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Powder Technology 124 (2002) 112 – 118

www.elsevier.com/locate/powtec

The equivalence between different residence time distribution models


in ball milling
Heechan Cho a, Leonard G. Austin b,*
a
School of Civil, Urban and Geosystem Engineering, Seoul National University, Seoul 151-742, South Korea
b
College of Earth and Mineral Sciences, The Pennsylvania State University, University Park, PA 16802, USA
Received 17 September 2000; received in revised form 30 August 2001; accepted 16 October 2001

Abstract

A number of different models have been used to describe the residence time distributions (RTDs) measured for dry and wet ball milling by
various investigators in various countries. It is useful to be able to compare the results between different workers and this requires a
knowledge of the equivalence of the models. A method is presented here that permits this comparison for the usual two parameter residence
time distribution models, where one parameter is the mean residence time and the other is a characteristic parameter that defines the shape of
the residence time distribution. The method defines the best correlation as that which produces the closest agreement of the predicted mill
product size distributions over a wide range of values of mean residence time. The correlations are given in graphical form and in equation
form. In some circumstances simulation results are not sensitive to the RTD model chosen, provided that the correct match of characteristic
parameters is used. D 2002 Elsevier Science B.V. All rights reserved.

Keywords: Ball milling; Residence time distribution models

1. Introduction pared by their effect on mill product size distribution not by


the shape of the RTDs, since it is the equivalent grinding
Austin et al. [1] have reviewed the experimental results behavior that is of interest.
of measurements of residence time distributions (RTDs) in
ball mills. Such results are often given as the characteristic
parameters of a model fitted to the data, treating the data as 2. Theory
equivalent to that expected from a plug flow section
followed by a fully mixed section, or m equal fully mixed First, it must be understood that the two residence time
sections in series, or the axial mixing factor in the Mori et al. distributions that have only s as the determinant (that is, the
[2] model, etc. These models are two-parameter models, plug flow case and the fully mixed case) cannot be used to
where the mean residence time s is one parameter and the describe accurately the results actually found with tumbling
other characteristic parameter can be the number of sections, media mills. On the other hand, it is usually found that two-
the relative size of sections, the dimensionless mixing parameter models are sufficient, bearing in mind the inher-
factor, etc. The results can be compared only by establishing ent variability involved in mill tests, therefore the use of
the relations between these characteristic parameters. three- or four-parameter models is not justified. Second, the
Austin et al. [1] compared the RTD models by showing data of Concha and Pearcy [3] quoted by Austin and Concha
the plots of variance of the distributions (in dimensionless [4] showed excellent fits of the Mori et al. model [2] to
form) versus the characteristic parameters. However, there is residence time distribution data from a 3.5  4.88 m (diam-
no proof that two residence time distribution models with eter by length) industrial ball mill and a good fit to that from
the same s and variance will produce the same degree of a 3  4.25 m industrial rod mill, so it is assumed here that
grinding. In the method given here, the models are com- this semi-theoretical model can be used as the basis for
comparison.
*
Corresponding author. Tel.: +1-814-863-0749; fax: +1-814-865-3248. It is also assumed that the kinetics of breakage model
E-mail address: lxa4@psu.edu (L.G. Austin). used in a mill simulator is strictly first-order, since it is

0032-5910/02/$ - see front matter D 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 0 3 2 - 5 9 1 0 ( 0 1 ) 0 0 4 8 0 - 6
H. Cho, L.G. Austin / Powder Technology 124 (2002) 112–118 113

where p1(s) is the fraction of the mill product that is in the


top size interval. Substituting for w1(t) and /(t)

Z " !#
l
1 ð1  t*Þ2
p1 ðsÞ ¼ pffiffiffiffiffiffiffiffiffiffiffiffi exp  S1 st* þ dt*
0 2 pDt *3 4Dt*
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi

1 þ 4DS1 s  1
¼ exp  ð4Þ
2D

where S1 can be taken as 1 (time  1). For the RTD resulting


from m equal fully mixed sections in series (where m is the
characteristic RTD parameter in this case), the same proce-
dure gives

1
p1 ðsÞ ¼
m ð5Þ
S1 s

m

Fig. 1. Comparison of the disappearance of the material from the top size
It can be noted that although this equation is developed
for the Mori et al. RTD model (D = 0.15) and the m equal fully mixed
sections in series RTD model (m = 4.08). for m equal sections in series, it will compute for m not an
integer. The correspondence between D and m is that which
implicit in the use of the residence time distribution concept gives the best fit of p1(s) from Eq. (4) with that from Eq. (5).
to solve the grinding equations without integrating along the Fig. 1 shows the best fit (absolute least squares) for a
mill axis [5,6]. Of course, in comparing the equivalence of range of S1s values that takes p1(s) from 1 to about 0.01 for
one residence time distribution to another the comparison is D = 0.15, that is, 99% of size 1 is broken. The maximum
made with all other parameters (such as the specific rates of error in using m = 4.10 as equivalent to D = 0.15 is 0.005,
breakage and primary breakage distribution functions) the that is, 0.5%. However, this increases to 1.2% for D = 0.30.
same. With these assumptions, the structure of the grinding This is to be expected because the Mori et al. RTD cannot be
equations is such that if two different RTDs can be found used to approach a single fully mixed section, since it is
that give a close agreement between the rates of breakage of based on a solution of the one dimensional axial diffusion
any one size over the complete range from little breakage to equation [1] that uses a boundary condition at the mill exit
almost complete breakage, then all the rest of the simula- that cannot reduce to a fully mixed mill even as D becomes
tions will also be in close agreement (see Appendix). large. The values of D reported by Austin and Concha [4]
This means that the comparison can be made by finding
the pair of characteristic RTD parameters that give the best
match between the two RTDs in the simulation of the
disappearance of the top feed size, for any arbitrarily chosen
specific rate of breakage of this size.
For example, the Mori et al. differential RTD is [1,2]

1  
/ðtÞ ¼ pffiffiffiffiffiffiffiffiffiffiffiffi exp  ð1  t*Þ2 =4Dt* ð1Þ
2s pDt *3

where t* = t/s. In this equation, the characteristic parameter


is D (the dimensionless axial mixing factor or diffusion
coefficient), t is time in the mill and s is the mean residence
time. Let the fraction of feed of size 1 left after grinding for
time t in the mill be w1(t), where

w1 ðtÞ ¼ exp½S1 st* ð2Þ

Integrating over all possible times in the mill


Z l
p1 ðsÞ ¼ w1 /ðtÞdt ð3Þ
0 Fig. 2. Correlation between D and m.
114 H. Cho, L.G. Austin / Powder Technology 124 (2002) 112–118

for a typical ball mill and a typical rod mill were 0.18 and
0.16, respectively. Fig. 2 shows the correlation between D
and m over the range D = 0.05 to 0.50. The correlation
equation is

m ¼ 0:8632D0:8304 ð6Þ

D ¼ 0:8376m1:2042

and the maximum fractional error is

e ¼ 1:7  103 þ 0:0446D

3. Correlations

Equivalent equations to Eqs. (4) and (5) for a model


consisting of a plug flow section of relative length h and a Fig. 3. Graphical correlations between the four RTD models.
fully mixed section of length 1  h in series, and a model
consisting of a large fully mixed section of relative length /
in series with two smaller each of length (1  /)/2 are Although the Mori et al. RTD is usually appropriate for
readily derived [1]. Table 1 gives the matching results for normal ball mills, and it would be good for a system tending
the following residence time distribution cases: to plug flow, it is not expected to be useful for systems
approaching fully mixed, such as the pancake type of semi-
1. Mori et al. versus m equal fully mixed autogenous grinding (SAG) mill. The one large–two small
2. Mori et al. versus plug flow + fully mixed model may be good for normal ball mills and SAG mills,
3. Mori et al. versus one large– two small but cannot approach plug flow systems.
4. m equal fully mixed versus plug flow + fully mixed. The m equal fully mixed series is limited in scope if m is
taken as integer, but if m is allowed to be noninteger then it
The correlations are shown graphically in Fig. 3, and the is not possible to do a mass balance on a fractional section
corresponding maximum errors in Fig. 4. which has no physical reality. This means that the computa-

Table 1
Correlation equations (h = relative length plug-flow section, / = relative length large section)
Case Correlation equation Maximum error
 0.83
Mori /m equal m = 0.86D  0.002 + 0.045D
m equal / Mori D = 0.84m  1.20  0.002 + 0.037m  1.204
Mori /plug + f.m. h = 0.76exp[  3.89D]  0.002  0.031D + 0.108 D 2
plug + f.m./ Mori D =  0.26lnh  0.07 0.001 + 0.009lnh + 0.007(lnh)2
0:86
Mori /1L + 2S /¼ 0.0142  0.0545D + 0.1004D 2
1 þ expð14:13D þ 3:07Þ
2
0:86  / 0:86  /
1L + 2S/Mori D ¼ 0:07 ln 0:0005 ln þ 0:38 þ0:007
21:50/ 21:50/

m equal / plug + f.m. h = 0.76exp[  3.24m  1.20] 0.031[1  exp(  0.538m)]  0.034
8 0 " #0:83 19
< lnh0:26 =
plug + f.m. /m equal m = 0.86[  0.26lnh  0.07]  0.83 @
0:031 1  exp 0:464 A  0:034
: 0:93 ;

0:86  / 0:83
1L + 2S /m equal m ¼ 0:86 0:07 ln 4.31  27.15/ + 63.50/2  65.23/3 + 24.84/4
21:50/
0:86 1:058
m equal /1L + 2S /¼ þ ðm  1:035Þ0:958
1 þ expð11:84 m1:20 þ 3:07Þ m  0:985

0:86  / 0:27 6
1L + 2S /plug + f.m. h ¼ 0:76  1.23  10  4(/1.65  10  exp/72.70)
21:50/
0:86
plug + f.m./1L + 2S /¼ 0.086  1.177h + 5.831h2  8.733h 3
1 þ expð3:65lnh þ 4:11Þ
H. Cho, L.G. Austin / Powder Technology 124 (2002) 112–118 115

with equal partial sections, as can be seen by comparing the


two:

1 1

p

, f p 1,0 ð7Þ
S1 s m S1 s n S1 sf
1þ 1þ 1þ
m m m

where f = m  n, 0 < f < 1.0, and m, n are integers. The


correspondence between the two then depends on m and f,
not just on m, as seen in Table 2. The bi-variant correlation
equation is

2
x1:3335
6 ð115:7  114:7xÞ0:1954 , 1:0Vmð¼ 1 þ xÞV2:0
6
6 x
6 , 2:0Vmð¼ 2 þ xÞV3:0
6 ð42:5  41:5xÞ0:2659
6
f ¼6 ð8Þ
6 x
6 ð43:23  42:23xÞ0:2336 , 3:0Vmð¼ 3 þ xÞV4:0
6
4 x
, 4:0Vmð¼ 4 þ xÞV5:0
ð43:89  42:28xÞ0:2203
Fig. 4. The maximum differences in the cumulative product size distribu-
tions produced by replacing the Mori et al. axial mixing model with the
other RTD models, using the parameter correlation equations.
4. Test case

In order to confirm the agreement between the different


tional method proposed by Austin and Cho [7] that elimi- two-parameter models, an open circuit mill simulation was
nates the use of the Reid Solution [5] cannot be applied to performed to compare the results using the Mori et al. RTD
this case. The case of n equal sections plus 1 small section to those using the m equal and the plug + f.m. RTD. The
can be treated by this method, but does not give an identity parameters chosen for the specific rates of breakage Si and
the primary breakage distribution Bi, j were

2
a
Table 2 xi 1
Correlations of m equal (partial) sections (Eq. (5)) with n equal sections 6A x , n > iz 1
plus 1 smaller (see Eq. (8))
Si ¼ 4 o 1 þ ðx=lÞK ð9Þ
m x n f Maximum error 0 , i¼n
(fraction)
1.0 0 1 0 0 2

1.2 0.2 1 0.0548 0.006


xi c xi b
6 U þð1  UÞ , nz i > j
1.4 0.4 1 0.1293 0.006 Bi; j ¼4 xjþ1 xjþ1 ð10Þ
1.6 0.6 1 0.2334 0.004
1.8 0.8 1 0.3964 0.002 1 , iV j
2.0 1.0 1 1.0000 0
2.0 0 2 0.0000 0
where A = 1.36 min  1, a = 0.8, l = 4.0 mm, K = 2.22,
2.2 0.2 2 0.0711 0.001
2.4 0.4 2 0.1609 0.001 U = 0.65, c = 1.1, b = 5.8, xi is the upper sieve size of
2.6 0.6 2 0.2787 0.002 the M2 sieve interval indexed by i, and xo is a standard
2.8 0.8 2 0.4516 0.001 size (1 mm). The milling conditions are given in Table 3,
3.0 1.0 2 1.0000 0 and the simulations were run to give a coarse product
3.0 0 3 0 0
3.2 0.2 3 0.0800 0.0005
3.4 0.4 3 0.1774 0.0006
3.6 0.6 3 0.3014 0.0006 Table 3
3.8 0.8 3 0.4778 0.0004 Mill chosen for simulations
4.0 1.0 3 1.0000 0 Mill diameter, m 3.5
4.0 0.0 4 0.0000 0 Mill length, m 4.88
4.2 0.2 4 0.0855 0.0002 Ball diameter, mm 12.5 – 50
4.4 0.4 4 0.1874 0.0003 Volume fraction of balls, J 0.4
4.6 0.6 4 0.3151 0.0003 Ball density, tons/m3 7.9
4.8 0.8 4 0.4934 0.0002 Interstitial filling of balls, U 1.0
5.0 1.0 4 1.0000 0 Fraction of critical speed 0.75
116
Table 4
Typical open circuit simulation results using the Mori RTD (D = 0.15), the m equal RTD (m = 4.08) and the Plug + f.m. RTD (h = 0.408)
Interval Size, Am S value, min  1 Feed, % < size Product size distribution, % < size
Coarse Medium Fine
Mori m equal Plug + f.m. Mori m equal Plug + f.m. Mori m equal Plug + f.m.

H. Cho, L.G. Austin / Powder Technology 124 (2002) 112–118


1 8000 1.18 100.0 100.0 100.0 100.0 100.0 100.0 100.0 100.0 100.0 100.0
2 5657 1.81 95.0 99.9 99.9 99.9 100.0 100.0 100.0 100.0 100.0 100.0
3 4000 2.12 87.0 99.8 99.7 99.8 100.0 100.0 100.0 100.0 100.0 100.0
4 2828 2.08 75.0 99.6 99.5 99.7 100.0 100.0 100.0 100.0 100.0 100.0
5 2000 1.88 60.0 99.3 99.2 99.5 100.0 99.9 100.0 100.0 100.0 100.0
6 1414 1.62 46.0 98.8 98.6 99.1 100.0 99.9 100.0 100.0 100.0 100.0
7 1000 1.34 34.0 97.8 97.5 98.2 99.9 99.8 100.0 100.0 100.0 100.0
8 707 1.05 24.0 96.0 95.6 96.4 99.8 99.5 99.9 100.0 100.0 100.0
9 500 0.81 17.0 92.7 92.4 93.1 99.4 99.1 99.7 100.0 99.9 100.0
10 354 0.61 12.0 87.5 87.4 87.7 98.6 98.1 99.0 100.0 99.9 100.0
11 250 0.47 8.0 80.0 80.0 80.0 96.7 96.2 97.3 99.9 99.7 100.0
12 177 0.35 5.5 70.5 70.6 70.4 93.3 92.9 93.8 99.6 99.2 99.8
13 125 0.27 3.8 59.7 59.8 59.6 87.8 87.6 88.1 98.7 98.2 99.2
14 88 0.20 2.5 48.7 48.7 48.7 80.0 80.0 80.0 96.9 96.3 97.5
15 62 0.15 1.6 38.3 38.2 38.4 70.3 70.4 70.1 93.4 92.9 93.9
16 44 0.12 1.1 29.3 29.0 29.5 59.4 59.5 59.2 87.8 87.6 88.1
17 31 0.09 0.7 21.8 21.5 22.0 48.4 48.4 48.3 80.0 80.0 80.0
18 22 0.07 0.5 15.9 15.6 16.1 38.1 37.9 38.1 70.2 70.4 70.1
19 16 0.05 0.3 11.4 11.2 11.6 29.1 28.9 29.2 59.4 59.6 59.2
20 11 0.04 0.2 8.1 7.9 8.2 21.6 21.4 21.8 48.4 48.5 48.3
21 8 0.00 0.0 5.6 5.4 5.7 15.7 15.5 15.9 38.0 38.0 38.1

Mean residence time, min 5.2 5.1 5.3 12.2 12.0 12.3 28.3 27.9 28.7
Mill capacity, tph 137.5 139.7 135.4 58.8 59.8 58.0 25.4 25.7 25.0
Percent difference in capacity 0 1.7  1.5 0 1.6  1.3 0 1.4  1.4
H. Cho, L.G. Austin / Powder Technology 124 (2002) 112–118 117

(80% < 177 Am ), a medium product (80% < 88 Am) and a Appendix A. Proof of equivalence matching
fine product (80% < 31 Am).
Table 4 gives the results. Since the RTD forms are not The treatments given by Gardner and Sukarijnajtee [9]
mathematical identities, the product size distributions are and Gardner and Verghese [10] can be joined with the
not exactly the same nor are the mean residence times transfer function model given by Luckie and Austin [11]
required to meet the product specifications. In producing to give the following simulation equation [12]
the correlations given above (see Correlations), by absolute X i

least squares fits, the differences (referred to as ‘‘errors’’) are pi ¼ di j f j , n z i z j z1 ðA1Þ


j¼1
not randomly distributed as would be the case with exper-
imental errors. Therefore, there will be consistent differ- where
8
ences between the simulated product size distributions, as > ej , i¼j
>
<
can be seen. However, in a real mill simulation there are
dij ¼ X
i1 ðA2Þ
always experimental and model errors, and the characteristic >
> cik cjk ðek  ei Þ, i>j
:
breakage parameters (A, a, l, K, U, c, b ) are never known k¼j
with accuracy, so the match between the results from the with
different forms of RTD can be considered satisfactory if the Z l
differences are of the same order of magnitude as the ej ¼ eSj t /ðtÞdt ðA3Þ
experimental reproducibility of actual test results. 0
and
8
>
> X
j1
5. Conclusions >
>  cik cjk , i<j
>
>
>
>
>
<
k¼i
The correlations between the different characteristic 1, i¼j
cij ¼ ðA4Þ
parameters of two-parameter residence time distribution >
>
>
>
> 1 X
models that give virtually the same simulations of product j1
>
>
size distributions and mill capacities are given both graphi- >
> Sk bik ckj , i<j
: Si  Sj
cally and in equation form. These are based not on the k¼j

comparison of the shapes of the residence time distributions In these equations pi is the mill product particle size
but on the comparison of their effect on the results of mill vector, fi is the mill feed and dij is the transfer matrix (the
simulation result over a wide range of mean residence times. weight fraction of mill feed size j that arrives in mill product
The Mori et al. residence time distribution is appropriate size i). The differential residence time distribution occurs
for normal ball mills but is not valid for mills where the only in the calculation of the vector ej, Eq. (A3).
RTD approaches that of a fully mixed system. In addition, Eq. (A3) can be put in dimensionless form as
allowance for different mean velocities of flow of different Z l
particle sizes cannot be used with this RTD model. For that
ej ¼ expðsj *t*Þ/*ðt*Þdt* ðA5Þ
case, m equal sections in series, plug flow plus fully mixed, t *¼0
or the one large– two small model are more appropriate.
However, the m equal sections in series where m is not where si* = Sjs, t* = t/s, and /*(t*) is the dimensionless
integer can only be directly employed with a program that residence time distribution for reduced time t/s, s being the
uses the Reid solution in the simulation algorithms, and mean residence time. In comparing the product size distri-
again this prevents the application of the Austin technique butions (produced from a given feed size distribution at a
[8] that allows for different mean velocities as a function of given s value in a given mill) for two different assumed
particle size. This case (m not an integer) can be converted residence time distributions, the best fit occurs when the two
to one of the sections in series models and the Austin ej vectors agree most closely, as all other factors (Si, bij, etc.)
technique is then applicable. The one large – two small are the same. However, the best agreement over all relevant
model is particularly convenient for this case. values of s is when all ej values over the range s* = 0 to l
Although three parameter models obviously enable a agree closely between the two compared RTDs. The ej
better fit between model predictions and an experimentally values are no longer dependent on j and Sj but only on
determined RTD, experience shows that the use of three- s*, where the match is required over the same range of s*,
parameter models is not generally justified by a worthwhile that is
Z l
improvement in the accuracy of mill simulations over a ej ¼ eðs*Þ ¼ expðs*t*Þ/*ðt*Þdt*,
range of operating conditions. The method given here could t *¼0
in principle be applied to the correlation of the two adjust- 0Vs*Vl ðA6Þ
able parameters of a three-parameter RTD model with the
two of another but the correlations would be complex since There is only one curve of e(s*) versus s* for a chosen
four variables are involved. (dimensionless) RTD model, and two different RTD models
118 H. Cho, L.G. Austin / Powder Technology 124 (2002) 112–118

are best matched over all times when the two curves of Eq. [2] Y. Mori, G. Jimbo, M. Yamazaki, Kagaku Kogaku 28 (1964) 204 –
213.
(A6) agree most closely.
[3] F. Concha, F. Pearcy, Fundamentos Dinamicos de la Mineralurgia,
Since this match is independent of the particle size and S Curso Panamericano de Metalurgia Extractiva, Universidad de Con-
values considered, it is convenient to choose size 1, set cepcion, Concepcion, Chile, 1985 (see Ref. [4]).
S1 = 1, which makes s* = s, and use least squares minimi- [4] L.G. Austin, F. Concha, Diseno y Simulacion de Circuitos de Molien-
zation of the differences between the two sets of p1(s) values da y Clasificacion, Lamas Cia, Concepcion, Chile, 1994, p. 171.
to get the best characteristic model parameter for the second [5] K.J. Reid, Chemical Engineering Science 20 (1965) 953 – 963.
[6] L.G. Austin, R.R. Klimpel, P.T. Luckie, Process Engineering of Size
model corresponding to the chosen values of the character- Reduction, SME-AIME, New York, NY, 1984, pp. 435 – 451.
istic parameter of the first model. [7] L.G. Austin, H. Cho, An alternative method for programming mill
This treatment also shows that deducing the correlation models, to appear in Powder Technology (2001).
(between the characteristic parameters of two different RTD [8] L.G. Austin, Minerals and Metallurgical Processing 16 (1999) 29 –
models) by equating the variances of the two RTDs [13] is 36.
[9] R.P. Gardner, K. Sukarijnajtee, Powder Technology 7 (1973) 169 –
not valid. 179.
[10] R.P. Gardner, K. Verghese, Powder Technonolgy 11 (1975) 87 – 88.
[11] P.T. Luckie, L.G. Austin, Minerals Science and Engineering 4 (1972)
24 – 51.
References [12] L.G. Austin, R.R. Klimpel, P.T. Luckie, Process Engineering of Size
Reduction, SME-AIME, New York, NY, 1984, p. 441.
[1] L.G. Austin, R.R. Klimpel, P.T. Luckie, Process Engineering of Size [13] L.G. Austin, R.R. Klimpel, P.T. Luckie, Process Engineering of Size
Reduction, SME-AIME, New York, NY, 1984, pp. 343 – 371. Reduction, SME-AIME, New York, NY, 1984, p. 370.

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