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ONIT
OPERATIONS
HANDBOOK
Volume 1
UNIT
OPERATIONS
HANDBOOK
Volu111e 1
Mass Transfer
edited by
John J. McKetta
The University of Texas at Austin
Austin, Texas
library of Congress Cataloging-in-Publication Data
Unit operations handbook I edited by John J. McKetta.

p. em.
Includes bibliographical references and indexes.
Contents: v. l. Mass transfer-- v. 2. Mechanical separations and
materials handling.
ISBN 0-8247-8669-6 (v. 1 : acid-free). -ISBN 0-8247-8670-X (v. 2:
acid-free)
1. Chemical processes--Handbooks, manuals, etc. I. McKetta, John
J.
TP155.7.U53 1993
660'. 284--dc20 92-25561:.
CIP
The contents of this volume were originally published in Encyclopedia of Chemical

Processing and Design, edited by J . J . McKeua and W . A . Cunningham. © 1976,
1977, 1981, 1982, 1983, 1985, 1986, 1988, 1989, 1990 by Marcel Dekker, Inc.
Neither this book nor any part may be reproduced or transmitted in any form
or by any means, electronic or mechanical, including photocopying, micro-
filming, and recording, or by any information storage and retrieval system ,
without permission in writing from the publisher.
Preface
Here in one convenient two-volume set is the comprehensive, up-to-date in-

formation on unit operations in chemical engineering presented by world author-
ities in their specialties. In all cases emphasis is placed on the design, control,
and functioning of the various operations. Each chapter, by an expert in that
particular area, is written to be easily understood and applied . Every profes-
sional practicing engineer involved in unit operations design and calculations
should have a copy of this book on his or her working desk.
Volume 1 offers an in-depth survey of mass transfer operations including
absorption, adsorption, desorption , diffusion distillation, liquid-liquid ex-
traction, crystallization, drying, and other processes. This volume also includes
detailed information on packed towers.
Volume 2 focuses on mechanical separations and materials handling. This
volume covers in great detail particle technology, gravity sedimentation opera-
tions, flocculation, filtration, electrodialysis, electrostatic precipitation, mixing ,
blending, and conveying.
Whenever possible, shortcut methods of calculation are included along
with nomographic methods of solution. In the front of each volume are two
convenient sections: (I) conversion to and from Sl units and (2) cost indexes
that will enable the reader to quickly update all cost information. Also for
the reader's convenience, each volume is separately and extensively indexed.
As Editor, I am grateful for all the help I have received from the great
number of authors who have contributed to these volumes, and the huge num-
ber of readers who have suggested topics to be included .
JOHN J. McKETTA
iii
Contents
Preface iii
Contributors ix
Conversion to Sl Units xiii
Bringing Costs up to Date XV
1 Molecular Diffusion
Molecular Diffusion 2
P. M. Sigmund and Hing Y. La
2 Absorption
Absorption 32
R.N. Maddox and J. H. Erbar
Absorption, Falling Film 101
Gianfranco Guerreri
Gas Absorbers, Cost 127
William M. Vatavuk and Robert B. Neveril
3 Adsorption
Adsorption, Design 133
T. Vermeulen
Adsorption, General :1 44
R. A. Anderson
Adsorption, Cost 184
William M. Vatavuk and Robert B. Neveril
4 Desorption
Desorption 190
C. J. Liddle and G. M . Hampson
5 Packed Towers
Packed Towers, Design 210
Timothy L. Holmes and Gilbert K. Chen
Packed Towers, Internals 229
Gilbert K. Chen
Packed Towers Shortcuts, Computer Calculation 258
Tom C. Tsai
Packed T owers Shortcuts, Diameter, Optimum 268
Adam Zanker
Packed Towers Shortcuts, Efficiency 271
Adam Zanker
v
vi Contents
Packed Towers Shortcuts, Liquid Holdup and Pressure Drop 273

Adam Zanker
Packed Towers Shortcuts, Linear Liquid Velocity 278
Adam Zanker
Mist Removal Equipment, Design and Selection 279
Timothy L. Holmes and Gilbert K. Chen
6 Distillation
Distillation 298
W. L. Bolles and James R. Fair
Distillation, Azeotropic and Extractive 352
C. D. Holland, S. E. Gallun, and M. J . Lockett
Distillation, Batch 390
G. A. R. Trollope
Distillation Control 397
F. G. Shinskey
Distillation, Estimates for Naphtha Cuts 430
D. B. Broughton and K. D. Vitti
Distillation, Flash 442
C. J. Liddle
Distillation, Optimization 468
W. T. Mitchell
Distillation Simulation 477
A. Chou, B. L. Bauman, and A.M. Fayon
DistiUation, Steam 502
R. W. Ellerbe
Foam Fractionation 523
Robert Lemlich
7 Entrainment Separation
Entrainment Separation 542
Otto H. York
8 Liquid-Liquid Extraction
Extraction, Liquid-Liquid 582
P. J. Bailes, C. Hanson, M.A. Hughes,
and M. W. T. Pratt
Extraction, Liquid- Liquid, Equipment Choice 687
K. -H. Reissinger and Jiirgen Schroeter
Extraction, Liquid-Liquid, Packed Tower Design 711
John S. Eckert
9 Crystallization Basics
Crystallization, Concepts 73 1
Ken Toy okura
Crystallization, Nucleation Systems 745
Maurice A. Larson and John Garside
Crystallization, Design 777
R. C. Bennet/
Crystallization, Extractive and Adductive 812
Glenn H. Dale
Contents vii
10 Drying Solids
Drying, Solids 865
Ralph E. Peck
Drying of Fluids with Adsorbents 894
G. E. Hales
Freeze Drying 920
C. Judson King
11 Membrane Processing
Membranes and Membrane Processes 939
William Karas
Membranes, Technology and Application 989
J . D. Adhia
Index 1005
Contributors
J. D. Adhia, Ph.D. Senior Expert, Chemical Industry, United Nations In-

dustrial Development Organization, Vienna, Austria
R. A. Anderson Manager, Adsorption Technology and Technical Service,
Molecular Sieve Department, Linde Division, Union Carbide Corpora-
tion , Tarrytown, New York
P. J. Bailes, Ph.D. Director of Undergraduate Studies in Chemical Engin-
eering, Department of Chemical Engineering, University of Bradford,
Bradford, United Kingdom
B. L. Bauman, Sc.D Advanced Engineering Consultant, Mobil Research
and Development Corporation, Princeton, New Jersey
R. C. Bennett Division Manager, Swenson, Division of Whiting Corp.,
Harvey, IUinois
W. L. Bolles Senior Engineering Fellow, Monsanto Company, St. Louis,
Missouri
D. B. Broughton UOP Process Division, Des Plaines, IIJinois
Gilbert K. Chen, Ph.D. President, Pacific/ Asia Division, Glitsch, Inc.,
Dallas, Texas
A. Chou, Ph.D. Advanced Engineering Associate, Mobil Research and
Development Corporation, Princeton, New Jersey
Glenn H. Dale Staff Engineer, Research and Development Department ,
Phillips Petroleum Company, Bartlesville, Oklahoma
John S. Eckert Director of Engineering (Retired), U.S. Stoneware Com-
pany
R. W. Ellerbe Project Manager, Rust International Corporation, Birming-
ham, Alabama
J. H. Erbar (deceased) Professor, School of Chemical Engineering, Okla-
homa State University, Stillwater, Oklahoma
James R. Fair, Ph.D. The McKelta Centennial Energy Chair and Head,
Separations Research Program, Department of Chemical Engineering,
The University of Texas at Austin, Austin, Texas
A. M. Fayon Mobil Chemical Company, Houston, Texas
S. E. Gallun, Ph.D. Engineering Associate, Basic Chemicals Technology,
Exxon Chemical Company, Baytown, Texas
ix
X Contributors
John Garside Professor, Department of Chemical Engineering, University

of Manchester Institute of Science and Technology (UMIST), Manchester,
United Kjngdom
Gianfranco Guerreri, Ph.D. Professor of Cherrucal Engineering, Politecruco
di Milano, Milan, Italy
G. E. Hales Region Manager, LINDE Molecular Sieves Department, Union
Carbide Corporation, Houston , Texas
G. M. Hampson Chemical Engineering Division, Teesside Polytechnic,
Middlesbrough, United Kingdom
C. Hanson (deceased) Department of Chemical Engineering, University of
Bradford, Bradford, United Kingdom
C. D. Holland President, Texas Institute for Advancement of Chemical
Technology, and Professor Emeritus, Department of Chemical Engineer-
ing, Texas A & M University, College Station, Texas
Timothy L. Holmes, Ph.D. Director, Research & Development, Otto H.
York Company, Inc., Fairfield, New Jersey
M. A. Hughes Department of Chemical Engineering, University of Brad-
ford, Bradford , United Kingdom
C. Judson King, Sc.D. Provost , Professional Schools and Colleges, Uni-
versity of California, Berkeley, California
William Koros, Ph.D. B. F. Goodrich Professor in Materials Engineer-
ing, Department of Chemical Engineering, The University of Texas at
Austin, Austin, Texas
Maurice A. Larson Professor, Department of Chemical Engineering, Iowa
State University, Ames, Iowa
Robert Lemlich, Ph.D., P.E. Professor Emeritus of Chemical Engineer-
ing, Univer sity of Cincinnati, Cincinnati, Ohio
C. J. Liddle, Ph.D. Principal, CIJA Systems, Wittlesford, Cambridge,
United Kingdom
Hing Y. Lo Esso Resources Canada Ltd., Calgary, Alberta, Canada
M. J. Lockett, Ph.D. Corporate Fellow, Union Carbide Industrial Gases,
Inc., Tonawanda, New York
R. N. Maddox, Ph.D., Sc.D. Leonard F. Sheerar Professor (Emeritus) ,
School of Chemical Engineering, Oklahoma State Un iversity, Stillwater,
Oklahoma
W. T. Mitchell Celanese Chemical Company, Corpus Christi, Texas
Robert B. Neveril Gard, Inc., Niles, Illinois
Ralph E. Peck (deceased) Professor Emeritus, Department of Chemical
Engineering, Illinois Institute of Technology, Chicago, Illinois
Contributors xi
M. W. T. Pratt (deceased) Department of Chemical Engineering, University

of Bradford, Bradford, United Kingdom
K.-H. Reissinger Department of Research and Development, Bayer AG,
Leverkusen, Germany
JOrgen Schroeter Department of Research and Development, Bayer AG,
Leverkusen, Germany
F. G. Shinskey Systems Division, The Foxboro Company, Foxboro, Mass-
achusetts
P.M. Sigmund R. M. Hardy & Associates, Ltd., Calgary, Alberta, Canada
Ken Toyokura, Ph.D. Department of Applied Chemistry, Waseda Uni-
versity, Tokyo, Japan
G. A. R. Trollope Manager, Process Engineering, Allied Chemical, Marcus
Hook, Pennsylvania
Tom C. Tsai, Ph.D., P.E. Formerly Consulting Engineer, TDS Associates,
Houston, Texas; currently Process Engineering Associate, Dow Chemical
U.S.A., Freeport, Texas
K. D. Uitti UOP Process Division, Des Plaines, Illinois
William M. Vatavuk, P.E. Senior Chemical Engjneer, Office of Air Quality
Planning and Standards, U.S. Environmental Protection Agency, Re-
search Triangle Park, North Carolina
T. Vermeulen (deceased) Professor of Chemical Engineering, University
of California, Berkeley, California
Otto H. York, Ph.D. President, Otto H. York Company, Inc., Fairfield,
New Jersey
Adam Zanker, Ch.E., M.Sc. Senior Research Engineer, Haifa Oil Refin-
eries, Ltd., Haifa, Israel
Conversion to Sl Units
To convert from To Multiply by
acre square meter (m') 4.046 X 10 3

angstrom meter (m) 1.0 X 10-1 0
are square meter (m') 1.0 X 10'
atmosphere newton/ square meter (N/ m') 1.013 X 10'
bar newton/ square meter (N/ m') 1.0 X 10'
barrel (42 gallon) cubic meter (m 3 ) 0.159
Btu (International Steam Table) joule (J) 1.055 X 10 3
Btu (mean) joule (J) 1.056 X 10 3
Btu (thermochemical) joule (J) 1.054 X 10 3
bushel cubic meter (m') 3.52 X w-'
calorie (International Steam Table) joule (J) 4.187
calorie (mean) joule (J) 4.190
calorie (thermochemical) joule (J) 4.184
centimeter or mercury newton/ square meter (N j m 1 ) 1.333 X 10'
centimeter or water newton/ square meter (Nj m 2 ) 98 .06
cubit meter (m) 0.457
degree (angle) radian (rad) 1.745 X 10 - '
denier (international) kilogram/meter (kg/m) 1.0 X 10 - '
dram (avoirdupois) kilogram (kg) 1.772 X w-'
dram (troy) kilogram (kg) 3.888 X 10- J
dram (U.S. fluid) cubic meter (m') 3.697 X 10-0
dyne newton (N) 1.0 X w-s
electron volt JOUle (J) 1.60 X 10- 19
erg joule (J) 1.0 X 10- '
fluid ounce (U.S.) cubic meter (m 3 ) 2.96 X 10 - '
root meter (m) 0305
rurlong meter (m) 2.01 X 10'
gallon (U.S. dry) cubic meter (m 3 ) 4.404 X 10 - '
gallon (U.S. liquid) cubic meter (m') 3. 785 X 10 - -'
gill (U.S.) cubic meter (m') I 183 X 10 - ·
grain kilogram (kg) 6.48 X w-'
gram kilogram (kg) 1.0 X 10- J
horsepower watt (W) 7.457 X 10 2
horsepower (boiler) watt (W) 9.8 1 X 10 3
horsepower (electric) watt (W) 7.46 X 10'
hundred weight (long) kilogram (kg) 50.80
hundred weight (short) kilogram (kg) 45 .36
inch meter (m\ 2 .54 X 10-2
inch mercury newton1'quare meter (N,m') 3.386 X 10'
inch water newton; >quare meter (N / m') 2.49 X 10 2
kilogram rorce newton (N) 9.806
xiii
xiv Conversion to Sl Units
To convert from To Multiply by
kip newton (N) 4.45 X 10 3

knot (international) meter/second (m/s) 0.5144
league (British nautical) meter (m) 5.559 X 10 3
league (statute) meter (m) 4.83 X IQ 3
light year meter (m) 9.46 X 10 1 '
liter cubic meter (m 3 ) 0.001
micron meter (m) I .Q X 10 -o
mil meter (m) 2.54 X 10 - O
mile (U.S. na utical) meter (m) I .852 X 10 3
mile (U .S. statute) meter (m) 1.609 X J0 3
millibar newton/square meter (N/ m') 100.0
millimeter mercury newton/ square meter (N/ m 2 ) 1.333 X I0'
oersted amperejmeter (A/ m) 79.58
ounce force (avoirdupois) newton (N) 0.278
ounce mass (avoirdupois) kilogram (kg) 2.835 X 10 - 1
ounce mass (troy) kilogram (kg) 3.JI X 10 - 2
ounce (U .S. fluid) cubic meter (m 3 ) 2.96 X 10 - '
pascal newton/square meter (N/ m 2 ) 1.0
peck (U.S.) cubic meter (m') 8.8 1 X t0- 3
pennyweight kilogram (kg) 1.555 X 10 -'
pint (U .S. dry) c ubic meter (m-') 5.506 X 10 - .
pint (U.S. liquid) cubic meter (m-') 4.73 2 X 10 -·
poise newton second/square meter (N sj m ') O.tO
pound force (avoirdupois) newton (N) 4 .448
pound mass (avoirdupois) kilogram (kg) 0.4536
pound mass (troy) kilogram (kg) 0.373
poundal newton (N) O.t38
quart (U.S. dry) cubic meter (m') I . IQ X 10 - 3
quart (U .S. liquid) cubic meter (m') 9.46 X 10 - .
rod meter (m) 5.03
roentgen coulomb/ kilogram (c/kg) 2.579 X 10- 4
second (a ngle) radian (rad) 4.85 X 10 - o
section square meter (m 2 ) 2.59 x to•
slug kilogram (kg) t4.59
span meter (m) 0.229
stoke square meter/second (m 2 /s) 1.0 x to -•
ton (long) kilogram (kg) J. Qt6 X JQ 3
ton (metric) kilogram (kg) J.Q X t0 3
ton (short, 2000 pounds) kilogram (kg) 9.072 X t0 2
torr newton/square meter (N/ m' ) 1.333 X ]Ql
yard meter (m) 0 .9t4
Bringing Costs up to Date
Cost escalation via inflation bears critically on estimates of plant costs.

Historical costs of process plants are updated by means of an escalation
factor. Several published cost indexes are widely used in the chemical process
industries :
Nelson-Farrar Cost Indexes (Oil and Gas 1.) , quarterly

Marshall and Swift (M&S) Equipment Cost Index. updated monthly
CE Pl a nt Cost Index (Chemical Engineering). updated monthly
ENR Construction Cost Index (Engineerin!!, News-Record), updated weekly
All these indexes were developed with various elements, such as material
availability and labor productivity, taken into account. However. the pro-
portion a llotted to each element differs with each index. The differences in
overall results of each index are due to uneven price changes for each
element. In other words , the total escalation derived by each index will vary
because different bases a re used . The engineer should become familiar with
each index and its limitations before using it.
Table 1 compares the CE Plant Index with the M&S Equipment Cost
TABLE 1 Chemical Engin eering and Marshall and Swift Plant and Equipment Cost
Indexes since 1950
Year CE Index M&S Index Year CE Index M&S Index
1950 73.9 167 .9 1971 132.3 321.3
1951 80.4 180.3 1972 137 .2 332.0
1952 81.3 180.5 1973 144 . 1 344.1
1953 84.7 IS2.5 1974 165.4 398.4
1954 86.1 184.6 1975 182 .4 444.3
1955 88.3 190. 6 1976 192.1 472.1
1956 93.9 208.8 1977 204.1 505.4
1957 98.5 225.1 1978 218.8 545.3
1958 99.7 229.2 1979 238.7 599.4
1959 101.8 234 .5 1980 26 1.2 659.6
1960 102.0 237.7 1981 297.0 721.3
1961 101.5 237.2 1982 3 14.0 745.6
1962 102.0 238.5 1983 316.9 760.8
1963 102.4 239.2 1984 322.7 780.4
1964 103.3 241.8 198:1 325.3 71<0.6
1965 104.2 244.9 1986 31S.4 7lJ7.6
1966 107.2 252.5 1987 323 .8 813.6
1967 109 .7 262.9 198ti 342 .5 852.0
1968 113 .6 273.1 1989 355.4 895.1
1969 119.0 285.0 1990 357.6 915.1
1970 125.7 303.3 1991 361.3 930.6
XV
xvi Bringing Costs up to Date
TABLE 2 Nelson-Farrar Inflation Refinery Construction Indexes since 1946

(1946 = lOO}
Nelson-Farrar
Materials Labor Miscellaneous Inflation
Date Com~onent Com~onent Egui~ment Index
1946 100.0 100.0 100.0 100.0
1947 122.4 113 .5 11 4 .2 117.0
1948 139.5 128.0 122 . 1 132.5
1949 143.6 137.1 121.6 139.7
1950 149.5 144.0 126.2 146.2
1951 164.0 152.5 145.0 157.2
1952 164 .3 163.1 153.1 163.6
1953 172.4 174.2 158.8 173.5
1954 174.6 183 .3 160. 7 179.8
1955 176.1 189.6 161.5 184 .2
1956 190.4 198.2 180.5 195 .3
1957 201.9 208.6 192.1 205 .9
1958 204.1 220 .4 192.4 213 .9
1959 207.8 231.6 196.1 222.1
1960 207.6 241.9 200.0 228 .1
1961 207. 7 249.4 199.5 232.7
1962 205 .9 258 .8 198.8 237 .6
1963 206.3 268 .4 20 1.4 243.6
1964 209 .6 280.5 206 .8 252 .1
1965 212 .0 294 .4 211.6 261.4
1966 216.2 310.9 220.9 273.0
1967 219.7 33!.3 226.1 286.7
1968 224.1 357.4 228 .8 304 . 1
1969 234.9 391.8 239 .3 329 .0
1970 250.5 441.1 254 .3 364.9
1971 265 .2 499 .9 268 .7 406 .0
1972 277.8 545 .6 278 .0 438.5
1973 292.3 585 .2 29 1.4 468 .0
1974 373 .3 623.6 361.8 522. 7
1975 421 .0 678 .5 415.9 575 .5
1976 445 .2 729.4 423.8 615 .7
1977 471.3 774.1 438 .2 653.0
1978 516.7 824 . 1 474.1 701.1
1979 573. 1 879.0 515 .4 756.6
1980 629.2 95 1.9 578. 1 822.8
198 1 693.2 1044 .2 647.9 903.8
1982 707 .6 1154 .2 622 .8 976.9
1983 712.4 1234 .8 656 .8 1025 .8
1984 735.3 1278 .1 665 .6 1061 .0
1985 739.6 1297 .6 673 .4 1074 .4
1986 730.0 1330.0 684.4 1089.9
1987 748 .9 1370.0 703.1 1121.5
1988 802.8 1405 .6 732.5 11 64 .5
1989 829 .2 1440.4 769. 9 1195 .9
1990 832 .8 1487.7 797.5 1225.7
1991 832.3 1533.3 827.5 1252 .9
Bringing Costs up to Date xvii
Index. Table 2 shows the Nelson-Farrar Inflation Petroleum Refinery Con-

struction Indexes since 1946. It is recommended that the CE Index be used
for updating total plant costs and the M&S Index or Nelson-Farrar Index
for updating equipment costs. The Nelson-Farrar Indexes are better suited
for petroleum refinery materials, labor, equipment, and general refinery
inflation.
Since
(1)
Here , A = the size of units for which the cost is known , expressed in terms
of capacity , throughput , or volume; B = the size of unit for which a cost
is required, expressed in the units of A ; n = 0.6 (i .e ., the six-tenths ex-
ponent) ; CA = actual cost of unit A; and C 8 = the cost of B being sought
for the same time period as cost CA-
To approximate a current cost , multiply the old cost by the ratio of the
current index value to the index at the date of the old cost:
(2)
Here, CA = old cost; / 8 = current index value ; and / A index value at

the date of old cost.
Combining Eqs. (1) and (2),
(3)
For example, if the total investment cost of plant A was $25,000,000 for
200-million-lb/yr capacity in 1974, find the cost of plant Bat a throughput
of 300 million lb / yr on the same basis for 1986. Let the sizing exponent , n,
be equal to 0.6.
From Table 1, the CE Index for 1986 was 318.4 , and for 1974 it was
165.4. Via Eq . (3) ,
CB = C(B IA}"(IBI/A)
25 .0(300/ 200) 0 6 (318.4 / 165 .4)
$61,200 ,000
JOHN J McKETIA
UNIT
OPERATIONS
HANDBOOK
Volume 1
1
Molecular Diffusion
2 Diffusion, Molecular
Diffusion, Molecular
At constant temperature and pressure, several definitions of diffusion

coefficients are available . The choice depends largely on the units of flux and
driving force gradients being considered and on the frame of reference with
respect to which matter transports.
In binary systems composed of substances i and j, one commonly used
diffusion coefficient is defined by Fick's first law [63]:
( l)
Here 1'!' is the mol ar flux of substance i and VC; is the driving force gradient in
terms of concentration of substance i, and the reference frame is the bulk molar
average velocity , u.
Another binary diffusion coefficient D ;1 has been defined by Bird in terms of
the relationship [56]
(2)
or
Jt = - pD ip.;Vy; (3)
in which p is the molar density of the mixture , J'; is the molar fraction of
substance i, r:t.; is the thermodynamic correction factor which is given by
a In G;
r:t.·= - - (4)
1 o ln X;
and a; is the acti vity of substance i.

Still another binary diffusion coefficient has been defined by Cha pman and
Cowling [9] by the equation
J'!' = -pD ij'V y; (5)
For the ideal mixture. 2 = I.
(6)
The Chapma n- Cowling difrusi on coe ffi cient is related to the Fick type
diffusion coeffi cient by
Diffusion, Molecular 3
(7)
where Vis the molar volume and VJ is the partial molar volume of component}.
For a binary system in which the volume changes of mixing are negligible,
a;:::::: I
(8)
and the various diffusion coefficients D;; are equal. In general. all oft hese binary
diffusion coefficients are referred to as the "mutual diffusion" coefficients . For
th e s pecial case of diffusion in a uniform homogeneous Auid , the term "self-
diffusion" is used. The diffusion of a molecule of i through a medium of
identical molecules of i is termed pure component self-diffusion and is given the
symbol D,,. The diffusion of a molecule of i through a homogeneous mixture of
molecules of i andj is called mixture self-diffusion or tracer diffusion . and is
designated by the symbol D; or Dt,
In an n + I component mixture the equation used to express the com-
position change of each component with respect to time and space is the
continuity equation which may be written for each of the independent
components as [7 . 57, 61]
- V · [ C,u + 1( J• i = I. II (9)
At constant temperature a nd press ure . in a system in which all components

have a constant partial molar volume , the Aux equations which express
diffusion rates with respect to a coordinate moving at the molar average
reference velocity u may be written as [4. 14]
J,* = - L
k= i
D;/1 V'Ck ( 10)
For an 17 + I component system. Eq. (2) defines an 17 x 11 ma trix of diffusion

coefficients (D) oft he type developed by Onsager [43. 61 ). The 11 2 elements D;/1
of the matrix (D) are termed the multicomponent diffusion coefficients.
The off diagonal diffusion coefficients D;/1 (i =I= k) have bee n termed the
"c ross diffusion coefficients" and the diagonal values ( D;/1 ) the "main
diffusion coefficients " [61) . The magnitudes of the cross coefficients, D;k .w , are a
measure of the coupling or interaction that takes place between the n + I
diffusing species. It has been suggested [7. 31] that the efrects of coupling can be
conveniently taken into account for some calculations by defining an effective
diffusivity D;m for each component such that
Jj = - D;,/ilC; ( I I)
Methods of estimating the binary diffusion coefficients Du. the multicom-

ponent diffusion coefficients D,k M, or the effective diffusion coefficients D,'" in
either gases or liquids are considered in the next several sections.
Diffusion in Gases
Diffusion in Gases at Low Pressures
If a gas is modeled in simple terms , it is possible to use the kinetic theory of gases
to show the relationship of diffusivity to temperature, pressure, and in-
termolecular forces [9, 29]. Chapman and Enskog have done this to develop
theoretical equations for diffusion coefficients in gases at low pressure by
assuming:
I. Spherical symmetry of the molecules

2. Only binary collisions between molecules are significant
3. Quantum effects are absent
In general, these assumptions are valid for nonpolar gases other than
hydrogen and helium at low temperatures . A convenient form of their result fo r
the density diffusivity product at zero pressure is
( 12)
Assuming that the Leonard-Jones 6-12 potential function may be used to

describe the molecular interactions between pairs of molecules, values of the
collision integral i1 12 may be estimated from published tables or from the
following approximation [36] :
(13)
The following combining rules may be used to obtain the binary Leonard-Jo nes
[68] parameters:
(14)
Diffusion. Molecular 5
f.2)l
I
~=(
k
~X
k k
( 15)
The Stiel-Thodos [58] three parameter corresponding states correlation based

on viscosity data may be used to obtain the estimates of the molecular
parameters from pure component critical data as follows:
I
3
a; = 0.1866 Vc, Zc, - uo (l6)
k - 65 ' 3 T Ci Z Ci ·
3 60
t:; - ( 17)
In these equations the units of p"'D 0 , T, and Vare g-molfcm · s, "K, and cm 3 jg-
mol, respectively . Here R = 82.057 cm 3 atmjg-mol ·'K.
Gotoh [23] has tested a similar set of equations using 340diffusivity data for
152 systems and found that they were capable of predicting the experimental
data with an average absolute error of 6 . 50.·~ . Furthermore, Gotoh suggests that
because some of the data used in the test had considerable experimental error,
the method would likely yield better results if tested with more accurate data. A
discussion of various techniques for estimating the molecular parameters a and
c:, the validity of the combining rules, and the use of Eq. ( 12) has also been
carried out by Gotoh [23].
Diffusion in Dense Gases
For nonpolar gases, the product of p'' Df 2 is essentially constant up to values of

density one-half the critical. At higher gas densities. however, significant
departures from the Chapman-Enskog theory occur. Most theories for
predicting dense gas diffusion coefficients result from Enskog [29], who
accounted for the departure from the dilute gas kinetic theory (because of the
effect of molecular size on collision frequency) . in terms of a factor Y which may
be defined by the relationship
( 18)
Enskog suggested that the correction factor Y for a real gas could be
obtained from P VT properties or from the equation of state for the gas by the
thermodynamic relationship
V(RV( ia3 TP) jJ- I )

y = bo (19)
Here , b0 is obtained from the real gas second virial coefficient as
(20)
Enskog Hard Sphere Formula
For a single component gas whose molecules were assumed to be ha rd spheres,

Enskog derived the relationship [29]
(21 )
where b 0 = 21J rr.N(J 3 (rigid sphere second virial coefficient) (cm 3 /g-mol
p = density of fluid (g-mol /cm 3 )
p Do = the dilute gas density-diifusivity product (g- mo ljcm · s)
0
Thorne-Enskog Mixed Hard Sphere Formula (Thorne-Enskog [59])
Thorne [59] genera lized the Enskog theory for a binary mixture of ha rd spheres .
His formul a, referred to as the T ho rne-Enskog theory, may be expressed as
pD
~ =
[ 1 + -bot Y tP ( 8- -3(Jt) + -b0 2Y2P ( 8 - -3(J 2) · · ·J - t (22)
p D 8 (Jt2 8 (Jtz
where (J; = molecular diameter of component i (A)
bot= l.2615(Jt 3 (cm 3 /g-mol)

boz = l.2615(J 2 3 (cm 3 jg- mol)
(Jtz=
(J ' + (Jz (A)
2
Yt = mole fraction of component
Y2 = mole fraction of component 2

p = density of fluid mixture (g-mol jcm 3 )
For .h =I , Eq. (4) reduces to
pD [ 5 J-t (23)
poDo = 1 + 8botP
which is equivalent to Eq . (2 1) truncated after the second te rm .

Both Eq s. (22) and (23) have been fo und to give reasona ble agree ment with
experiment a t conditions where attracti ve forces between molecules are not
importa nt , as a t high reduced temperatures. At other conditio ns, however, the
results predicted from either of these theories is less satisfactory.
Approximale Dense Gas Molecular Theory (ADGMT)
Woessner et al. [68] developed an approximate dense gas molecular theo ry

( ADG MT) by calculating the Enskog correction factor from the Redlich-
Kwong equation of state . The expressions for the Enskog factor and the
pressure according to the equation of state may be written as
aM
pD I + 2b .11 RT3t z
(24)
p'' D '
I ( I ) ( aM )
1 - b*p + I + b*p 2bM RT 311
p = RTp (a tm) (25 )

I - bMp ( I + bMp)T' I1
where p = density of the fluid
aM = y, 2 a1, + 2yi.I' 2 a 12 + y/a 22 (cm 6 · atm · K 2

Ji2 jg-mol ) (26)
bM = y, 2 b,, + 2y,yzhiz + y/bll (cm 3 /g-mol) (27)

b* =y,b( + y 1 b! (cm 3
/g-mol) (28)
aii = 3. L922(a;J)3 R( £~) 312

(cm 6 · a tm · (29 )
a ; + aj A
O';j =- -
2- ( ) (30)
R = 82.057 (cm 3 · atmjg-mol ··K) (3 1)
£~ = ( ~; x £~jy (·K) (32)
b;J = 04373a/ (cm 3 /g-mol) (33 )

(a, + 4az)
bf = 0.087335a 1 3 (cm 3 jg- mol ) (34)
0'1 2
(a , + 4al)
b! = 0.087335a 2 3 - (cm 3 jg-mol) (35)
0' I 2 I I
1 2 1
p''' Do = O.OOL8583(- '- ) T +--
M1 M,
------,:'--_ _ _- =--- (g-mol jcm · s) (36)
a 2 1 20.1 zR
I
a; = 0 .1866 Vc . Tz c-, uo (A) (37 )
k = 65.3 Tc, Z c, · ( K)
~ 3 60
(38)
Three independent . intensive properties of a gas mixture are required to

calculate diffusivities for binary systems from Eq . (24) . They are temperature,
composition , and density or pressure. If press ure is used as one of these, then
8 Diffusion. Molecular
densities may be calculated from solution of Eq. (25) as suggested by Woessner

et al. [68]. The molecular constants a and e used by those authors were obtained
from previously published [21] values derived from measured dilute gas
transport properties. A further adjustment was made by them for the heavy
component well depth parameter, ez, to satisfy the relationship e 1 /ez = Tc,/Tc2 •
Generalized Reduced Density Correlation [52]
The similar share of pD/ p 0 Do vs p, curves for different systems indicates that a
single "universal'' curve might be used to give reasonable estimates of dense gas
diffusion coefficil nts. To obtain such a "universal" curve, a large body of
available self- and mutual diffusion data for a variety of systems was gathered
[52], and a genera l least-squares fit of Eq . (39) to these data was made.
pD 2 J
PoDo =a+ bp, + cp, + dp, (39)
While mutual and self-diffusion data for dense fluids composed of

hydrocarbons, N 2 , C0 2 . and the stable gases CF 4 and SF, comprised most of
n.~cbta, a limited number of data for gas-liquid and liquid-liquid systems at
relatively low reduced temperatures were used to improve the predictive
capabilities of the correlettions in the region between the dense fluid and the
normal liquid state. Data available for very light gases such as hydrogen or
helium were not used because of probable quantum effects, and data available
for alcohols were not used because of probable polar effects.
A summary of the data used is shown in Table I. In the first three columns of
the table are shown the system, the number of data used, and the source of the
data . A total of 396 data points were used in the correlation for the various
systems shown in this table.
Shown in Fig. I is a plot of the least squares values of pD jp 0 De vs p,
obtained from the general curve fit of the reduced density expansion to the data
described in Table I. The average absolute deviation of the curve fit was 14. 1%.
The correlation was found to best fit the data when the polynomial was
truncated after four terms . The four coefficients so determined are shown in
pD
- 0-0 = 0.99589 + 0.096016p, - 0.22035p, 2 + 0.032874p/ (40)
pD
Also shown in Fig. lis a portion of the experimental values of mutua! and self-
diffusion coefficients for several different systems obtained from the sources
listed in Table I. As may be seen in the figure, there is a considerable difference
between the reduced density correlation and some of the experimental values
shown. In Table I a summary is given of the average absolute percent deviations
that resulted between the experimentally observed values and the correlation
values for each of the systems used in the leas t squares fit. At present it is
difficult to determine the portion of error that is attributable to experiment
from that which is a result of inadequacies in the correlation. Nevertheless, in
TABLE 1 Description of Data Used in Obtaining Correlati ons and Comparisons oft he Predicti ve Abilities
of Various Meth ods on D ifferent Systems
Average 0
' Deviation Io.. p - o,.l, I
o •• p
0
No. of
System Data R eference Correlation ADGMT" Thorne-Enskog
Dense Gases
CH, --C H. 83 D awson. Kho ury, and
Kobayashi [ 16] 10.0 6.44 21 .3
CH,-CH, 12 Woessne r et al. [68] 1.85 4.07 19.1
CH.-Nz 26 Sigmund [52] 6 25 7.08 16.8
CH 4 - N2 6 Berry a nd Koeller [6] 4.35 4.06 9. 7
CH,-C 2H6 15 Berry a nd Koeller [6] 10.9 8.01 2 1.9
Cz H 6- N 2 6 Berry and Koeller [6] 20.1 25 0 4.7
CH ..- Ar 7 Islam a nd Stry land [32] 46 5 46.7 30 6
CH. - C., H s 57 S igm und [52] 9.05 58.2 10.8
C H, - nC, H 10 26 Sigmund [52] 11 .5 101.0 15.3
CF 4 -Cl, 54 Khoury and Kobay ashi [35] 9.4 3 25 .0 18.1
SF" SF6 29 Tison and Hunt (60] 7. 12 32.8 217
C 0 2- C02 7 Robinson a nd Stewart (48] 14.3 20.0 28 .4
C3 H s - C3 H s 8 R o binso n a nd Stewart (48] 18 9 "27.7 25.4
C3 H a- C3 D s 8 Woess ne r et al. [68] 10. 1 47 8 19 I
Average " ;, deviation for dense gases 10. 21 30. 17 18. 13
Liquids
nC 7H1 6- nC1 2H 26 13 Lo (41 ) 16.7 51 74 8 1.8
C3Hs - nC6 H, . H ayd uk et al. [27] 3.6 279 55.3
C3 H s-nC7 Ht 6 H ayduk et al. [27] 11 .2 I''> 63 .7
C3 H s- nCs H ts H ayduk et a l. [27) 15.8 172 J.n
C3 H 8 - nC 1, HJ• H ayd uk e t al. [27) 3:1 g 5082 27b.U
Cz H 6- nC6 H,. H ayduk et al. [26] 13 .9 529 81.7
C 2H 6- nC 7Hts H ayduk et al. [26] 5.5 484 86. 1
C2H6-nCsH 1s Hayduk et al. [26] 9.39 395 llX .O
C2H6 - nC1 2H 16 H ayduk et a l. (26] 27 .6 2932 "222.0
C2 H r,-nC 16H H H ayd uk et al. [26] J7 .5 4168 315.0
C H , - nC6 H 1• Hayduk et a l. (28] 26.5 654 102.0
C H 4 - nC - H 16 Hayduk et al. ["28] 28.6 751 124.0
CH. - nC" H 's Hayduk et a l. [28] 32.2 845 156.0
C H. - nCt zH z6 H ayduk et a l. [28) 60.9 3013 274.0
CH, - nCt 6HH Hayduk et al. [28] 163 4663 44 1.0
C H.-C3H s 14 Sage (24] 74.8 263 61.5
C H. - nc. HIO II Sage [24] 33.5 213.2 40.2
Average "" devia t ion for liquids 40.43 1873 .0 90 OR
Overall average"., devia ti o n 14. 1 272 27 .5
"Approximate dense gas molecular theory of Woessner e1 al. [68] .

spite of large devia tions for some of the systems listed in Table I, there is good
agreement between correlation and data for many different investigat ions.
From this and the high degree of similarity in the variations of pDjp 0 Do with p,
for the several different systems shown in Fig. I, it is evident that the correlation
represents the essential features of any general relationship that might exist.
Also shown in Table 1 are average absolute percent deviations between the
data published in the sources cited in the third column of the table and two
theoretical predictive techniques which have been described in the literature.
These two theoretical methods are the Thorne-Enskog (59] hard sphere model
and the approximate dense gas molecular theory (ADGMT) of Woessner et at.
[68]. The studies cited in the table have been divided into the categories of dense
gases and liquids. Average deviations for each predictive method are given for
these categories, and the overall average absolute percent deviat ion is given at
the end of the table. A comparison of these averages indicates that the
correlation is for the general purpose of diffusion coefficient prediction, a
significant improvement over the other methods shown, but it is not , however ,
completely satisfactory for liquids.
1 .1
0
0
'i
ij
• •
" 13
0
•
"
0 N2 - CH 4
6 CH 4 - C3 H 8
0
0 0 0 CH4 - n C4 H10
Cl. 0
Cl.
• CH4 - CH 4
., CF4 - CF4
0 .4 ... C3H8- C3H8
- Correlation
FIG. 1. Comparison of pD/p 0 D0 from correlation with data for various substances.
Diffusion in Liquids
It is best to have a predicti ve theo ry which co mbines theo retica l and empirica l
considerations to yield workable predictions alon g with fun da mental under-
standing. A theo ry for estimating liquid - liq uid diffusion coeffi cients is not
poss ible at present beca use a so und theory o f the liquid sta te is not ava ila ble.
There is still grea t uncertainty when predicting bin a ry difrusio n coefficient s at
high dilution . So me o f the work d one in this area has been rev iewed and
disc ussed by Reid and Sherwood [4 7] and Simons and P a nter [54].
Normally, the binary d iffus ion coeffi cien ts are est imated in two steps. Fi rst,
the two diffusion coefficients a t infinite dilution are calcula ted with one of t he
predictive methods. Next. the va lue o f the bin ary diffusion coeffi cient at a
desired concentration is estimated using the two limit ing di ffusion coefficient s
with one oft he proposed ex pressions for correlating the effect of concentra tion
on diffusion coefficient.
Diffusion Coe fficients at Infinite Dilution
A number o f empirica l a nd se miempirical co rrelations have been developed for

estimating diffusion coeffi cients a t infinite dilution. These eq uations and a few
o f the more recently develo ped ones are presented here.
W ilk e-Chang [67]
Wilk e and C hang proposed an empirical equati on using an associatio n

parameter (Ta ble 2) to account for the effects o f so lute and solven t :
(-+1 )
where Dt 2 . =diffusio n coefficient at infi nite dilut ion o f the diffusing species
M 2 = molecular weight of the so lvent
'72 =viscosit y o f the solvent
T = absolu te temperature
TABLE 2 Association Para meter fo r Selected Solvent at 20 C
Met hyl Ethyl

Solvent Water Alcohol Alcohol Benzene Ether Heptane
2.6 1.9
vlb =molar volume of the solute at its normal boiling point

¢ = association parameter
The authors claimed that data for iSS points among 123 different
solute-solvent systems are expressed by the correlation with an average
deviation of 12% between calculated and observed results .
Scheibel [50]
Eliminating the association parameter, Scheibel modified the Wilke-Chang

relation to give
p2 )~ T
Dl2° = 8.2 X 10- 8 ( I + 3- J ---
1 (42)
VI " -3
17 2 y lb
Othmer-Thakar [44]
Using the viscosity and heat of vaporization of water as a base, Othmer a nd

Thakar developed the following equation for estimating the diffusion
coefficient at infinite dilution
D
12
0 = 14 X 10- 5 V 0 · 6 n n l.l _!J.H_l
( lb · r2·rw !J.Hw
)-1 (43)
where !J.H 2 = latent hea t of vaporization of solvent at T

!J.H,. =latent heat of vaporization of water at T
Sitaraman-lbrahim-Kuloor [55]
Sitaraman, Ibrahim, and Kuloor, by including the latent heat of vaporization

of solute and solvent at their normal boiling points , have suggested an
expression for predicting D 11 a:
(44)
For some 76 systems, Sitaraman et a t. have found the average error between
values calculated from Eq . (44) a nd observed was a bout 13 ~ ·~ .
Reid and Sherwood [47] have tested these four correlations with experimen-
tal data and found that they yield approximately the same average percentage
error, between 2S and 28 ~1,, for a wide variety of substances.
Lusis and Ratcl!ff [42]
A correlation is presented by Lusis and Ratcliff for the mutual diffusion

coefficient in binary liquid systems at infinite dilutions:
(45)
Satisfactory results were obtained by the use of Eq . (45) for long straight
chain molecules diffusing in other class of organic solvents or other cla ss of
organic compounds in long straight chain solvents. However, large error results
from calculation with Eq . (45) when long straight chain solutes diffuse into
similar solvent. This led the authors to agree with the suggestion made by Van
Geet [64] that the mechanism of diffusion for long chain molecules is different
from that for other species, the rate-determining step being the activated
displacement of a segment of the chain rather than of the molecule as a whole.
Reddy -Dorarswamy [46]
A pair of equations were suggested by Reddy and Dorarswamy . The Wilke-

Chang correlation for predicting liquid diffusivities was modified by replacing
the association parameter by the square root of the solvent molar volume:
I
M2 2 T
DI2 o =l0xl0 -8 I I' (46)
1'/2 (JlTfJ2T
and
I
M 2TT (J ,
DI 1o= 8.5 x l0 - s I I ' if r~ > t. 5 (47)
172 C\Tfl 2 3
An average error of 13.5 ~,~ from Eq. (46) for 76 systems and of 18% from Eq .
(47) for 20 systems were found when comparing values calcu lated with the
proposed correlations with experimental data.
Akgerman
Akgerman extended the Akgerman-Gainer equation for diffusion of gas in

liquid to liquid - liquid systems by considering molecules to be spherical and
that the geometric parameter
I I I
~~ = n/arcsin [ fl 2 3 j ( V13 + V1 3 )] (48)
is in the diffusion coefficient equation
(49)
The activation energy difference is given by
£ j)l /(~,+1)]
£~2- Eo,2 = £2/ [ 1- ( E:~i (50)
where tbe jumping energy for the pure solvent, £ 2 / , or for the pure solute, £ 111,
is
T
Rio-
To
E;! = E~, - 1 I (51)
To T
where T 0 is some base temperature, taken to be 273.15 K . The Akgerman-

Gainer equation contains no adjustable parameter or empirical factors . It has
been applied to 96 different liquid systems and over 200 data points, and it gives
a root-mean-square error comparable to that of the Wilke-Chang equation.
Concentration Dependence of Liquid Diffusion Coefficients
Up to the present time, there is still no general framework available for the
quantitative explanation of the variation of the binary mutual diffusion
coefficient with composition in the liquid phase. Considerable efforts have been
expended on this problem, and several rela tions have been proposed to predict
the effect of concentration level upon diffusion coefficient in liquid - liquid
systems.
Roseveare-Powell- Eyring [49]
Roseveare, Powell, and Eyring, on a serniempirical basis, have suggested:
(52)
Rathbun-Babb [45]
Rathbun a nd Babb developed the empirical correlation
(53)
where sis an adjustable parameter. A value of0.6 was recommended for binary
systems containing an associated and a nonpolar compound .
Vignes [65]
An empirical equation was developed by Vignes for the variation of the

diffusion coefficient with composition in terms of the same thermodynamic
factor and the two diffusion coefficients at infinite dilution. Cullinan [I OJ
derived the same equation shortly thereafter by modifying the absolute rate
theory set forth by Eyring.
D 12 = (D 21 o)x'(D 12 o)x2( -
o ln
-at)
- (54)
8 ln x 1
Equation (54) has been tested by Vignes a nd shown to be satisfactory for a large
number of groups of binary systems.
Lefflen-Cul/inan [39]
Lefflen and Cullinan attempted to further improve the Vignes equation a nd

arrived at a new expression with the viscosity of the mixture included :
(55)
They claimed that comparison with data for a large number of known
systems showed that this modified version improves the overa ll predictability
except for mixtures of n-alkanes. The concept of segmental diffusio n was used
to explain the inconsistency.
Dark en [15]
D arken has shown that the tracer diffusion coefficient of a tagged molecule is
identical to the so-called intrinsic mobility of the species:
kT
D* = - (56)
, ry f, ,
Therefore, the mutual diffusion coefficient and the trace r diffusion coeffi cient in
binary solution are related by
D 1 2 -_ (xl D*2 + X2 D*1) (dln

- --a1)
dln X
(57)
1
when Eq . (56) is substituted int o

(58)
Equation (58) was derived from statistical mechanics. Equation (57) can be
used to calculate mutual diffusion coefficients if the tracer diffusion coefficient
can be measured or predicted from other sources.
Haluska-Colver [25]
Haluska and Colver derived the expression
(59)
by proposing that the friction factor ~ 12 be estimated in the following manner
(60)
for the diffusion equation derived from statistical mechanics
Dl2 -_ -
V 2-RT(dlna 1
- - - -) (61)
~12 dlnx 1
where
RTC',
~~ z''= -
D o- (62)
12
(63)
This method was tested with several binary systems (toluene-methylcyclo-

hexane, toluene - aniline, methylcyclohexane - aniline, and chloroform - carbon
tetrachloride) and was found to correlate the data successfully . The error was of
the same magnitude as that obtained by the Yignes correlation.
Gainer [19]
Predictions of the concentration dependence of the liquid diffusion coefficient

have required the use of activity data in most previous developed equations and
correlations. A method was proposed by Gainer, based on a modified absolute
rate theory approach, to estimate the variation of diffusivity with concentration
change using only the physical properties of the liquid involved, such as
viscosity and molar volume, by writing
D 12 ' = (!__!_)(!!___)~ exp ( £~, - Ev,,) (64)

~ 1t/ 2 172 RT .
£~ 2 - £ 0 12 = £~,- ( ~ 1 )
2 <; 2
X { j~(~)(~)(
'12 2
£~2-H
2
)
r 12
(65 )
(66)
(67 )
Equation (67) can be used in combination with some othe r correlations to

give new equa tio ns to predict the mutua l diffusion coefficient fr o m physical
pro pe rties o f the liquids a nd o ne limiting diffusion coefficie nt.
Whe n the Vignes equa tio n is used. the fo llowing expressio n res ulted :
o r with C ullin a n's equa tio n , it is
D 1 ,- " x 2 x ' [ ( ·12

D 1 2 = - - ry z 1'/t
"
-
)0.5(M
-
)0.25 (!l£. )0.5 Jx,( -d In-a-)
2 vap I I
(69)
rJ l]t M1 !l. E,.P 1 d ln x 1
S hieh-Lyons [5 1]
While a tte mpt ing to ra tio n a lize the tra ns po rt p rope rties o f simp le n-alk a ne
systems. Shie h and Lyo ns discove red some interesting be hav io r pa tterns. For
a ll bina ry n-a lk a ne liquid mixtures. D 1 2 /rx 1 2 was fo und to be a linea r fu nction o f
the densit y p, Fig . 2. All these lines extra po la te to zero mo bilit y a t p = 0 .84 ,
corresponding to a supe rcooled melt o f n-pa raffin o f very hig h molecu la r
weight. T he slo pe o f these lines are linea r function o f n 1n 2 where 11 1 and n 2 a re
the numbe r o f ca rb on a to ms in the two co m ponen ts . Fig. 3.
D1 z/a12 = b + kp (70)
a nd
(71)
2.8
2 .4 o • Experimental
Pred ict ed
.."'
0 2 .0
N '
E
u
1 .6
I() CB- C14
0
...-
X 1.2
....
N
tl
' N
0 .8
o""
0.4
OL-___ L_ _ _ _J __ _ _ _L __ _ ~ _ _ _ _J __ _ _ _L __ _~-----L----L---~----~
0 .64 0 .66 0 .68 0 70 0 .72 0 74 0.76 0 .7 8 0 .80 0.82 0 .84 0 .86

3
DENS IT Y gm I cm
FIG. 2. Linear relationship between 0 1 ,fa 1 2 and density in binary n-alka ne syste ms at 25T.
17 0 r---------------------------------------------------------,
15 .0
c7- c12
I c6- c16
I
13. 0
:.:: c 8 - c12o cl a - c14

I
c7 - c14
11 .0
c7-c16 c B - c16
9.0
7.0
6 .0 7 .0 8 .0 9 .0 10.0 1 1 .0 12 .0 13.0 14.0
FIG . 3 . Slo pe of D, 2 ~ nd p re lat ionshi p in bin~ry 11-alkane systems at 25 C.

where a, b =constants
k , k = proportionality constants
p = density
n 1 , n 2 = numbers of carbon atoms in the components

a 12 = nonideali ty correction factor
Equations ( 70) and ( 71) can be used to predict binary diffusion coefficients in n-
alkane systems.
Diffusion Coefficient of Gases in Liquids
As shown in Table I. studies of diffusion coefficients of hydrocarbon gases in

hydrocarbon liquids may be obtained using the empirical correlation given by
Eq. (40). For non hydrocarbon systems the empirica l correlation given by Wilke
and Chang [6 7] (Eq. 41) may be used .
A more theoretical approach has been developed by Akgerman and Gainer
[2] wh o presented an equation based on modified absolute rate theory for
predicting diffusion coefficients of gases in liquids.
(72)
(73)
where ~ ~ is a geometrical parameter describing the number of nearest neighbors

around a central molecule and can be estimated from self-diffusion data. A
value of 6 has been proposed. It was assumed that the activation energy for
viscosity is composed of two parts, the energy required to form a hole and the
energy required for a molecule to move into that hole. Similarly for diffusion.
there is an energy required to form a hole and energy required for a solute
molecule to move into the prepared hole. Hence
(7-1)
where) refers to jumping energy and
R In I]') + -R In (' -·r,)

(---=-
I]! 2 T!
( 75)
I I
(76)
a nd
£11 1 = 5875.3M 1 - o. l so (77)
Although the e mpirical Eqs. (40) and (41) are adequate for many systems,
Eq. (72) is better for the following cases: (I) systems involving a small solute gas
molecule, such as H 2 or He: (2) systems involving solvents having viscosities
greater than 3 to 5 cP: a nd (3) for comparison of relative diffusion rates.
Self-Diffusion in Liquids
In the various model approaches to the stud y of self-diffusio n , the liquid is, with
a few exceptions, either considered as a dense gas or a disordered solid. A review
of the various approaches a nd models is given by Ertl, Ghai, and Dullien [ 18,
22] . They have shown that most o f eq uatio n developed , whe n suitably
rearranged . lead to expressions which are similar or almost identical to the
Stokes-Einstein relation :
kT
D= - - (78)
61J7r:R
T he Stokes-Einstein equation has often been used to test self-diffusion d a ta

pertaining to the diffusion of spherica l molecules of eq ua l s ize. It has also been
app lied to the sel f-diffusion of extremely nonspherical mo lecules. H owever , it
has been found to give too small values.
Dullien 's equation [ 17] is
(79)
The rela tion , with V be ing the molecule volume a nd Vc the critica l volume. was
obtained by using a genera l relation between transport coefficients of pure
liquids a nd a molecular kinetic model of liquids. It fits the experiment a l data of
32 liquids with a mean deviation of 4%.
Van Geet-Adamson's equation [64] is
3 3
log D = -3.28- -10-- £(10
- - 0.82) (80)
2.3 R T
where E is activation energy . This equation was developed based on data of n-

alkanes. T his equation was found to provide self-diffusion coefficients with a n
accuracy o f abo ut 5 /~ for n-a lk a nes with the number o f carbo n in the liq uid
from 5 to 32 and for tempera tures between - 50 a nd 300oC.
The Effect of Tem perature and Pressure on Liquid Diffusion Coefficient
In most of the earlier equations and correlations, such as those of Wilke-Chang

and Scheibel, which were developed based on the hydrodynamic theory, a linear
relationship between the product of diffusion coefficient and solvent viscosity

and absolute temperature is usually indicated:
D12'1 2
- T- = constant (8 1)
This relationship has been found to be approximately correct.

The most successful feature of the absolute rate theory is its prediction of a
logarithmic relationship between the diffusion coefficient and the reciproca l of
absolute temperature. Gainer [20), modifying the absolute rate theory equa-
tion, has suggested an improved expression for the variation of diffusion
coefficient with temperature by taking into account the difference between the
activation energy due to diffusion a nd to viscosity:
D12'12
- - exp (Ev '' - E~ ) = constant
2
(82)
T RT
Equation (83) has been tested by Gainer to describe more closely the variation
of liquid difrusion coefficient with temperature than Eq . (82).
Very little has been reported on the effect of pressure on liquid diffusion
coefficient. Benedek and Purcell [5] found an approximate linear relationship
between diffusion coefficient and pressure. An increase of pressure by I atm was
shown to increase the value of the self-diffusion coefficient of water by 0.006° 0 •
The influence of pressure changes under normal conditions on liquid diffusion
coefficient can generally be neglected.
Multicomponent Diffusion
I fthe values of DikM can be estimated either by measurement or by theory. then

Eqs. (9) and (I 0) can be solved [51. 6 1]. Analytic solutions can be obtained by
ass uming concentration independence of[D). Examination of the errors which
result from not acco unting for concentration dependence have been made [3 . 7).
A thorough discussion of the linearized trea tment of Eqs. (9) a nd (I 0) to
calculate multicomponent concentration profiles appears e lsewhere [57 , 6 1) .
T he solution for a ternary system in one dimension can be written as [38, 57, 61]
L'1C(t • .:) = ! 11!1C1 + !11!1C2 (83)
L'1C2(1 , .:) = ! 21!1C1 · + f 22!1C2 (84)
D - M - D ,M[J . D - M - DM(j .
where f,tk.. = tk -
DIM - Dl M
tk j( D M)
I
tk I
+ D 2M - D I M
tk } '( D
1
-~' ) (85 )
6 ;k = I, i= k
= 0, i =I= k
and where D/1 are the eigenvalues of the matrix [D] . For the ternary case they
are given by [38, 61]
(86)
(87)
The f( Dk) are the solutions to equivalent binary problems with the same
initial and boundary condition as the multicomponent problem [37 , 61], but
with the binary diffusivity replaced with the Dk :
.1C; =initial concentration driving force of component i
= C;(O. 0+)- C;(O. 0-)

.1C; =concentration profile of component i at time 1
When the effective diffusivity approximation is used , the simple binary solution
applies to each component as follows :
(88)
Predictive Relations for M ulticomponent Diffusion Coefficients
The Stefan-Maxwell Relations [7]
Originally developed to describe diffusion in low densit y ga s mixtures , the

Stefan-Maxwell relations have been used to relate [13] the mole fraction
gradient of a component to the mutual diffusivities , D;k> compositions, and
differences in diffusion velocity, v, between that component and each of the
other species in a mixture. For example , in a mixture containing each of the
species A. B. C, and D. the relationship may be written for component A as
In general, for an + I component mixture , this equation is usually written [7]

for the ith species as
n+ I ]
-CV'Y; = I -D (J( yk- it Y;) (90)
k= I ik
where J ( = C; v;, i=l, ... ,n+l.

Diffus1on. Molecular 23
As shown by Toor e t al. [62] and Stewart et al. (5 7]. when Eq . (2) is written in
matrix notation as
(1*) = - [D] C(V Y) (91)
the elements of(D] may be determined by in verting the ma trix [P][D r 1

where
for C constant
- C(VY) = [P ]( J*) (92)
The elements of( P] are obtained fro m Eq. (90) and a re given by Too r et al. (62]
as
(93)
(94)
[D] = [Pr t (95)
Thus the ele ments of the multicompon ent diffusion matrix. D;k. may be
obtained in terms o f the available mutua l diffusivities D ;k a nd the mole fraction
)';. For purposes o f illustratio n . the elements o f the matrix [D] for a three-
component system a re
DIIM = DI3[D 23Yt + Dl l (l - Yt) ] / A (96)

1
D 11 '~ = J'1 D23(Du- D1 2)/A (97)
D 21"' = y 2 D 13 (D 23 - D 2 !)/A (98)

DdH = D 23 (D tJY2 + D 21 (1 - J'l) ] / A (99)
A = y1 D 23 =Y1 D1 3 +y3 D1 2 ( 100)
The mutua l diffus ivities D ;, = Dk ; fo r either liquids or gases may be calculated

by the procedure described prev io us ly.
Although the Stefan-Maxwell relations were o riginall y develo ped to
describe multicom po ne nt diffusion in low density gases, several investigators [8,
30, 40] have discussed the application of these rela tions to multicomponent
diffusio n in liquids. L ig htfoot e t a l. (40] ta ke into acco unt n o nidea lity o f the
liquid solution a nd ex press the Stefan-Maxwell equa tion for diffusing liq uid s as
( 101 )
Hydrodynamic Theory
The hydrodynamic theory has been used successfully to describe isotherma l

diffusion in multicomponent liquid systems [33, 34] . In this approximate theory
the chemical potential gradient or driving force for diffusion is balanced by a
"resisting" force. This force balance may be written as [33, 34]:
- V' J.l; = U;l'/l'i (102)
where a; = the hydrodynamic size-shape factor
v; =the diffusion velocity of component i
'1 = the viscosity

V' J.l, = the chemical potential gradient of component i
Equation (15) may be used to write the following expression for the diffusion
flux :
c
Jt = C;v; = - - ' V'p; (I 03)
U ;l'/
For a three-component system Kett and Anderson (34) have related Eq. (1 03) to
Eq. (2) to obtain expressions for the DiJ . For D 11 their result is
(I 04)
where V'; = partial molar volume of component i

a; = activity of component i in solution
Similar expressions were presented for D 1 2 , D 21 , and D 22 and will not be

repeated here.
The viscosity of the solution was estimated using the following mixing rule :
n+ I
In '1 = L
i= l
X; In '7; (105 )
The hydrodyna mic factor was estimated by the relationship
RT
(i =I, 2, 3) (106)
where D 1 is the self-diffusivity of component i. and D;/ is the infinite dilution

diffusivity of component i in).
Values of the thermodynamic properties (il ln a;) jilC1 were evaluated from
the van Laar equation as
( 107)
Other multicomponent theories for diffusion in liquids have been described

in the literature [II. 12]. As stated by Cullinan [ 12]. the relative merits of these
various methods depend to a large extent on the accuracy of multicomponent
solution thermodynamics.
The Wilke Eflective DiffusiviiJ' Equation
Wilke [66] used the Stefan-Maxwell equations to derive the following

expression for the effect1ve binary diffusion coefficient of a single gas diffusing
into a stagnant multicomponent mixture or n + I components:
1- YA
DAm = "- +.,..-1: - - - ( 108)
L _li_
i= t D .4i
i ;t: A
Where A refers to the diffusing gas. m to the mixture , n + I is the number of

components, and DAi is one of the mutual diffusion coefficient pairs of the 11,
A - i pa irs.
Even though Eq ( 108) is strictly valid only at conditions where species A is
present in trace amounts . or where species B. C. and D have similar velocities , it
is sometimes used to define effective diffusivities in a system in which all
components are diffusing. This process. in effect. defines then+ I elements ,
Dim• in a diagonal matrix. Equation {6) then gives the solutions to the 17 + I
binary problems for an 17 + I component system. The Wilke equation. used in
this way. gives values where each case may be considered as the result for the
diffusion of component i in the mixture m. As a result, then + I answers are the
sets of values Y ei and Y ""' = I - Y ei· In general. the I Y ei-=/= 1.0. and the results
should be normalized using the relationship
( 109)
Use of the normalizing procedure avoids the ambiguities noted by Toor et al.
[3] .
Symbols
a constant in Shieh-Lyons equation

G; activity of component i
ai1, aM., a* constants in Redlich-Kwong equation
A;i van Laar constant
b constant in Shieh-Lyons equation
bo hard sphere molecular volume
bij, bM, b* constants in Redlich-Kwong equation
B second varia! coefficient
B ;i van Laar constant
C; molar concentration of component i
D molecular diffusion coefficient
[D] multicomponent diffusion matrix
Dt tracer diffusion coefficient
D; self- or tracer diffusion coefficient in a mixture
D;; sel f-d iffus ion coefficient
D ii Fick-type mutual diffusion coefficient
Dii Bird-type mutual diffusion coefficient
Dij Chapman-Cowling mutual diffusion coefficient
D;m effective diffusivity for component i diffusing into mixture M
D;,M multicomponent diffusion coefficient
E energy of activation
E., activation energy due to viscosity
E •., activation energy due to diffusion
£,/l - 0 activation energy for viscosity due to dispersion
E,,l - H activation energy for viscosity due to hydrogen bonding
£;/, Ej jump energy
t:J.E,.p energy of vaporization
t:J.H2 heat of vaporization of solvent
t:J.H2b hea t of vaporization a t normal boiling point
Jt molar flux of component i relat ive to the molar average velocity of the
system
k Boltzma n 's constant
k, K proportionality constants
M; molecular weight of component i
N Avagadro's number
number of carbon atoms in component i
p pressure
r,, distance between molecules
R universal gas constant
R radius of particle
s adjusta ble para meter
T absolute temperature
ro base temperat ure
time
molar average velocity
mol ar volume
partial mol a r volume
molar volume at norma l boiling point for component i
X; mole fraction of co mponent i, liquid
mole fract ion o f co mponent i. gas

normalized m o le fracti o n of component i. gas
correct ion fact o r
rectang ul ar s pace coordinates
compressibility factor
critica l compressibility factor
Greek Letters
non idealit y co rrect1on fac tor

kronecter delta
"'· ''I
I·J·'"·J m inimum of the intermo lecula r potentia l between molecules i; i a nd j
'"=i· ':t ij fric ti on coefficients
~. pa rame ter which d escr ibes th e geomet ric configurat ion of the d iffusing
molecule a nd its neares t neigh bor
'1; viscos ity of co mponent i
-
Jlo chemical potentia l of co mpone nt i
V; velocity or component i
p density
pD densit y-diffusi vit y prod uct
molecular diame ters
collisio n in tegra l
association parameter
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ONIT

Unit operations handbook I edited by John J. McKetta.

The contents of this volume were originally published in Encyclopedia of Chemical

Here in one convenient two-volume set is the comprehensive, up-to-date in-

Packed Towers Shortcuts, Liquid Holdup and Pressure Drop 273

J. D. Adhia, Ph.D. Senior Expert, Chemical Industry, United Nations In-

John Garside Professor, Department of Chemical Engineering, University

M. W. T. Pratt (deceased) Department of Chemical Engineering, University

To convert from To Multiply by

acre square meter (m') 4.046 X 10 3

To convert from To Multiply by

kip newton (N) 4.45 X 10 3

Cost escalation via inflation bears critically on estimates of plant costs.

Nelson-Farrar Cost Indexes (Oil and Gas 1.) , quarterly

TABLE 2 Nelson-Farrar Inflation Refinery Construction Indexes since 1946

Index. Table 2 shows the Nelson-Farrar Inflation Petroleum Refinery Con-

Here, CA = old cost; / 8 = current index value ; and / A index value at

At constant temperature and pressure, several definitions of diffusion

and a; is the acti vity of substance i.

J'!' = -pD ij'V y; (5)

For the ideal mixture. 2 = I.

At constant temperature a nd press ure . in a system in which all components

For an 17 + I component system. Eq. (2) defines an 17 x 11 ma trix of diffusion

Methods of estimating the binary diffusion coefficients Du. the multicom-

Diffusion in Gases at Low Pressures

I. Spherical symmetry of the molecules

Assuming that the Leonard-Jones 6-12 potential function may be used to

The Stiel-Thodos [58] three parameter corresponding states correlation based

Diffusion in Dense Gases

For nonpolar gases, the product of p'' Df 2 is essentially constant up to values of

V(RV( ia3 TP) jJ- I )

Here , b0 is obtained from the real gas second virial coefficient as

Enskog Hard Sphere Formula

For a single component gas whose molecules were assumed to be ha rd spheres,

Thorne-Enskog Mixed Hard Sphere Formula (Thorne-Enskog [59])

where (J; = molecular diameter of component i (A)

bot= l.2615(Jt 3 (cm 3 /g-mol)

Y2 = mole fraction of component 2

For .h =I , Eq. (4) reduces to

which is equivalent to Eq . (2 1) truncated after the second te rm .

Approximale Dense Gas Molecular Theory (ADGMT)

Woessner et al. [68] developed an approximate dense gas molecular theo ry

p = RTp (a tm) (25 )

where p = density of the fluid

aM = y, 2 a1, + 2yi.I' 2 a 12 + y/a 22 (cm 6 · atm · K 2

bM = y, 2 b,, + 2y,yzhiz + y/bll (cm 3 /g-mol) (27)

aii = 3. L922(a;J)3 R( £~) 312

R = 82.057 (cm 3 · atmjg-mol ··K) (3 1)

£~ = ( ~; x £~jy (·K) (32)

b;J = 04373a/ (cm 3 /g-mol) (33 )

Three independent . intensive properties of a gas mixture are required to

densities may be calculated from solution of Eq. (25) as suggested by Woessner

Generalized Reduced Density Correlation [52]

While mutual and self-diffusion data for dense fluids composed of

"Approximate dense gas molecular theory of Woessner e1 al. [68] .

Diffusion Coe fficients at Infinite Dilution

A number o f empirica l a nd se miempirical co rrelations have been developed for

W ilk e-Chang [67]

D 1 2 -_ (xl D2 + X2 D1) (dln