactor network interpretation of the bubble

cloud is as dead volume. Hence the expected dead vol-

ume fraction is of the order of 5% rather than the !5%

estimated by the network model analysis.

Packed bed reactor. Fig. 8 shows a schematic vertical

section through this reactor, which consists of a 5 m by

5 m by 4.150 m deep cuboid vessel with 2.2 m depth of

bouyant granular packing operated in up #ow. The feed

enters the lower distribution chamber, then passes up

through the packed bed and hold down plate into an

upper collection chamber before discharging from the

reactor via wall mounted weirs. A second reactant is

introduced into the base of the packed bed and #ows in

co-current mode through the packing. The dumped

packing has a void volume fraction of approximately

55%.

Visual inspection of the experimental data (Fig. 9)

shows a delay in the detection of the `dyea in the outlet

stream and a substantial tail on the RTD. This suggests

that the reactor requires a minimum three `threada

model for characterisation. This model is shown in

Fig. 10. The reactor con"guration however suggests that

a four `threada model may be more suitable from a phys-

ical standpoint. Both models were constructed to ascer-

tain the improvement in "delity between a two `threada

model and a three `threada model. The overall improve-

ment was found to be insigni"cant with respect to the "t

to the experimental data. However, comparison of the

characteristics of the individual threads o!ered further

insights into the possible structure of the operating bed.

The low-dispersion `threada,1 in each model, was un-

changed between the 3 and 4 `threada models but the

high dispersion `threada of the 3 `threada model split

into 2 CSTR `threadsa in the 4 `threada model. It may be

inferred that the low dispersion `threada 1 models the

region in the reactor that is occupied by the packed bed.

However, the void volume of the packed depth is consis-

tently underestimated by approximately 20%. The

volume estimates of the high-dispersion regions are

equivalently high. The description of the high-dispersion

region by the 4 `threada model is particularly interesting

since the over estimate of the volume is con"ned to

a single `threada. The placement of the `knota between

`threadsa 2 and 3 coincides with the operating volume of

the upper collection chamber. By elimination the over

estimated `threada is assigned to the lower distribution

volume. The relative under and over estimates of the

volumes in this part of the reactor may be attributed to

2 causes:

1. Failure of the model to adequately describe the condi-

tions at the interface between the distribution volume

and the packed region.

2. Interaction between the lower portion of the packed

bed and the distribution volume such that a propor-

tion of the bed is disturbed.

The reactor network model assumes that there is no

dispersion through `knotsa which is likely to be valid

A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917 5913

Fig. 11. Schematic plan of the internally recirculating CSTR.

Fig. 12. Exit age distribution for the internally recirculating CSTR.

Fig. 13. Reactor network to model the exit age distribution of the

internally recirculating CSTR.

within the reactor if either the feed or discharge `threadsa

exhibit low dispersion. Whilst this assumption is imper-

fect at Pe"17 the error introduced is insu$cient to

describe the phenomenon observed in the analysis. The

corollary of this is that the placement of the model

`knota does not coincide with the expected physical

boundary between the packed bed and the distribution

volume. This was con"rmed by the observation of in-

stabilities at the interface between the packed bed and the

lower distribution volume. Particles occupying the lower

300 mm of the packing were observed shearing o! the

bed and temporally dispersing in the distribution vol-

ume. Thus both the 3 and 4 thread models have identi"ed

the stable packed bed only as a low-dispersion region.

Since the objective of this study was to characterise the

active portion of the reactor, the 3 `threada model is

adequate.

Internally recirculating CSTR. This reactor consists

of a 12 m wide by 3.1 m deep oval channel with a

centre line length of 236 m and an operating volume of

approximately 8200 m`. Fig. 11 shows a plan view sche-

matic of the vessel. The feed is introduced through the

outer perimeter wall and the discharge exits via the

interior perimeter wall approximately ¹

`

of a lap down

stream of the feed position. Clockwise internal circula-

tion is mechanically induced by a system of surface

paddles.

The experimental procedure involved the injection of

a delta function pulse into the feed followed by a long tail.

This is indicated in Fig. 12 by the closed circles. The long

tail arises from the entrapment of `dyea in an external

recycle. Entrapped `dyea passes through a number of

external unit operations before returning to the feed. The

original delta function input is very heavily damped and

the intermittent peaks observed in this trace cannot be

attributed to this source. It is more probable that these

peaks arise as a result of random #ushing of residual

`dyea from the reactor inlet chamber where the original

injection was made.

The experimental output trace, open circles in Fig. 12,

shows two distinct patterns of behaviour. The early peri-

od behaviour extending from 0"0.0}0.6 shows clear

periodicity with decaying amplitude. The late period

behaviour extending from0"0.6 onward shows approx-

imate exponential decay. Based on the form of the input

trace and the observed response the experimental data

was modelled in two parts.

1. The response to the delta function input was modelled

in detail by the network shown in Fig. 13.

2. The response to the long tail was modelled solely on

the aggregated system behaviour, i.e. an exponentially

decaying RTD.

A calculation method for this type of reactor network

model is described by Battaglia et al. with reference to

land "ll leachate (Battaglia, Fox and Pohland, 1993). The

high dispersion of the Battaglia et al. system required

fewer than 10 terms of their series solution to achieve

a satisfactory result. In this work the development fol-

lowed a route equivalent to Battaglia et al. with the series

summation being implemented in (VBA). The recycle was

opened out and the circulating #ow considered to be

made up of a number of parallel `threadsa. Each `threada

was considered to represent the fraction of #uid entering

the reactor and completing a constant fraction of a lap

plus an integer number (s) of additional laps before exit-

ing. The general concept is illustrated in Fig. 14 together

with the recurrence relationships for the `threada para-

meter values. The numerical subscripts in Fig. 14 relate

to the parameters in Fig. 13. The total number of parallel

5914 A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917

Fig. 14. Numerical equivalent network for the evaluation of the inter-

nally recirculating CSTR model.

threads considered (c) was determined by a precision

criterion given by Eq. (24).

c"1#Int

log

¹"

(p)

log

¹"

1!

¹

`

#¹

`

¹

0

, (24)

where the numerical subscripts refer to the `threada

numbers in Fig. 13.

Analysis of the experimental data resolved the peri-

odicity in the early period to be 11.55 min (0.061¹

0

).

However the expected "rst peak at 4.75 min (0"0.025) is

almost completely absent from the experimental data.

The "rst strong peak is detected at 16.3 min (0"0.086).

This result has two possible explanations.

1. The sampling frequency at the outlet was insu$ciently

high to resolve the peak.

2. The dispersion normal to the direction of #ow was

incomplete.

A simple test to check the possible sample frequency

explanation indicates that at least two samples would

have been gathered which contained signi"cant concen-

trations of `dyea. This test indicates that the samples

collected at 4 and 6 min (0"0.0211 and 0.0316) are those

a!ected and the expected concentration of `dyea is likely

to be double that observed in any of the samples prior to

the "rst signi"cant peak. Whilst this test is not conclusive

the result suggests that incomplete normal dispersion is

the more likely explanation. Based upon these deduc-

tions the derived reactor network structure and para-

meter values are given in Fig. 13. The aggregated or late

period behaviour of this model is as expected equivalent

to a CSTR (n

2

"1) with a mean residence time of

¹

0

"190 minutes. The convolution of the long tail of the

input trace with the CSTR characteristics describes the

late period behaviour of the experimental RTD very

satisfactorily.

7. Discussion

Suitability of ETIS model. From a theoretical stand-

point the ETIS model may be criticised because of its

lack of rigour with respect to the inlet and exit boundary

conditions. It is however this lack of rigour which makes

the model easy to use particularly in circumstances of

high dispersion. The extension of the classical tanks in

series model into the continuous (ETIS) form also con-

tributes to the ease of use since it becomes possible to use

simple optimisation algorithms for the interpretation of

experimental data. The ETIS model also eliminates the

quantisation e!ects observed in the tanks in series model

at low n

2

. The elimination of these e!ects is a signi"cant

advantage since it is at low n

2

or Pe that the tanks in

series analogy is at its most useful. To achieve an equiva-

lent removal of quantisation using the tanks in series

model requires the addition of further `threadsa to the

network with independent residence times.

Hitherto, the absence of a solution to the `closeda

dispersion model has been widely accepted. This solution

was however published by Thomas and McKee in 1944.

The rigorous handling of the inlet and outlet boundary

conditions is a signi"cant bene"t relative to the ETIS

model and unlike the `opena dispersion model does not

add to the di$culty of use. The series solution presented

in their paper is however numerically intensive in use and

becomes practically non-convergent at low values of

0 and high values of Pe. Frequently in the past the tanks

in series model has been assumed equivalent to the

`closeda dispersion model. The equivalence has been

established by equating the respective variances (Eqs. (10)

and (15)). This assumption has been shown to be false

except under the condition n

2

"1 and Pe"0. Practic-

ally however the di!erences become small enough for the

distributions to be regarded as the same when n

2

'15

and Pe'28.97. The di!erences between the two distri-

butions are such that, for a chosen variance or equivalent

pair of n

2

and Pe values, the reactor design based upon

the ETIS model yields a slightly larger volume than that

based on the `closeda dispersion model. This arises from

the more `peakya nature of the `closeda dispersion

model RTD. The `closeda dispersion model predicts that

signi"cantly more material is discharged from the reactor

with an exit age between 0.25 ¹

0

and ¹

0

.

The ETIS model as applied in the three case studies

has provided very satisfactory "ts to the experimental

data. There are few areas in which the application of the

more numerically intensive `closeda dispersion model

would practically bene"t the interpretation of the data.

Thread 3 of the simulated very large CSTR may describe

the data better if the `closeda dispersion model were

used. This `threada, though, accounts for less than 3% of

the reactor throughput and the value of n

2

(22) is toward

the upper end of the range in which the ETIS

and `closeda dispersion models di!er signi"cantly.

A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917 5915

Application of the `closeda dispersion model to `threada

1 of the packed bed reactor network may improve the "t

to the experimental data in the region 0.2(0(0.3 and

0"0.75. However, as can be seen from Fig. 9 the scope

for improvement is small.

Dispersion at knots. A basic assumption of the reactor

network structure is that there is no dispersion through

the `knotsa. This assumption is completely consistent

with the application of the `closeda dispersion model to

characterise the interconnecting `threadsa. Such a high

level of consistency cannot be claimed for the use of the

ETIS due to the lack of rigour in the de"nition of the inlet

and outlet boundary conditions. The implied assump-

tions for the tanks in series model relate to the inlet and

outlet of a CSTR and would indeed be consistent with

the no dispersion through the `knotsa assumption. The

same implicit assumption is made in the ETIS model but

is conceptually di$cult when n

2

is not an integer.

The extent of dispersion through the `knotsa is only

likely to be signi"cant where both source and sink

`threadsa are themselves characterised by high disper-

sion. The qualitative e!ect of removing the central `knota

joining 2 CSTR `threadsa is shown in Fig. 2. By analogy

with the previous discussion regarding the suitability of

the ETIS model for the characterisation of individual

`threadsa it may be deduced that the no dispersion

through `knotsa assumption holds within experimental

accuracy when n

2

'15 and Pe'28.97 in the more plug

#ow `threada. Quantitative assessment of the breakdown

of the no dispersion through the `knotsa assumption is

not reported here but might be approached via consid-

eration of the Kurtosis of the RTDs.

Ordering. Using the simple conservative `dyea -tracing

methods reported here it is not possible to order the

`threadsa in a reactor network without additional struc-

tural information. To make progress with respect to

ordering of model elements in the absence of structural

information it is essential to employ a non-conservative

`dyea -tracer method with a second-order decay process.

The application of such techniques will not be discussed

here.

8. Conclusions

The ETIS model in conjunction with the reactor net-

work structure has been shown to be a versatile method

of describing the characteristics of a small but diverse

group of reactors. The ETIS model has been compared

with the conventional tanks in series approach and has

been found to be superior due to the elimination of the

quantisation which is inherent in the latter approach.

The ETIS model has also been compared with the

Thomas and McKee `closeda solution to the dispersion

model. The `closeda dispersion model has been shown to

di!er signi"cantly from the ETIS model in the range

0(Pe(28.97 and 1(n

2

(15. The `closeda disper-

sion model is also found to have the advantage of

rigorously de"ned inlet and exit boundary conditions.

Combination of the ETIS model with the reactor net-

work structure permits a considerable increase in the

versatility of networks with out the concomitant increase

in numerical intensity which characterises networks of

CSTRs.

Notation

C dimensionless concentration Dimensionless

D eddy di!usion coe$cient L` t¹

E(0) exit age distribution function Dimensionless

e base of natural logarithms

(2.718...)

Dimensionless

f #ow fraction Dimensionless

I `mixinga index Dimensionless

¸ characteristic length L

N

"

dispersion number Dimensionless

n

2

number of tanks in series Dimensionless

p precision Dimensionless

Pe peclet number Dimensionless

Q liquid feed rate L` t¹

S a term in the series solution

of the closed dispersion

model

Dimensionless

¹ mean residence time t

T Hydraulic mean residence

time

t

t elapsed time t

tM mean of the residence time

distribution

t

u velocity L t¹

< volume L`

v volume fraction Dimensionless

z axial displacement L

Greek letters

I gamma function

p E$ciency

3.14159

2

G strand dimensionless

residence time

dimensionless time Dimensionless

0M mean of the dimensionless

RTD

Dimensionless

o` variance of the dimensionless

RTD

Dimensionless

Subscripts

10 pertaining to the recovery of

10% of the injected `dyea

5916 A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917

90 pertaining to the recovery of

90% of the injected `dyea

c `closeda dispersion model

e experimental

H hydraulic

i inlet

M merril

m modal

o `opena dispersion model

R whole reactor

s thread index

sc short circuiting

¹ pertaining to the TIS and ETIS

models

Acknowledgements

The author would like to acknowledge the assistance

of the following colleagues who contributed their experi-

mental data for the case studies. Ms. Laura Burrows,

Experimental data from the internally recirculating

CSTR. Mrs. Barbara Gray, Experimental data from the

packed bed reactor. Mr. Tony Robinson, Calculation of

the simulated RTD for the Large CSTR.

References

Battaglia, A., Fox, P., & Pohland, F. G. (1993). Calculation of residence

time distribution from tracer recycle experiments. Water Research,

27(2), 337}341.

Elgeti, K. (1996). A new equation for correlating a pipe #ow reactor

with a cascade of mixed reactors. Chemical Engineering Science,

51(23), 5077}5080.

Kramers, H., & Alberda, G. (1953). Frequency response analysis of

continuous #ow systems. Chemical Engineering Science, 2, 173}181.

Levenspeil O. (1972). Chemical reaction engineering, (2nd ed), ISBN

0-471-5306-6 New York: Wiley.

Levenspeil, O., & Smith, W. K. (1957). Notes on the di!usion-type

model for the longitudinal mixing of #uids in #ow. Chemical Engin-

eering Science, 6, 227}233.

Monteith H. D., & Stephenson J. P. (1981). Mixing e$ciencies in

full-scale anaerobic digesters by tracer methods. Journal WPCF

53(1).

Smith, L. C., Elliot, D. J., & James, A. (1993). Characterisation of mixing

patterns in an anaerobic digester by means of tracer curve analysis.

Eccological Modelling, 69, 267}285.

Teefy S. (1996). Tracer studies in water treatment facilities: A protocol and

case studies. ISBN 0-89867-857-9. AWWA Research Foundation

and American Water Works Association.

Thomas, H. A., & McKee, J. E. (1944). Longitudinal mixing in aeration

tanks. Sewage Works Journal, 16(1), 42}55.

Tomlinson E. J., & Chambers B. (1979). The e!ect of longitudinal

mixing on the settleability of activated sludge. TR122 WRc July

1979.

Yagi, S., & Miyauchi, T. (1953). On the residence time curves of the

continuous reactors. Chemical Engineering (Tokyo), 17(10), 382}386.

A. D. Martin / Chemical Engineering Science 55 (2000) 5907}5917 5917

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