Chemical Engineering Science 66 (2011) 2587–2595

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Chemical Engineering Science

journal homepage: www.elsevier.com/locate/ces

The effect of reliable prediction of final pressure during pressure equalization

steps on the performance of PSA cycles
Milad Yavary a,b, Habib Ale-Ebrahim a,b,n, Cavus Falamaki a,b
a
Chemical Engineering Department, Amirkabir University of Technology, P.O. Box 15875-4413, Tehran, Iran
b
Petrochemical Center of Excellency, Amirkabir University of Technology, P.O. Box 15875-4413, Tehran, Iran

a r t i c l e i n f o abstract

Article history: The present work aims at modeling the performance of isothermal PSA cycles for the production of H2
Received 15 November 2010 from refinery fuel gas by introducing a more reliable calculation of the final pressure during the
Received in revised form pressure equalization steps. The latter calculation is performed based on the law of conservation of
8 February 2011
mass in a system comprehending the depressurizing and pressurizing beds in contact. Single adsorbent
Accepted 7 March 2011
(zeolite 5A) dual and six-bed PSA processes have been considered. The PSA cycle performance is
Available online 24 March 2011
compared with a conventional model considering an arithmetic mean for the final pressure during the
Keywords: pressure equalization steps (old model). It is shown that the new model predicts lower values for
Pressure equalization step product purity and recovery when compared with the old model. The error in the estimation of the
PSA
product recovery is larger than the corresponding value for product purity and may exceed 9%. It is
Adsorption
shown that the error in the calculation of purity and recovery strongly depends on the number of beds.
Separations
Mathematical modeling The error in the calculation of product recovery increases approximately two-fold increasing the
Simulation number of beds from 2 to 6. Therefore, the present study shows that implementation of a more robust
method for the evaluation of final pressure during the equalization steps is imperative for the
development of new models of industrial PSA processes, especially for the number of beds exceeding 2.
& 2011 Elsevier Ltd. All rights reserved.

1. Introduction has prompted the development of processes to recover hydrogen

Pressure swing adsorption is an interesting gas separation
process because of its low energy requirement and capital
investment cost (Ribeiro et al., 2009). In the recent decades,
pressure swing adsorption (PSA) systems have been changed
and modified regularly. Also, their application has expanded from
bulk gas separation and drying to purification and trace contami-
nant removal. One of the earliest PSA cycles was introduced by
Skarstrom (1959), originally suggested for air drying using a
simple dual-bed unit. Nowadays, more efficient processes have
been developed for an increasing number of commercial applica-
tions. A significant difference between the Skarstrom and the
recently applied multibed process is that the latter has some
additional steps such as pressure equalization and concurrent
blowdown in the PSA cycle for modifying the process perfor-
mance. These additional steps help enhance both product purity
and product recovery significantly (Doong and Yang, 1987).
By increasing the demand of hydrogen for petroleum refinery and
petrochemical processing, an economic aspect of these applications
n
Corresponding author at: Chemical Engineering Department, Amirkabir University
of Technology, P.O. Box 15875-4413, Tehran, Iran.
E-mail addresses: mld.yavary@aut.ac.ir (M. Yavary), alebrm@aut.ac.ir
(H. Ale-Ebrahim).
with high purification from steam reformer off gas, catalytic naphtha
reformer off gas, and ethylene plant effluent gas (Yang and Lee, 1997).
In many important industrial applications, high purity hydrogen is
used, such as hydrocracking, hydrogenation of fats and oils, methanol
production, manufacture of silicon, etc. Furthermore, due to the
recent environmental concerns, developments in the fuel cell industry
towards the replacement of fossil fuels by hydrogen were prompted,
and as a result, water is released from the combustion instead of
greenhouse gases. These important applications justify the high
motivation for advanced research in the field of high purity
(99.99%) hydrogen production. Recovery of purified hydrogen from
various process gases constitutes the largest commercial application
of PSA separation (Malek and Farooq, 1997, 1998).
At present, the PSA processes are used widely for H2 recovery
in the chemical and petroleum refining industries. To define the
performance of PSA processes, purity and recovery of H2 obtained
by performing both experiments and mathematical modeling
have been used (Yang et al., 2008). In these processes, several
adsorbents such as alumina, activated carbon, and zeolite are
used. In most cases, some impurities should be pretreated first to
avoid adsorption of major impurities in the main adsorbent
section (Chlendi and Tondeur, 1995). As an adsorbent, zeolite
5A is widely used in the main section of the adsorption bed in PSA
processes (Yang and Lee, 1997).

0009-2509/$ - see front matter & 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ces.2011.03.005
2588 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595

The incorporation of pressure equalization steps in pressure The component and overall mass balance for this system are
swing adsorption cycles may result in a considerable improve- represented by Eqs. (1) and (2a, 2b) for constant pressure steps
ment of product recovery and energy consumption. It is essential and variable pressure steps, respectively. Variation in the gas
to apply a robust mathematical model for the prediction of the interstitial velocity over the length of the bed is described by Eqs.
effect of pressure equalization steps on the process performance. (2a) and (2b).
Recently, Chahbani and Tondeur (2010) discussed the predic-
@2 ci @ci @c @u 1ebed @qi
tion of final pressure in the pressure equalization steps. Its major DL þ þ u i þ ci þ ¼0 ð1Þ
importance in simulation of PSA processes is the elimination of @z2 @t @z @z ebed @t
simplifying assumptions and precise prediction of process’s beha-
@u 1ebed X n
@qi
vior. In prior works, final pressure in pressure equalization steps C þ ¼0 ð2aÞ
was considered to be either the arithmetic or the geometric mean @z ebed i ¼ 1 @t
of two bed’s pressures. The present work aims at modeling the
performance of isothermal PSA cycles for the production of H2 @u @C 1ebed X n
@qi
C þ þ ¼0 ð2bÞ
from refinery fuel gas by introducing a more reliable calculation @z @t ebed i ¼ 1 @t
of the final pressure during the pressure equalization steps. The
latter calculation is performed based on the model of Chahbani where DL is the dispersion coefficient (m2/s), i is the component
and Tondeur (2010). Single adsorbent (zeolite 5A) dual and six- (B¼CH4, A ¼H2), z is the axial position (m), t is the time (s), u is
bed PSA processes for purification of hydrogen from a mixture of the interstitial gas velocity (m/s), R is the gas constant (J/mol/K), T
hydrogen and methane (as an impurity) will be considered. The is the gas temperature (K), P is the gas pressure (Pa) within the
PSA cycle performance is compared with conventional models bed, and ebed is the bed voidage.
considering arithmetic means for the final pressure. As the main The sorption rate into the adsorbent (qqi/qt) could typically be
goal is to show the importance of the accurate calculation of described by an LDF model as follows:
pressure, isothermal performance was considered for the sake of @qi
¼ ki ðqi qi Þ ð3Þ
brevity. It will be shown that the incorporation of the aforemen- @t
tioned calculation results in significant changes in the purity and
recovery of the final product. The effect of different process 15Dei
ki ¼ ð4Þ
variables (adsorption pressure, feed velocity, P/F ratio: ratio of R2p
the H2 purge stream volumetric flow rate to the H2 feed stream
where ki is the effective LDF coefficient within the solid phase
volumetric flow rate) on product purity and recovery of the cycle
(s  1), qn is the equilibrium value of concentration of component i
steps and concentration profiles will be considered.
in the solid phase (mol/m3), qi is the solid concentration of
component i in the solid phase (mol/m3), Dei is the effective
diffusivity of component i in the solid (m2 s  1), and Rp is the
2. Mathematical model and numerical simulation
radius of the spherical adsorption particle. The boundary condi-
tions of each step are given in Table 1.
The mathematical model is based on the following simplifying
The Langmuir–Freundlich isotherm was used to predict the
assumptions:
adsorption equilibrium, and it was extended to predict the
multicomponent isotherm by the following loading ratio correla-
(i) adsorption and desorption steps are considered to be
tion (LRC) equation:
isothermal;
(ii) ideal gas law; qmi bi Pini
qi ¼ P n ð5Þ
(iii) flow pattern is described by an axially dispersed plug 1 þ nj¼ 1 bj Pj j
flow model;
(iv) adsorption equilibrium is represented by the LRC isotherm where the isotherm parameters are functions of temperature:
for a binary mixture;
qm ¼ k1 þ k2 T, b ¼ k3 ek4 =T , n ¼ k5 þk6 =T ð6; 7; 8Þ
(v) there are no radial variations in the concentration or
velocity; and The coefficients of the isotherm equation were taken from the
(vi) adsorption rate is approximated by a linear driving force paper of Yang and Lee (1997). These coefficients are shown in
(LDF). Table 2.

Table 1
Boundary conditions.

Steps Mass balance Velocity


Adsorption (AD) i  u9z ¼ 0 ¼uOH
DL @c @z z ¼ 0 ¼ u9z ¼ 0 ðci 9z ¼ 0 ci 9z ¼ 0 þ Þ
þ

@ci 
@z z ¼ L ¼ 0

Feed pressurization (FP) i  u9z ¼ L ¼ 0
DL @c z ¼ 0 þ ¼ u9z ¼ 0 ðci 9z ¼ 0 ci 9z ¼ 0 þ Þ
 @z
@ci 
@z z ¼ L ¼ 0

@ci 
Depressurizing pressure equalization (DPE) u9z ¼ 0 ¼0
@z z ¼ 0 ¼ 0

@ci 
@z z ¼ L ¼ 0

Pressurization pressure equalization (PPE) i  u9z ¼ L ¼ 0
DL @c@z z ¼ 0 ¼ u9z ¼ 0 ðci 9z ¼ 0 ci 9z ¼ 0 þ Þ
þ

@ci 
@z z ¼ L ¼ 0

@ci 
Blowdown (BD) u9z ¼ L ¼ 0
@z z ¼ 0 ¼ 0

@ci 
@z z ¼ L ¼ 0

@ci 
Purge (PR) u9z ¼ L ¼ uOL
@z z ¼ 0 ¼ 0

i 
DL @c@z z ¼ L ¼ u9z ¼ L ðci 9z ¼ L ci 9z ¼ L Þ

 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595 2589

To calculate the cycle recovery and purity, Eqs. (11) and (12) latter has been generally treated as an ordinary depressurization of
were used (Huang et al., 2008): the high pressure column (from P1 to Peq) and as an ordinary
R tAD pressurization of the low pressure column (from P2 to Peq) consider-
ðucH2 Þ9z ¼ L dt
PurityH2 ¼ R tAD 0 ð9Þ ing a constant pressure at the open end of the columns (Peq). The
0 ðucH2 þucCH4 Þ9z ¼ L dt

R tAD R tPG
ðucH2 Þ9z ¼ L dt ðucH2 Þ9z ¼ L dt
RecoveryH2 ¼ R 0tPR R0tAD ð10Þ
0 ðucH2 Þ9z ¼ 0 dt þ 0 ðucH2 Þ9z ¼ 0 dt

Purity is calculated at the end of the adsorption step. The

required values for calculation of recovery are obtained at
adsorption, feed pressurization, and purge steps.

2.1. Cycle sequences

The cycle sequences used for the dual and six-bed PSA processes
are summarized in Tables 3 and 4, respectively. The latter is based on
a new algebraic model derived for complex PSA cycle schedules
reported by Mehrotra et al. (2010). The six-bed cycle comprises four
equilibration steps for each column, two pressurizing pressure
equalization and two depressurizing pressure equalization.
In this method, the solution identifies all the cycle schedules
for a given number of beds, the minimum number of beds
required to operate the specified cycle step sequence, the mini-
mum number and location of idle steps to ensure alignment of
coupled cycle steps, and a simple screening technique to aid in
identifying the best performing cycles that deserve further
examination. The effect of different cycle sequence design on
process performance for a six-bed PSA system is the subject of a
separate future work of the authors of the present work.

2.2. Calculation of the final pressure in pressure equalization steps

Pressure equalization step between two beds is shown in Fig. 1.

Till now, because of modeling difficulty of the equalization step, the

Table 2
Equilibrium parameters of Langmuir–Freundlich isotherm.

k1 k2 k3 k4 k5 k6

H2 4.31  0.01060 0.002515 458.2 0.9860 43.03

CH4 4.89  0.00896 0.000534 1795.9 0.396 187.4

Table 3
Cycle sequence for dual-bed process.

Bed 1 FP AD DPE BD PG PPE

Bed 2 BD PG PPE FP AD DPE
Fig. 1. Pressure equalization step.

Table 4
Cycle sequence for six-bed unit process.

Bed1 Adsorption DPE1 DPE2 BD PG PPE1 Idle PPE2 FP

Bed2 PPE2 FP Adsorption DPE1 DPE2 BD PG PPE1 Idle
Bed3 PG PPE1 Idle PPE2 FP Adsorption DPE1 DPE2 BD PG
Bed4 BD PG PPE1 Idle PPE2 FP Adsorption DPE1 DPE2 BD
Bed5 DPE1 DPE2 BD PG PPE1 Idle PPE2 FP Adsorption
Bed6 Adsorption DPE1 DPE2 BD PG PPE1 Idle PPE2 FP Adsorption

AD: adsorption, BD: blowdown, FP: feed pressurization, PG: purge, DPE: depressurizing pressure equalization, and PPE: pressurizing pressure equalization.
Steps duration for dual-bed:
tAD ¼ tPG ¼ 18tcycle/50, tBD ¼tFP ¼ 3tcycle/50, tDPE ¼ tPPE ¼4tcycle/50, tcycle ¼ 500 s.
Steps duration for six-bed:
tAD ¼ tcycle/3, tBD ¼tFP ¼ tcycle/9, tPG ¼3tcycle/18; tDPE1 ¼ tPPE1 ¼tDPE2 ¼ tPPE2 ¼tidle ¼tcycle/18, tcycle ¼540 s.
2590 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595

equilibrium pressure has been considered to be either the arithmetic for the equilibrium pressure can be obtained by applying some
or the geometric mean of P1 and P2 (Chiang, 1996). In the following, simplifying assumptions (see Chahbani and Tondeur (2010).
an analytical solution for calculation of Peq based on the model For the design of cycle sequences, following assumptions are
proposed by Chahbani and Tondeur (2010) is presented. The original considered:
model cannot be solved analytically. However, an analytical solution
 process is isothermal;
 each column is considered homogenous at the initial and final
states;
Table 5  gaseous and solid phases are in equilibrium at the initial and
Bed and adsorbent characteristics. final states; and
 equalization time is large.
Adsorption bed
Bed length, L (cm) 100
Bed inside radius, RBi (cm) 2.2
The mass balance for two beds, before and after pressure
Bed outside radius, RBo (cm) 2.55
Bulk (bed) density, rb (g/cm3) 0.739 equalization steps, leads to the following equations:
External void fraction, e 0.315 pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
B2 4AC B
Adsorbent
Peq ¼ ð11Þ
2A
Pellet size (spherical) 4–8 mesh
Average pellet size, Rp (mm) 1.57
Pellet density, rp (g/cm3) 1.16 y10A P1 þ y20A P2
m¼ ð12Þ
2

Fig. 2. Pressure history: (a) dual-bed and (b) six-bed.

 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595 2591

et average of these values in the bed length was used. P1 and P2 are
n ¼ rb ðq10 þ q20 Þ þ ðP1 þ P2 Þ ð13Þ
RT the bed 1 and bed 2 pressures, respectively.

2et b
A¼ ð14Þ
RT 2.3. Numerical solution

A The Successive Substitution (SS) method was devised to solve

B ¼ ð2rb qm nÞbþ ð1bmÞ
b Eqs. (1), (2a), (2b), and (4) (Liu et al., 1998; Gerald and Wheatley,
C ¼ nðmb1Þ2rb qm bm
where et is the total porosity, qm and b are the isotherm
coefficients, y10A and y20A are the initial mole fraction of component
A (here hydrogen) of beds 1 and 2, respectively, and q10 and q20 are
the initial amount of adsorbing component (here methane) of
beds 1 and 2, respectively; for the calculation of q01 and q02, an
ð15Þ
2004). The parameters used for the adsorption beds and adsorbent
ð16Þ are listed in Table 5. As the LDF coefficient increases moderately with
the adsorption pressure, average values were used (0.587 and
0.049 s  1 for H2 and CH4, respectively). These values were confirmed
by breakthrough experiments in previous work (Yang and Lee, 1997).
Mass axial dispersion coefficient was chosen to be about 6 cm2 s  1.
The composition of the feed gas (moisture free) was chosen as
70 vol% H2 and 30 vol% CH4.

Fig. 3. Adsorption pressure effect on process performance: (a) dual-bed and (b) six-bed (P/F ratio of 0.11 and a feed velocity of 2.2 cm s  1).
2592 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595

3. Results and discussion 3.1. Adsorption pressure effects

Fig. 2a and b shows the pressure history during the nth cycle
for dual and six-bed systems (n a1). Throughout the following
discussion, we compare the results of our model (new model)
with the results from a model obtained using the arithmetic mean
for the evaluation of the final pressure during the pressure
equalization steps (old model). The value of final pressure at
pressure equalization step computed with the new model for
dual-bed process is 5.36 atm (and 6 atm from old method). The
values for six-bed process are 6.42 and 3.14 atm from the new
method (7.67 and 4.33 atm from old method) at the first and
second depressurizing pressure equalization steps.
The effect of the adsorption step pressure on process performance
with a P/F ratio of 0.11 and a feed velocity of 2.2 cm s  1 is shown in
Fig. 3a (dual-bed) and b (six-bed). Despite the rapid variation in H2
purity for pressures below 9 atm, recovery declines almost linearly
with pressure changes. Comparison between the new and old model
results shows that the performance differences are significant. For the
dual-bed process, difference in percentages of purity between the two
mathematical models varies in the range of 0.18–0.35%. The corre-
sponding range for the recovery parameter is 4.06–4.11%. For the six-
bed process, the range of variation for purity difference is about 0.5–
1.2%. These values for recovery are 8.4% and 9.6%. It is observed that

Fig. 4. Axial profiles of the H2 mole fraction in the gas phase at the end of the adsorption step: (a) dual-bed and (b) six-bed (P/F ratio of 0.11 and a feed velocity of
2.2 cm s  1).
 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595 2593

the difference in the results for the six-bed process is more significant.
It is noticeable that the recovery is more sensitive to adsorption
pressure increase and its changes are more significant (compared to
purity).
The predicted axial profiles of the H2 mole fraction in the gas
phase at the end of the adsorption step are shown in Fig. 4a and b.
Since the slope of the mass-transfer zone becomes steeper at
higher pressures, beds can be used more effectively, and simulta-
neously higher purity of the product is achievable. However,
when pressure exceeds 11 atm, the difference between the con-
centration profiles becomes smaller. The reason is that the
adsorption isotherm converges to the maximum limit adsorption
amount at higher pressures. Fig. 4a shows that the concentration
profiles for the dual-bed system are very close for the new and old
model. However, for the six-bed system, the new model predicts a
significantly different axial profile with respect to the old model.
It should be mentioned that the new model is theoretically more
sound and robust and hence its results are more realistic.
3.2. P/F ratio effects
The effect of purge to feed ratio (P/F ratio) on the performance
of dual and six-bed systems for an adsorption pressure of 11 atm
and a feed velocity of 2.2 cm s  1 is shown in Fig. 5a and b. As far
as the purity and recovery are concerned, the new and old models
predict significant different performances.
For the two-bed process, difference in product purity between
the two simulation models changes from 4.26% to 3.71% in the P/F
ratio range of 0.075–0.175. Generally, the new model predicts

Fig. 5. P/F ratio effect on process performance: (a) dual-bed and (b) six-bed (adsorption pressure of 11 atm and a feed velocity of 2.2 cm s  1).
2594 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595

lower values for the product recovery and purity with respect to
the old one.
For the six-bed process, the difference in product purity
between the two models is approximately constant and equal to
0.81% within the P/F ratio range of 0.075–0.175. The error due to
the implementation of an arithmetic mean for the final pressure
increases significantly as the number of beds is increased from
2 to 6. The difference of product recovery between the two
models for the six-bed process is appreciable and varies from
9.3% to 8.95% within the P/F ratio range of 0.075–0.175. Again,
the difference in the calculated recovery between the two
model increases significantly by increasing the number of beds
from 2 to 6.
3.3. Feed velocity effects
One of the key parameters in determining the performance of
the PSA process is the linear velocity. Fig. 6a (dual-bed) and b (six-
bed) shows the process performance obtained with different
linear velocities at an adsorption pressure of 11 atm and a P/F
ratio of 0.11.
For the dual-bed process, the difference in product purity
between the two models is approximately zero at the extreme
values of 1.1 and 3.3 cm s  1. However, a maximal difference of
0.27% is observed at a middle velocity of 2.2 cm/s. The difference
in product recovery between the two models varies from 4.26% to
3.44% with the feed velocity varying from 1.1 to 3.3 cm s  1.

Fig. 6. Feed velocity effect on process performance: (a) dual-bed and (b) six-bed (adsorption pressure of 11 atm and a P/F ratio of 0.11).
 M. Yavary et al. / Chemical Engineering Science 66 (2011) 2587–2595
For the six-bed process the difference between the calculated
results of the two models within the velocity range of
1.1–3.3 cm s  1 is significant for both product recovery and purity.
The difference for the product purity changes in the range of
0.8–1.2% and for the recovery in the range of 9.2–8.48% for the
velocity range of 1.1–3.3 cm s–1.
4. Conclusions
It is essential to adopt a robust mathematical model to predict
accurately the impact of pressure equalization steps in modeling
the PSA processes. It has been shown that rough approximations
usually considered for the evaluation of the final pressure would
lead inevitably to erroneous simulations. The accurate assessment
of PSA performance including pressure equalization steps
strongly depends on how this step is mathematically modeled.
The analytical solution of Chahbani and Tondeur (2010)
provides a more realistic mathematical procedure with respect
to the use of an arithmetic mean for the calculation of the final
pressure for the pressure equalization steps. Compared to an
isothermal model using an arithmetic mean for the calculation of
final pressure (old model), generally, the new model predicts
significantly different values for the product purity and recovery
parameters (lower values). It was observed that product recovery
is more affected by the new final pressure calculation procedure
than product purity. The effect of implementation of the new
model on PSA performance is more pronounced when the number
of beds is increased from 2 to 6. Error in the evaluation of product
recovery may reach 4% and 9% for dual and six-bed processes,
respectively. Increase in performance difference of PSA processes
with more beds is because of the additional number of pressure
equalization steps eventually accumulating the discrepancies due
to the individual beds.
2595
Therefore, the present study shows that implementation of a
more robust method for the evaluation of final pressures is
imperative for the development of new models of industrial PSA
processes, especially for the number of beds exceeding 2.
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