Chemical Engineering Science 58 (2003) 2433 – 2440
www.elsevier.com/locate/ces
Shorter Communication
Approximate formulas for nonlinear di$usion and adsorption of a
spherical particle
Hsiao-Kuo Hsuen∗
Department of Chemical Engineering, Yuan-Ze University, Chung-Li, Taiwan 320, Republic of China
Received 24 September 2002; received in revised form 7 January 2003; accepted 20 January 2003
1. Introduction
Modeling of /xed-bed and batch adsorption processes
involving porous adsorbent particles often requires a quanti-
tative description of intraparticle di$usion rates. In general,
the di$usion mechanism occurring within the adsorbent par-
ticles of the processes includes pore di$usion of 3uid phase
and surface di$usion of adsorbed phase in parallel. Due to
the mathematical complexities associated with the di$usion
equations for such a mechanism, simpler rate expressions
are desirable. The most widely used one is the so-called
linear driving force (LDF) approximation, which was orig-
inally developed by Glueckau$ (1955) for surface di$usion
with a constant di$usivity. As both pore and surface di$u-
sion occur in parallel, a mathematically equivalent equation
to the LDF can be obtained if the adsorption isotherm is
linear and local equilibrium between the pore 3uid phase
and the adsorbed phase is assumed. The LDF can also be
derived by assuming parabolic concentration pro/le within
the particle (Liaw, Wang, Greenkorn, & Chao, 1979).
For a nonlinear isotherm, Lai and Tan (1991) assumed
parabolic and quartic pro/les for the combined gas and
adsorbed phase concentration inside the adsorbent particle
and derived approximate formulas with parameters that de-
pend on the slope of adsorption isotherm at the external
surface of the particle. In their models, only pore di$usion
is taken into account. Starting with the concentration layer
concept, Yao and Tien (1993) developed two approxima-
tions for calculating the uptake rate of adsorbate in spherical
adsorbent, which are suitable for both linear and nonlinear
adsorption isotherms. Nevertheless, their models are appli-
cable for either pore di$usion or surface di$usion, but not
for both in parallel. Based on di$erent assumptions, Yao
and Tien (1998) further formulated four models for the
rate of adsorption in an adsorbent particle with a nonlinear
∗ Corresponding author. Tel.: +886-3-4638800 ext.569;
fax: +886-3-4559373.
E-mail address: skhsun@ce.yzu.edu.tw (H.-K. Hsuen).
0009-2509/03/$ - see front matter ? 2003 Elsevier Science Ltd. All rights reserved.
doi:10.1016/S0009-2509(03)00081-2
adsorption isotherm, which are the parabolic model, the
shell-core model, the modi/ed shell-core model and the gen-
eral driving force model. Their models are applicable for the
particles in which the intraparticle mass transfer is controlled
by pore and surface di$usion in parallel. Their results also
revealed that the general driving force model provides the
best approximation and other models only yield good results
for limited conditions. By employing the parabolic pro/le
assumption for the combined pore 3uid and adsorbed-phase
concentration, Zhang and Ritter (1997) proposed an approx-
imate model that accounts for parallel pore and surface dif-
fusion. Carta and Cincotti (1998) derived an approximate
rate law for nonlinear adsorption and di$usion in a spherical
adsorbent based on an equivalent /lm thickness of one-/fth
of particle radius. Parallel pore and surface di$usion as well
as the e$ects of variable surface di$usivity are considered
in their approximation.
Although a great reduction in computational e$orts is ob-
tainable for Zhang and Ritter’s model (1997) and Carta and
Cincotti’s (1998) formula, signi/cant errors arise as real sit-
uations become far away from the assumptions used in their
derivations. For example, as a clean adsorbent is subjected
to a step change in the surface concentration, the intraparti-
cle concentration pro/le developed at the initial stage is far
from parabolic. Certainly, the intraparticle mass transport
under such a condition cannot also be adequately described
by employing an equivalent /lm thickness of one-/fth of
particle radius since its actual value is much smaller. Yao
and Tien’s models (1998) might provide good results for
such a circumstance because the shell-core assumption they
used is close to real situation. However, no further investi-
gations with practical adsorption systems were reported in
their work. The objective of the present work is to develop
approximate formulas for calculating the uptake of a spher-
ical adsorbent with nonlinear adsorption and di$usion sub-
jected to a step change in the surface concentration. Parallel
pore and surface di$usion as well as concentration depen-
dence of surface di$usivity are considered in the intraparti-
cle mass transfer. The investigations on the accuracy of the
2434 H.-K. Hsuen / Chemical Engineering Science 58 (2003) 2433 – 2440

developed formulas will be performed using practical ad- and surface di$usion. The in3uences of these factors will be
sorption systems with quite di$erent di$usion and adsorp- discussed in the examples investigated later. By de/ning a
tion characteristics. Comparisons of the present formulas new dimensionless di$usion time, ,
˜ through
with other related ones reported in the literature will be also d ˜ 1 + (d y=dM x)
M
carried out. = ; (10)
d 1 + (d y=d
M x)
M
associated with the initial condition
2. Theory ˜ = 0 at  = 0; (11)

The adsorption model employed in the present work takes the original model equation can be converted to a linear one,
into account parallel pore and surface di$usion in a spher- which is
 
ical adsorbent particle. It is assumed that local equilibrium @z 1 @ 2 @z
between the pore 3uid phase and the adsorbed phase is =  ; (12)
@˜ 2 @ @
achieved at each point on the adsorbent surface. Both pore
and surface di$usion coeKcients are considered to be con- where
stants. With the assumptions stated above, the mass balance z = x + y: (13)
equations with their associated boundary conditions are writ-
ten as The associated initial and boundary conditions are

  @z
@c @q 1 @ 2 @c @q  = 0; = 0;  = 1;

p + p = 2 r
p Dp +  p Da ; (1) @
@t @t r @r @r @r
z =  + 1; ˜ = 0; z = 0: (14a-c)
q = Q(c); (2)
A linear formula with -dependent
˜ mass transfer parameter
@c for z(=
M xM + y)M is written as (Hsuen, 2000)
r = 0; = 0; r = R; c = cs ; t = 0; c = 0: (3a-c)  
@r d zM 3 −0:5 18 0:5
= √ ˜ + − 3 + 6:6218˜ (1 +  − z):
M
It is more convenient to rewrite the above equations in di- d ˜  
mensionless form as (15)

 
@x @y 1 @ 2 @x @y The solution of Eq. (15) can be readily obtained as
+ = 2  +  ; (4)
@ @  @ @ @

6
zM = xM + yM = (1 + ) 1 − exp − √ ˜ 0:5
y = f(x); (5) 
  
@x 18
 = 0; = 0;  = 1; x = 1;  = 0; x = 0; (6a-c) − − 3 ˜ − 4:4145˜1:5 : (16)
@ 
where One more assumption was employed to calculate individual
c q  p qs amount of xM and y,
M which is
x= ; y= ; = ;
cs qs
p cs yM = f(x):
M (17)
Da r Dp t This assumption has been employed by some previous in-
= ; = ; = : (7a-f )
Dp R R2 vestigators (Yao & Tien, 1993; Zhang & Ritter, 1997) to
develop approximate formulas for nonlinear adsorption and
The left-hand side of Eq. (4) can be rewritten as
di$usion in porous particles. Its validity is somehow simi-
  
@x @y @x @y 1 +  @y
@x
lar to Eq. (9); that is, exact relation only exists for a linear
+ = +  : (8) isotherm and some deviations may develop as relation be-
@ @ @ @ 1 +  @y @x
tween the pore 3uid phase and the adsorbed phase starts to
A critical assumption is employed for simpli/cation; that is, depart from a linear one. Substituting Eq. (17) into Eq. (10)
gives
1 +  @y
@x 1 + (d y=d
M x)M
@y
= ; (9) d ˜ 1 + f (x) M
1 +  1 + (d y=d
M x)M = : (18)
@x 
d 1 + f (x)M
where xM and yM are the average values of x and y over the ad-
If the expression of the adsorption isotherm is known, Eq.
sorbent, respectively. This assumption is exactly true for a
(18) can be solved with the employment of Eqs. (16) and
linear isotherm. For a nonlinear one, the error introduced re-
(17). The sorbate uptake of the particle, including the pore
lies on the degree of nonlinearity of the isotherm covered by
3uid and the adsorbed phase, is determined by
the intraparticle concentration pro/les, adsorption strength
of the adsorbent, and relative importance of pore di$usion xM + yM = xM + f(x):
M (19)
 H.-K. Hsuen / Chemical Engineering Science 58 (2003) 2433 – 2440 2435

As the Langmuir isotherm is applied for the description of Table 1

phase equilibrium of the pore 3uid phase and the adsorbed Physical parameters for the adsorption systems investigated
phase, the amount of the adsorbed phase can be calculated Parameter A B C
by

p 0.61 0.32 0.61
qm bc p (kg=m3 ) 850 1230 850
q= : (20) R (m) 0.001 0.003 0.0028
1 + bc
b (kg=m3 ) 148.02 6.44 0.0569
The dimensionless equation can be formulated as qm (kg=kg) 0.2208 0.0678 0.0139
Dp (m2 =s) 1:79 × 10−9 3:00 × 10−6 1:97 × 10−8
xM Da (m2 =s) 1:79 × 10−10 1:00 × 10−8 3:8 × 10−9
yM = ; (21) p qm b=
p 45541.6 1678.3 1.1
1 − (1 − x)
M
A : C6 H14 -activated carbon at 298 K (Kapoor & Yang, 1991).
where B: ethane-5A zeolite at 298 K (Nagel, Kluge, & Flock, 1987).
qs C : H2 -activated carbon at 298 K (Doong & Yang, 1986; Ritter & Yang,
= : (22) 1987).
qm
Thus, xM can be expressed as a function of zM through Eqs.
(16) and (21), which is

−( − zM + 1 − ) + ( − zM + 1 − )2 + 4(1 − )zM
xM = : (23)
2
Inserting Eq. (23) into Eq. (18) leads to

M 2 + 4(1 − )
d ˜ [(1 −  −  + zM + ( − zM + 1 − )2 + 4(1 − )z)]
=  : (24)
d M 2 + 4(1 − )
[(1 −  −  + zM + ( − zM + 1 − )2 + 4(1 − )z)]

After incorporating Eq. (16), Eq. (24) can be readily solved

by a solver for ordinary di$erential equations (Gear, 1971).
Applying the proposed approximations stated above, one
The exact solutions of Eqs. (4), (6a) – (6c) and (21) were
can obtain
obtained in a numerical way, in which the method of collo-
cation based on B-spline interpolation (de Boor, 1978) was d ˜ 1
= (27)
employed for spatial discretization and integration in time d (1 − )(1 − y)
M
was carried out using Gear’s method (Gear, 1971). and
So far, we have derived approximate formulas for the ad-
   
6 18
sorption systems with a constant surface di$usivity. In the yM = 1 − exp − √ ˜ 0:5 − − 3 ˜ − 4:4145˜1:5 :
following, we will further elaborate on the cases involving  
concentration-dependent surface di$usivity. The adsorption (28)
of the sorbent particle via surface di$usion may be viewed When the Volmer isotherm is applied, the surface di$u-
as mass transfer from the particle surface to a sphere with sion coeKcient has the form (Garg & Ruthven, 1972)
uniform distribution of the adsorbed phase. Thus, the ef- Do
fective surface di$usion coeKcient lies between the value Da = : (29)
(1 − q=qm )2
at particle surface and the one evaluated based on the av-
erage amount of adsorbed phase. In the present work, we Employment of the present approximations leads to Eq. (28)
propose to use a geometric mean of these two limits to and
evaluate its e$ective value. For the Langmuir isotherm the d ˜ 1
dependence of surface di$usion coeKcient on the amount = : (30)
d (1 − )(1 − y) M
of adsorbed phase can be described by (Garg & Ruthven,
1972)
3. Results and discussion
Do
Da = : (25)
1 − q=qm The accuracy of the developed formulas for constant
Neglecting the accumulation and transport of 3uid phase surface di$usivity has been examined using three adsorp-
within the particle, one can write the dimensionless mass tion systems with quite di$erent adsorption characteristics.
balance equation for the adsorbed phase as The adsorption and di$usion parameters for each system

   are listed in Table 1. Calculations were all carried out for
@y 1 @ 2 1 @y a clean particle subjected to a step change in the surface
= 2  : (26)
@  @ 1 − y @ concentration. The results in Fig. 1 show the ratios of
2436 H.-K. Hsuen / Chemical Engineering Science 58 (2003) 2433 – 2440
Fig. 1. Ratio of approximate uptake to its exact value for system A: (
( ) Carta and Cincotti (1998).
approximate uptake calculated using the present formulas
to its exact value for system A at various adsorption times.
The ratios calculated based on Zhang and Ritter’s model
(1997), Carta and Cincotti’s model (1998), and the general
driving force model developed by Yao and Tien (1998) are
also given in the /gure for comparison. Inspection on the
value of equivalent Henry’s constant (=qm bp =
p ) for low
concentration of pore 3uid of system A reveals that it has
a very strong adsorption isotherm and, thus, the amount of
adsorbed phase inside the particle is much greater than that
of pore 3uid. Despite of a smaller value of surface di$u-
sivity, the surface di$usion term still dominates the mass
transport inside the particle due to the much higher concen-
tration of the adsorbed phase. As derived previously, all the
Langmuir isotherms can be converted to the same dimen-
sionless expression (Eq. (21)). The degree of nonlinearity
of such a dimensionless expression can be quanti/ed by the
parameter . As  is close to zero, the isotherm behaves lin-
early. On the other hand, high nonlinearity is expected as
 approaches unity. In Fig. 1, results are presented for four
di$erent values of , namely 0.01, 0.4, 0.9 and 0.99, so as
to investigate the e$ects of nonlinearity of the adsorption
isotherm on the accuracy of the approximations. It has been
shown that excellent accuracy was found for the present
formulas for four  values. It indicates that high accuracy
can be always achieved independent of the degree of non-
linearity of the isotherm for the system investigated. This
observation is attributed to the dominance of surface di$u-
sion in the intraparticle mass transport and of the amount of
adsorbed phase in the total uptake. Yao and Tien’s model
(1998) gives fairly good results for the  values of 0.01,
0.4 and 0.9 but greatly overestimates the uptake amount for
•) present work; (4) Yao and Tien (1998); (
) Zhang and Ritter (1997);
 = 0:99. Although the formulas of Zhang and Ritter (1997)
and of Carta and Cincotti (1998) are derived based on dif-
ferent assumptions, they reduce to an equivalent form of the
LDF as the adsorption isotherm becomes linear. Therefore,
both of them bear the same disadvantages as the LDF. As
seen, these two formulas seriously underestimate the uptake
at short times for the four values of . For  = 0:01; 0:4 and
0.9, the results obtained using Zhang and Ritter’s (1997)
and Carta and Cincotti’s (1998) formulas are quite close to
each other and cannot be distinguished in the /gure. How-
ever, for  = 0:99 Zhang and Ritter’s formula (1997) yields
higher ratios than Carta and Cincotti’s (1998) for the entire
time domain.
Fig. 2 compares the accuracy of the four approximate
models at four di$erent  values for the ethane-5A zeolite
system (B). This system also appears to be a strong adsorp-
tion one. However, accumulation of pore 3uid and pore dif-
fusion play more important roles in the di$usion equations
as compared with system A. Such characteristics imply that
the degree of nonlinearity of the adsorption isotherm cov-
ered by the intraparticle concentration pro/le might exhibit
signi/cant impacts on the accuracy of the present formu-
las. As seen in Fig. 2, the present formulas gives excellent
predications for  = 0:01 and 0.4, and accuracy decreases
as the  value increases. In other words, larger deviations
appear for a higher degree of nonlinearity of the adsorption
isotherm. Such an observation was also found for Yao and
Tien’s Model (1998); nevertheless, their model yields much
greater errors for  = 0:9 and 0.99. Similar to system A
(Fig. 1) both Zhang and Ritter’s formula (1997) and Carta
and Cincotti’s formula (1998) give extremely low ratios at
short times. These two formulas yield almost same results
 H.-K. Hsuen / Chemical Engineering Science 58 (2003) 2433 – 2440
Fig. 2. Ratio of approximate uptake to its exact value for system B: (
( ) Carta and Cincotti (1998).
Fig. 3. Ratio of approximate uptake to its exact value for system C: (
( ) Carta and Cincotti (1998).
for  = 0:01. However, Zhang and Ritter’s (1997) formula
leads to higher ratios for  = 0:4; 0:9 and 0.99.
Comparisons carried out in Fig. 3 are for the hydrogen-
activated carbon system (C), in which the ratios of approx-
imate uptake calculated using the four approximate models
to its exact value at four di$erent  values are presented.
According to the parameter values given in Table 1, this
system is considered to be a weak adsorption one. In such
2437
•) present work; (4) Yao and Tien (1998); (
) Zhang and Ritter (1997);
•) present work; (4) Yao and Tien (1998) (
) Zhang and Ritter (1997);
a system, both pore di$usion and surface di$usion play sig-
ni/cant roles in the intraparticle mass transport. In addition,
both the pore 3uid and the adsorbed phase substantially con-
tribute to the overall uptake of the adsorbent. Thus, accu-
racy of the present formulas is expected to be in3uenced by
the degree of nonlinearity of the isotherm covered by the in-
traparticle concentration pro/le. As shown, the present for-
mulas give excellent results for  = 0:01 and yield slight
2438 H.-K. Hsuen / Chemical Engineering Science 58 (2003) 2433 – 2440

Fig. 4. Ratio of approximate uptake to its exact value for the system with variable surface di$usivity and the Langmuir isotherm: ( •) present work;
( ) Carta and Cincotti (1998).

Fig. 5. Ratio of approximate uptake to its exact value for the system with variable surface di$usivity and the Volmer isotherm: ( •) present work;
( ) Carta and Cincotti (1998).

overestimates for  = 0:4. For  = 0:9 and 0.99 large devi-
ations are only observed at short times due to the increased
nonlinearity of the adsorption isotherm. As the sorbate dif-
fuses into the inner part of the adsorbent, surface di$usion
and accumulation of adsorbed phase become less important
because of the decreased ratio of the adsorbed phase con-
centration to the pore 3uid concentration. In addition, ac-
companied by the increase of sorbate concentration at the
particle center, the portion of Langmuir isotherm covered
by the intraparticle concentration pro/le shrinks. All these
factors lead to smaller errors of the present formulas at
relatively long times. Yao and Tien’s Model (1998) also
yields pretty good results for  = 0:01 and 0.4, but greatly
overestimates the uptake amount for  = 0:9 and 0.99. The
results calculated by Zhang and Ritter’s (1997) and Carta
and Cincotti’s (1998) formulas are similar to those of the
 H.-K. Hsuen / Chemical Engineering Science 58 (2003) 2433 – 2440 2439

previous cases; both of them seriously underestimate the up- Volmer isotherms. The developed formulas compare well
take at short times. with the exact solutions of the general adsorption and di$u-
Fig. 4 presents the results obtained using the present for- sion model over a wide range of nonlinearity of adsorption
mulas and the one developed by Carta and Cincotti (1998) isotherms. The computational results also revealed that
for the case of variable surface di$usion coeKcient as de- the present formulas provide more accurate predications
scribed by the Langmuir equation (Eq. (25)). The approxi- than other related ones reported in the literature for the
mations developed by Yao and Tien (1998) and by Zhang conditions currently investigated.
and Ritter’s (1997) were not included for comparisons since
their models do not take into account the concentration de-
pendence of surface di$usivity. As seen, excellent agreement Notation
between the results obtained using the present formulas and
the exact solutions for  = 0:1. The deviations increase as b Langmuir isotherm parameter, m3 =kg
 increases. From Eq. (26) it is quite clear that the mag- c concentration of 3uid phase, kg=m3
nitude of  directly re3ects the variation range of surface cs surface concentration of 3uid phase, kg=m3
di$usion coeKcient, and hence the accuracy of the approxi- Do di$usivity parameter, m2 =s
mation for the e$ective surface di$usivity. For an extremely Dp pore di$usivity, m2 =s
small value of , the present approximation approaches an Da surface di$usivity, m2 =s
exact one since the di$erence between the upper and the f dimensionless adsorption isotherm expressed as a
lower limits of surface di$usivity vanishes. Larger errors are function of x
expected as  is increased. As illustrated, for  = 0:9 fairly q concentration of adsorbed phase, kg=kg
good results are still obtained from the present formulas with qm Langmuir isotherm parameter, kg=kg
the maximal percentage error around 9%. As  is increased qs surface concentration of adsorbed phase, kg=kg
to 0.99, the maximal percentage error rapidly increases to Q adsorption isotherm expressed as a function of
about 31%. On the other hand, Carta and Cincotti’s (1998) c; kg=kg
formulas seriously underestimate the uptake amount at short r radial coordinate, m
times just like the previous cases with constant surface R particle radius, m
di$usivity. x dimensionless concentration of pore 3uid
The results given in Fig. 5 are for the sorbent particles xM average dimensionless concentration of pore 3uid over
in which the concentration dependence of surface di$usion the adsorbent
coeKcient is described by the Volmer equation. Although y dimensionless concentration of adsorbed phase
the Volmer equation exhibits a higher degree of nonlinear- yM average dimensionless concentration of adsorbed
ity than the Langmuir one in the surface di$usivity, the ac- phase over the adsorbent
curacy of the results obtained using the present formulas do t time, s
not deteriorate seriously as compared to the counterparts of z variable de/ned by Eq. (13)
the previous case. For the same reason mentioned above,
the decrease of accuracy is also observed as  is increased. Greek letters
It is also seen that the present formulas yield much better
predictions than the one developed by Carta and Cincotti’s  ratio of e$ective surface di$usivity to pore di$usivity,
(1998) since their model seriously underestimate the uptake de/ned by Eq. (7d)
amount at short times.
p particle porosity
 dimensionless radial coordinate, de/ned by Eq. (7e)
 partition ratio at particle surface, de/ned by Eq. (7c)
4. Conclusion  dimensionless step change in surface concentration,
de/ned by Eq. (22)
Approximate formulas for parallel pore and surface p particle density, kg=m3
di$usion in a spherical adsorbent governed by a nonlin-  dimensionless di$usion time, de/ned by Eq. (7f) or
ear adsorption isotherm were derived in the present study. by Do t=R2 for Eqs. (26), (27) and (30)
The developed formulas provide a quantitatively correct ˜ dimensionless di$usion time, de/ned by Eq. (10)
prediction of sorbate uptake for an adsorbent subjected to
a step change in the surface concentration. The E$ects of
the features of adsorption isotherm and of di$usion mech-
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