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N. WAKAOand J. M. SMITH

University of California, Davis, California

(Received 10 April 1962)

Abstract-A

theory is proposed for predicting diffusion rates at constant pressure through bi-disperse

porous media. The total rate is the sum of separate contributions for diffusion through macropores,

micropores and a series path. To apply the theory requires a knowledge of the pore volume-pore

radius distribution for the porous material.

Experimental diffusion measurements are reported for five high-area alumina pellets of different

densities made from the same Boehmite powder. The results show that for the least dense pellets

macropore diffusion is dominant. In contrast the micropore contribution controls the diffusion rate

in the most dense pellet. The theory predicts rates in good agreement with the data over the pressure

range investigated, 1-12 atm. Comparison with other diffusion data is hindered by the lack of porevolume-distribution information. However, such data are available for a silver catalyst and for a lowarea alumina. For these different materials the theory also predicts reliable diffusion rates.

DIFFUSIONIN CATALYST

PELLETS

importance of pore diffusion resistance in

some gas-solid catalytic reactions (for example

cumene cracking [l] and o&o-hydrogen conversion

[2]) has resulted in several studies of pore diffusion

rates [3-71. Because of the range of pore sizes that

exist in many solid catalysts, both Knudsen and bulk

diffusion processes may be significant. The interpretation of diffusion data in terms of the appropriate diffusivities in such cases lead to some

confusion in the early work. However, correct

and equivalent interpretations have been developed recently by SCOTT and DULLIEN [8], MASON et

al. [9] and ROTHFELD and WATSON[lo].

For optimum rates of reaction the pore-size

distribution should be such that the total of

diffusion and reaction resistances are a minimum.

One can anticipate the time when catalysts can be

prepared specifically to give a pore-size and area

relationship for optimum performance.

Before

this can be done, it is necessary to develop a means

of predicting diffusion rates as a function of the

physical properties of the porous material. The

objective of the present study is to propose a method

for correlating and predicting diffusion rates in

terms of the porosity and pore size-distribution

data. The work is restricted to pelleted type

materials prepared by compressing particles of

THE

Thus the resulting pellet has two pore systems:

micropores within the powder particles and macropore space between the powder particles. To

evaluate the proposed method experimental diffusion measurements were made on high-surface

alumina pellets over a range of pressure and

macropore sizes. These data constitute the only

results that cover a broad enough range of variables

and include sufficient pore size-distribution information to evaluate the method critically. However,

partial comparisons can be made with published

data on silver [5] and low-surface alumina [IO]

catalysts.

MECHANISMOF DIFFUSION IN CATALYSTPELLETS

In a bi-disperse porous system at constant pressure

the mass transport will be a combination of diffusion

through (1) macro- and (2) micropores,

the relationship

between the two depending

upon the

bulk density (macropore volume). Fig. 1 is proposed

to represent the system as far as diffusion is concerned.

The dotted squares identify the powder

particles containing

micropores

and the spaces

between them represent the macropores.

It will

be assumed that the area void fractions are the

same as the volume void fractions.

Then the

probability

that a given location

(on a plane

825

This expression accounts for bulk diffusion according to the molecular diffusivity D,, and Knudsen

diffusion with a diffusivity D, determined by the

pore radius a

D, = 2ijAa/3

FIG. 1.

Diffusion

adding the contributions to mass transfer of A for

each of the three mechanisms. The resulting

diffusion rate per unit cross-sectional area of the

pellet is

materials.

RT- -s,zD, 2

(Mechanism 1)

(&2

Da = (1 - ay,+)/DA, + I/&,,

$I(1 - &,)2

Di = (1 -

(1 - &,)2

RT (1 - uyJIDAB + l/D,

(4)

series. The area for this contribution is 1 - E: (1 - &a)2or 2~,(1 - EJ.

The general equation for the rate of diffusion of

A in a circular capillary per unit area at constant

pressure in a binary system of gaseous A and B

[8-lo] is

NAYP

(Mechanism 2)

repeated to make up the pellet has a length Ax,

from the centre of one powder particle to that of its

neighbour (Fig. 1). The composition change across

the element is AyA. The diffusivities Da and D,

apply for the macro- and micro-regions respectively, and are given by the equations

6

Or

2

*A

- 2E(1 - s) (l/D,) + (l/Di) Ax

(Mechanism 3)

(1)

surfaces are rejoined. Then the void area per unit

total area on the rejoined plane will be the probability of two successive events, or (E)(E) = E.

The diffusion through the plane can be divided

into three additive parts (parallel mechanisms):

(1) Through the macro-pores with an area of E:

and an average pore radius Z,,.

(2) Through the particles having an area (1 - 8,)

and an average pore radius L&. The effective void

area of micropores per unit area in the particles is

2

- (1 - Q2Di 2

N AT-

be in a void space is E. If E,,,.si, and E, represent the

volume fractions of macropores, micropores and

solid,

E, + Ei + Es =

(3)

(2)

(6)

~YAYDAB

(l/h,)

component A in the macro- and micropore regions.

Since the pores cover a range of sizes, mean values

of the diffusivity based upon mean macro- and

micropore sizes should be used.

Equation (4) applies to the unit cell of Fig. 1.

If it is summed to include the whole pellet of thickness L, and if equations (5) and (6) are introduced

for D, and Di, the diffusion flux NA can be expressed

in terms of L and the end compositions yA, and

yA,.

826

1-aYA2

+(DA~/Dki)

1 -

+(DAB/%,>

aYAl

ayA

+I [tl - Ea)2/si21

+ @k,/k.)

I

2

4sLl(I - e3

+ 1 + [(i - &,)2/E;]

1 _

ayA,

1 + [(l -

Dki

: +

cc1

RTLa

_=E21n

A PDAB

1-

aYA2

+cDAdBk)

1 -

"YA,

+ (D.&k)

aYAz

1 - aYAl

@)

+ @?&/p~k.)

a(yA,

+ <&/pDk,>

4%0

+

qJ2/$J

%~)~/~iZl +

[(l

(7)

@k#k.)

qJ2jEiZ1

in a stainless steel chamber [7], were maintained by

slowly bubbling streams of each gas (helium and

nitrogen) into a surge tank [3] containing water.

The lines containing the two gases extended to

the same depth in the surge tank. The pure gases

(nitrogen 99.97 per cent pure and helium 99.99

per cent) were directed tangentially into the chamber

near the end surfaces of the pellet. The exit streams

from the chamber were analysed in calibrated,

thermal conductivity cells (Gow-Mac Co., Type

30s) immersed in a constant temperature bath

maintained at 25C. The entire flow rates of each

In most bi-disperse porous catalysts the macropore radius Za is much larger than the micropore

value, &. Then Dki/Ljko is small with respect to

(1 - &a)2/&i2. Also the ratio DAB/nki iS large enough

for the arithmetic mean to approach closely the

logarithmic mean. Hence, equation (7) is closely

represented by a simpler result:

1-

1 +

Dk,

i.e. E, = 0 or ~~ = 0, equation (7) reduces to the

simple integrated form of equation (2);

1 -

d(YA,

- 80)

YAz)

YA,)/21 + (%/p~k,)

a(YAt - J)AI)

1 + [(l - &J2/&l

(9)

.

l-a[(YA~

+ YA2)/21

1 +z$(

-a

)2]

Equation (9) predicts the effect of macro- and

microporosities and mean pore sizes (through

9, and 9, and equation 3) on the diffusion rate.

The result is based upon the model of Fig. 1 which

includes the assumption that the three contributions

are independent of each other. Of particular

significance is the simple result that in a random

distribution of pores the effect of porosity is proportional to s2.

EXPERIMENTAL

WORK AND RESULTS

Fig. 2 is similar to that used and described by

HENRY et al. [3]. It is based upon the original procedure by WICKE[ 111, for measuring counter-current

diffusion rates through porous materials under

constant pressure conditions.

Equal and constant

827

FIG. 2.

1,2

3

4

5

6

7

8

9

10

Experimental apparatus.

He, Na cylinders

Surgetank

Manometer

Pressuregauge

Porous pellet

Pellet container

He, NZ reference gases

Thermal conductivity cell

Soap-film meter.

N.

WAKAOand J. M. SMITH

the micropores were essentially the same for all the

pellets with a narrow peak at about 20 A. This result

indicates that the pelleting process did not destroy

the powder particles. The minimum in the volume

distribution vs. pore-radius curves occurred at

about 100 A, and this was taken as the boundary

between micro- and macropores for determining

void fractions. The densities of the six pellets were

meters were employed to measure the rates which

varied from O-5 to 2 cma/min (S.T.P.).

Data were obtained for the nitrogen (component

A) and helium (component B) system, at pressures

from 1 to 12 atm and at 24C.

The pellets consisted of cylindrical disks of

Al,OZ - lHzO (Boehmite) 1 in. in diameter and

about 4 in. in thickness (see Table 1). They were

Table 1.

Pellet *

A

B

C

D

E

Thickness

(mm.)

12.6

12.6

13.0

12.7

12.6

Total

pore volume

Vt (cm3/g)t

2.14

l-39

1.10

0.728

O-560

Density

Total

Wm3)

Total

void

fraction

0.488

0.679

0.800

1.041

l-206

O-80

O-72

0.67

0.57

0.51

Micropores

Macropores

Voidfraction

.%

$1

Voidfraction

ea

&

0.17

0.27

0.33

0.39

0.42

25

24

23

23

23

0.63

0.45

0.34

0.18

0.09

15,000

2300

1100

460

370

t Pore volume is per gramme of AlaOs; i.e. per gramme of pellet weighed after ignition.

Carver Model-B Press without adding lubricant or

other contaminant. The powder was contained in

a stainless steel ring, 1 in. I.D., and the ring and

powder together placed in the press to form the

pellet. The ring and pellet as a unit were then

installed in the stainless steel chamber using

flanges with O-rings to obtain a tight seal. This

arrangement allowed operation up to 15 atm

pressure without leakage. The powder used was

spray dried alumina from the American Cyanamid

Company and had an average particle size of about

90 F. Pellets (A to E) of five different densities,

and hence different macropore sizes and void

fractions, were obtained by using different masses

of alumina in the press.

The total pore-volume data and volume distribution vs. pore-radius calculations were obtained by

Mr. Marvin F. L. Johnson of the Sinclair Research

Laboratories, Harvey, Illinois, by nitrogen adsorption and mercury penetration

measurements.

Measurements were made on six pellets, each of a

different density but all made from the same

Boehmite powder.

Examples of the volume

distribution-pore-radius

curves have been pre828

in this investigation. Hence, the void volume for

samples A-D were obtained by interpolation and E

by extrapolation, The resulting physical properties

for the five samples are summarized in Table 1.

The measured diffusion rates, related data and

calculated results are given in Table 2. It has been

shown (9) that the ratio - Na/N, should be inversely

proportional to the square roots of the molecularweight ratio, regardless of type of diffusion. For

helium and nitrogen this result is -N,,/N, = 2.64.

The measured rates given in Table 2 indicate ratios

close to this value.

ANALYSIS OF DATA AND THEORY

In using equation (9) to calculate the diffusion rate

the mean micro- and macropore radii are necessary

in order to evaluate i&, and &,. This requires

data on the distribution of micro- and macropore

sizes. The distribution curves [13] for the micropores are narrow with a very sharp peak at 20 A,

so that cj will be close to this value. Since the mean

radii are used to evaluate the Knudsen diffusion

Table 2.

Diffusion rate

mole fraction of

(mol/sec)

Na in Helium Nitrogen

Run PresHe in

no. sure Na-side

He-side-SNB

S.NA

x 10-4

x 10-4

P

1 - YAI

YAz

A 1

1GO

1.92

3.25

4.81

0.353

0402

0.127

0.133

0.333

0.302

0.273

0.326

0.124

0.0915

B 1 1.26

2 5.05

3 12.0

0.358

0.391

0.372

c 1 1.92

2 4.23

3 7.80

4 12.4

RTLNA

--

(JJA, -

NB

YA#%B

RTLNA

@A,

YA,)~~B

observed

NA

Contribution of

series

macromicro-

0.125

2.66

o-209

O-228

0.226

o+MO293 0~00200

0.410

0.397

0.119

0,162

0.169

2.54

2.53

2.35

0.222

0.234

0.252

0.248

0.247

0.271

0.244

0.240

0.261

oGoO555 0.00377

O+MlO938 0.00620

oMI134

oGO9Oo

0.115

0.106

0.109

0.1264

0.1622

0.2198

0.0485

0.0655

0.0845

260

2.54

260

0.0800

0.114

0.142

OG90

0.133

0.155

0.086

0.118

0.124

o+loO929 0GO301

0.00351

0.0113

0.00754

0.0237

0.154

0.240

0.321

0.320

0*0500

0.0620

0.0931

OWI80

0.1044

0.1297

0.1258

0.1507

OWO8

0.0498

0.0484

0.0584

2-56

2.61

2.60

2.58

OGKO

0.0641

0.0740

0.0900

0.0584

0.0697

0.0862

0.101

0.0428

0.0553

0.0629

0.0663

OW132

0.00443

o+IO777

0.0115

0.00425

0.00896

0.0155

0.0228

D 1 1.05

2 2.70

3 3.28

4 5.18

5 6.58

6 11.5

0.0387

0.0560

0.147

0.180

0.202

0.197

0.0203

0.0298

0.0335

0.0483

0.0640

0.0641

0.0281

0.0473

0.0523

0.0648

0.0604

0.0872

0.0107

0.0184

0.0200

0.0249

0.0241

0.0352

2.63

2.57

2.62

260

2.51

2.48

0.00996

0.0176

0.0214

0.0282

0.0287

0.0418

0.00889

0.0182

0.0210

0.0285

0.0335

0+473

OGO571

0.0103

0.0115

0.0139

0.0154

0.0180

0+0170

OGO424

o+IO511

0.00785

0.00975

0.0159

OGO148

0.00367

oGo441

OGO671

0.00832

0.0134

E 1 1.68

2 3.56

3 6.25

4 9.30

5 10.86

0.0451

0.0582

0.140

0.0853

0.147

0.0127

0.0149

0.0890

0.0375

0.0522

0.0184

0.0321

0.0390

0.0630

0.0564

0.00714

0.0122

0.0147

0.0237

0.0233

2.58

2.63

2.65

2*66

2.42

O+IO659

0.0114

0.0166

0.0235

0.0253

003566

0.0108

0.0171

0.0233

0.0267

OGO154

0.00239

0GO303

ow343

0.00377

0.00296

OTlO605

0.0102

0.0144

0.0166

O+KU16

0.00236

oGO393

oGO553

0.00637

2

3

4

A = Nitrogen,

B = Helium,

S = Cross-sectional

for pi gives

6%

contributions in equation (9), the averaging procedure should be for this type of mass transfer.

The total rate of Knudsen diffusion through the

micropores, using equation (3) is

QA = - &

Oba(xa2)n(a)da

ai

i&

=B

---a,

RT3Ax

ab

so

na2n(a)da

s0

axa2n(a)da

(12

ali

7ca2n(a)da

s 0

between a and a + da, per unit length of pore.

Hence, equation (12) can be written in terms of the

known pore volume per gramme of alumina.

Vi

ai=vi

*kz2n(a)da

s0

P 2vA by, _

(10)

s0

with a radius between a and a + da, and a, the

upper limit of the microradius, in this case 100 A.

In terms of the mean diffusivity &, the total

diffusion rate is

QA = - ;

s0

adVi

(13)

(11)

pore-volume-pore-radius

distribution curves and

found to be 23-25 A. The integral is applied over

the microvolume region, 0 to Vi. The result

829

N. WAKAO

and J. M. SMITH

of the distribution data into separate curves for

the micro- and macroregions. Since the micropore

distribution was the same for all the pellets, this

value of pi is applicable for pellets A-E.

The diffusion data for the most dense pellets

also can be used to obtain a value of Zi. Thus as

s,, + 0, equation (9) reduces to the micropore term

only. Under these conditions,

should be equal to EF&/D~~.From Fig. 3(a) this is

EiD

2

D"

AR

can be estimated

in Table 1. The

Fig. 3(b), is (E~)_~

(15)

&, =

RTL

NA

P(YAi - YA&%S

=P{l

-a[(yA,

involving the pressure in the denominator of the

right-hand side of equation (14) becomes small with

respect to D;iB/bki.

Fig. 3(a) is a plot of

RTL

vs. E,.

NA

O+M20atm-

(YAl - YA,P&

by extrapolating the sl data given

result, illustrated by the graph in

=

O-44. Then from equation

0~0020(0~697)~(044)2

00

8

c

i

0.4

.;o

8

it

0.3

0

9

0.2

e

.o

r

0.001

0.2

0.4

0.1

0

Estimation

0.2

0.4

Macro void

FIG. 3.

(15)

= 0.0072 cm/sec

(16)

where DiB = 0.697 atm(cm)/sec is the value of

DA,obtained from the Chapman-Euskog expression

[12] for the N,-He system at 1 atm pressure and

24C. Using this result for & in equation (3)

gives Z, = 23 A assuming circular pores. The

excellent agreement between the two results is

probably due to the narrow distribution of micropore radii.

Equation (13) can also be used to evaluate Z,,

for the macropores by changing the limits of

(14)

yAz)/21) + @%/~d

of Knudsen

830

diffusion

fractlan

c-6

, r,

in micropores.

2.

oa

IO'

r

IO'

0

Total pore

FIG. 4.

volume, V,,

Mean macropore

cdh

V, - Vi. The values of (z, SO calculated for the

original six pellets are plotted vs. total pore volume

V, in Fig. 4. Values of Za for pellets A-E were

obtained by using the V, data in Table 1 and Fig. 4.

The values of (5, so evaluated are given in the last

column of Table 1. These were used to determine

the corresponding

mean Knudsen diffusivities

Dk,.

pressure,

Exp data of

Total

o

P.

atm

pellet

Comparison

Knowing i& (OGO720 cm2/sec) and &._ equation (9) can be used to predict diffusion rates through

the pellets as a function of density and gas pressure.

The porosities a. and ai are available from the porevolume measurements. The observed and predicted

total rates are compared in Fig. 5 for three of the

pellets by plotting N,R7X/(yA, - vA,)D& vs.

pressure. Experimental and calculated results for

all the pellets are given in Table 2. Also included

in Fig. 5 are curves for the separate contributions

to the total rate, corresponding to the separate terms

in equation (9). For the low-density pellets, illustrated by the results for pellet B in Fig. 5, diffusion

through the macropores is dominant. The contributions of the micro- and series mechanisms are

10 per cent or less of the total. For the most dense

pellet E, this is reversed and the contribution of the

macropore diffusion is least signitkant. The total

rate decreases sharply as the density increases.

The agreement between the predicted and experimental result lends confidence to the proposed

theory, particularly since thereare no arbitrary constants involved in equation (9).

Evaluation of equation (9) requires data (a) for

pellets of different densities to test the validity of

the porosity functions in each term, and (b) for

P,

o Pellet

FIG. 5.

atm

D

P,

o Pellet

1: Macro contribution.

2: Micro contribution.

3 : Series contribution.

831

atm

E

N. WAKAOand J. M. SMITH

different pressures to test the validity of the functions giving the relative significance of bulk and

Knudsen diffusion. Complete data of this nature

do not appear to be available except for that presented here. However, some information has been

published which permits partial evaluation of

equation (9).

3.

I.0 _

8

II

IL

n

rates through silver catalyst pellets of different

densities at 1 atm pressure. Void-fraction data

were obtained but not volume pore size-distribution

information.

Hence, the appropriate values of

D,. and Dkkiare not available. However, for lowdensity pellets under conditions where Knudsen

diffusion is negligible, such information is not

needed to apply equation (9).

The results of most prior investigators have been

reported in terms of an effective diffusivity, D,,

defined by the expression

De

dYA

FIG. 6.

simple form

D

e=E

DAB

there results

1 - aYA

= D,P In

(18)

l- MyA,

Equation (18) can be combined with Equation (9)

to give an expression for D, in terms of the properties of the porous material. Expressed as the

diffusibility, De/DAB, the result is

D

DAB

e=

dyA,

+ "

(20)

are shown in Fig. 6 plotted as D,/DAB VS. ~2.

The dotted line on the Fig. represents equation (20).

The results for the least-dense pellet (si = O-57)

agree reasonably well with Equation (20). The

data for the higher-density pellets show large

deviations for equation (20). This is expected, from

1 -RYAN

+(D~B/P&.)

- YAz)

1 - @[(YA, + YAJPI

+ (KBIP~,,)

4%(1 - %)

+ 1 + [(l - &,)/S] *

theory.

(17)

1 - ay, dx

N,RTLu

Comparison

dYA, - YAz)

1 - a[(YA, + YAz)/~~ + 1 +;$$fe

I

For low-density pellets only the macropore contribution should be signmcant (see Fig. 5). Also if

the macropores are large enough, or the pressure

high enough, the Knudsen part of the diffusion in

the macropores should be negligible. Under these

(19)

121

cl

of Knudsen diffusion in the macropores and

increasing importance of the micropore and series

contributions.

832

4.

ROTHFELD and WATSON [lo] measured diffusion

(Type Al-0104-T,

Harshaw Chemical Co.) and

presented data for the isobutane (A)-helium

(B)

system at pressures of 200 to 700 mm Hg. This

dense pellets D or E in Table 1 with respect to void

fractions. The values of E, and Ei were 0.18 and

0.34 respectively. However, the micro- and macropores were much larger and the surface area much

smaller (76 m2/g vs. 350 m2/g for pellets A-E).

The pore volume vs. pore-radius distribution data

did not show a sharp minimum between macro- and

microregions in contrast to the high-area alumina.

There was a signi6cant volume in pores of intermediate radii. Therefore, taking the minimum in

the distribution curve as the boundary between

micro- and macropores introduces errors in calculating ii and Cr,. This difficulty was circumvented by

extrapolating the micro- and macrosections to give

separate distribution curves. From these curves,

using equation (13), the mean pore radii were found

to be Zi = 84 A and & = 4800 A. Composition

information was not available so that yA1 and Ye,

were unknown. This prevents an exact comparison

of theory and experimental data. However, most

diffusion measurements of this type are made with

nearly pure gases on the opposite faces of the pellet

so that yA, = 1 and yA2 = 0, is probably a good

approximation. Using these results diffusion rates

were calculated from equation (9). The experi-

FIG.

based upon the same co-ordinates as Fig. 5. The

agreement suggests that the theory is also applicable

to this different type of porous material.

In summary a model has been proposed for

diffusion in bi-disperse porous catalysts. The

development gives a relationship between diffusion

rate, porosity and pore-size characteristics, that

agrees well with available data. To predict diffusion

rates from the equations it is necessary to know

the pore-volume-pore-radii

distribution in the

porous material.

study was sponsored by the

United States Army Research Office (Durham) through

Grani #DA-ARO(@-31-124-Gl91.

Acknowledgement-This

NOTATION

a Pore radius

li, Mean radius for diffusion in the macropores

CZb

tit

DAB

D'AB

De

DC2

cm

cm

cm

Upper limit of radius of micropores

Mean radius for diffusion in the micropores

cm

cm2/sec

Binary bulk diffusivity for system A-B

cn+/sec

DABP atm

Effective diffusivity defined by equation (17) cm2/sec

Composite diffusivity, defined by equation (5)

cm2/sec

Composite diffusivity, defined by Equation (6)

CllG/StZC

cm2/sec

defined by equation (11)

Mean Knudsen diffusivity of gas A in the macropores

cm2/sec

cm

Geometrical length of porous pellet

Molecular weight

g/g mole

Diffusion rate per unit area of gas A (nitrogen)

g mole/(cm2)sec

cm-

Number distribution of pores

atm

Total pressure

g mole/set

Diffusion rate

Gas constant

cm3(atm)/(K)g mole

cm2

Cross-sectional area of pellet

SNA = total diffusion rate through pellet

K

T Temperature

V Pore volume per g (ignited,

cm3/g

Vt = total pore volume,

Vt = micropore volume

Average molecular velocity of gas A

Cm/SeC

BA

Distance in the direction of diffusion

X

cm

Mole fraction of gas A in the system;

YA

y_Q = mole fraction nitrogen on nitrogen side of

pellet ;

yA2 = mole fraction nitrogen on helium side of

pellet

OL Ratio of diffusion rates 1 + NBINA

E

Void fraction

Subscripts

a, i Macro- and micropores, respectively

A, B Nitrogen and helium, respectively

1,2 Nitrogen and helium sides of pellet

833

N. WAKAOand J. M. Surrn

RFFERENCES

[l] PRAYERC. D. and LAGOR. M., Advances in Catalysis Vol. VIII, p. 294. Academic Press, New York 1956.

[2] WAKAON., SELWOOD

P. W. and SETH 5. M., Amer. Inst. Chem. Engrs. .I. To be published.

[3] HENRYJ. P., CHENNAKF..SAVAN

B. and SMITHJ. M., Amer. Inst. Chem. Engrs. J. 1961 7 10.

[4] HOOGSCHAGEN

J., Industr. Engng. Chem. 1955 47 906.

[5] MASAMUNE

S. and %rrrr J. M., Amer. Inst. Chem. Engrs. J. 1962 8 217.

[6] Scorr D. S. and Cox K. E., J. Chim. Phys. 1960 57 1010.

[7] WEISZ P. B.,Z. Phys. Chem. 1957 11 1.

[8] Scorr D. S. and DULLIENF. A. L., Amer. inst. Chem. Engrs. J. 1962 8 293.

[9] EVANSR. B., WATSONG. M. and MACONE. A., Gaseous Diffusion in Porous Media at Uniform Pressure, IMP-AEC-15.

Institute for Molecular Physics, University of Maryland, 1 June 1961.

[IO] ROTHFELD

L. B. and WATSONC. C., Gaseous Counter Diffusion in Catalyst Pellets. Paper presented at the 54th Ann.

Meeting Amer. Inst. Chem. Engrs., New York, 3-7 December 1961.

[ll]

WICKEE. and RALLENBACH

R., KoNoidZ. 1941 97 135.

[12] HIRXHFELDER

J. O., CURT~SSC. F. and BIRD R. B., Molecular Theory of Gases andliquids, Chap. 8. John Wiley, New

York 19.54.

[13] MISCHKER. A. and Sm

J. M., Thermal Conductivity of Alumina Catalyst Pellets. Submitted for publication to

Ind. & Eng. Chem., Fundamentals Quarterly.

R&urn&La

auteurs proposent une theorie pour ltvaluation des vitesses de diffusion a pression

constante a travers un milieu poreux ;i double dispersion.

La vitesse totale est la rtkultante des vitesses de diffusion a travers les macro et micropores et

diverses voies. Lapplication de la theorie nkcessite la connaissance de la repartition des volumes

et rayons des pores du mat&au.

Des mesures experimentales de diffusion sont effectukes pour cinq sortes de granules dalumine

a grande surface active de differentes densites, obtenues a partir de la m&me poudre de Boehmite. Les

r&hats montrent que la diffusion par les macropores est predominante pour les plus faibles densites.

Inversement, la diffusion par les micropores correspond aux plus grandes densitb.

Les vitesses

prevues theoriquement dans lintervalle 1-12 atm correspondent bien aux r&hats

experimentaux.

Le manque dinformation sur les distributions des volumes des pores concemant dautres rksultats

de diffusion empkhe toute comparaison.

Cependant ces donnks sont valables pour un catalyseur dargent et pour une alumine a faible

surface spkcifique.

La theorie donne aussi des evaluations de vitesses de diffusion correctes pour ces differents

mattriaux.

834

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