J Radioanal Nucl Chem (2011) 287:609616

DOI 10.1007/s10967-010-0878-9

The behavior of xenon dynamic adsorption on granular activated

carbon packed bed adsorber
Chongyang Zhou Shujuan Feng Guoqing Zhou
Yuren Jin Junfu Liang Jingming Xu

Received: 2 August 2010 / Published online: 26 October 2010

Akademiai Kiado, Budapest, Hungary 2010

Abstract In order to retard radioxenon release into the

atmosphere from nuclear power station or to sensitively
monitor its concentration to ensure environmental and
human safety, it is necessary to know the behavior of xenon
dynamic adsorption on granular activated carbon pack bed
adsorber. The quantities, including the dynamic adsorption
coefficient (kd), the amount of xenon adsorbed (q), the
length of mass transfer zone (LMTZ) and the length of the
unused bed (LUB), used to describe the adsorption
behavior, were sorted out and calculated. The factors,
including xenon concentrations, pressures and temperatures, to affect these quantities were investigated. The
results show that: (1) The values of kd and q decrease with
increasing temperatures, but increase with increasing
pressures, (2) The values of LMTZ and LUB increase with
increasing temperatures or pressures, but are independent
of concentrations. Knowledge of these quantities is very
helpful for packed bed adsorber operation.

DP
h
LMTZ
LUB
t0.05

t0.50

t0.95

W
q
qm
b

Keywords Adsorption  Design  Activated carbon 

Packed bed
List of symbols
C0
Equilibrium concentration of inlet gas (V V-1)
kd
Dynamic adsorption coefficient (L g-1)
F
Volumetric flow rate of the inlet gas (mL min-1)
C. Zhou  J. Liang  J. Xu (&)
Division of Nuclear Chemistry and Technology, Institute
of Nuclear and New Energy Technology (INET), Tsinghua
University, Beijing 100084, Peoples Republic of China
e-mail: [email protected]
C. Zhou  S. Feng  G. Zhou  Y. Jin
Northwest Institute of Nuclear Technology, P. O. Box 69-1,
Xian 710024, Peoples Republic of China

T
Q
R
A0

Pressure drop (kPa)

Depth of the bed (cm)
Length of mass transfer zone (cm)
Length of unused bed (cm)
Breakthrough time (the time when the outlet
concentration is at 5% of the inlet concentration)
(min)
Equilibrium time (the time when the outlet
concentration is at 50% of the inlet concentration)
(min)
Saturation time (the time when the outlet
concentration is at 95% of the inlet concentration)
(min)
GAC mass in the packed bed (g)
Gravimetric capacity or amount adsorbed
(mL K-1)
Saturation amount adsorbed for a single
monolayer (mL K-1)
Constant corresponding with both adsorption and
desorption rates in Langmuir equation
Absolute temperature (K)
Adsorption heat (kJ mol-1)
Gas constant (J K-1 mol-1)
Pre-exponential factor

Abbreviations
GAC Granular activated carbon
GC
Gas chromatograph
TCD
Thermal conductivity detector
Introduction
In the atmosphere, xenon is one of the least stable noble
gases, and at a concentration of 0.087 cm3 m-3, it is not

123

610

123

the quantity LUB is used to scale the bed up from the

experimental size [13]. If these two quantities were also
combined to evaluate xenon adsorption on packed bed, it
should have become integrity.
The LMTZ, LUB and q were combined to explain the
properties of packed bed and q was quantitatively compared for the adsorption of acetone and toluene vapor
somewhere [14]. However, kd has not been calculated there
because they fitted the values of q and equilibrium concentrations (C0) following Langmuir and Freundlich
equations. It is well known that Langmuir equation can be
transformed into Henry equation at low concentrations and
in that case, kd can be called Henry constant.
Normally, if the quantities, such as kd, q, LMTZ, and
LUB, are applied, the breakthrough curve is the first to be
determined, where the dynamic adsorption experiment on
packed bed have been performed. For a real packed bed,
the operational factors, such as temperatures, pressures,
flowrates and concentrations, will affect these quantities
more or less and these should be determined by experiment
for different kind of adsorbent and adsorbate pair.
In this publication, we discuss xenon adsorption on
GAC, and present our method for calculating the pertinent
quantities from the xenon breakthrough curve. After these
quantities are calculated, the design and evaluation of
packed bed adsorber is simplified, and the dependencies
between these quantities manifest themselves.

Theoretical
Breakthrough curve
The breakthrough curve is an S-shaped curve that results
from the hindrance inside the packed bed adsorber of the
xenon profile by the mass-transfer force, as shown in
Fig. 1. For dynamic adsorption, obtaining the breakthrough

Cx/C0 100

easy to extract. Also present in the atmosphere are

radioxenon isotopes, such as 133Xe or 135Xe, which are
produced by artificial fission or from spontaneous fission of
heavy nuclei (238U, 240Pu, etc.) [1]. The artificial source
includes nuclear tests, nuclear power stations, nuclear
reactors, etc.
Nuclear power is an important component of the
response to societys ever-increasing demands for energy.
The concentration of artificial fission nuclides in the
atmosphere, including radioxenon, will increase due to
the increasing number of the nuclear power stations. For
the nuclear fuel 235U, the 133Xe yield is 6.77% and the
amount of 133Xe is 2.57 9 1014 Bq g-1 (235U) [2]. Since
the radioxenon yield is high and it disperses easily, the
leakage or release of this radioactive gas presents a public
health concern.
Two important steps are still required to protect the
public from radioxenon from nuclear power stations: one is
to take measures to retard its release into the atmosphere,
and the second is to sensitively monitor it to ensure environmental and human safety [35]. Because the absolute
quantity of radioxenon and stable xenon in the atmosphere
is fairly low, the adsorption separation technique has been
adopted to enrich the xenon and to separate out large
amounts of undesired compounds such as He, N2, O2, etc.
In order to achieve these two purposes, the special equipment is required to be developed. Normally, the granular
activated carbon (GAC) is chosen to adsorb xenon and the
key component for the special equipment is the packed bed
adsorber, which involves the quantities of designing and
evaluating.
kd and q are the two important quantities which characterize the capacity of GAC and can be used to design
packed bed [6]. The value of kd is the volume of gas stream
adsorbed by per unit weight of GAC, where the volume of
adsorbate adsorbed is called q. As q varies depending on
the concentration, it is not suitable as a basis for packed
bed design. At low concentrations (less than several thousands times of 10-6 V V-1), kd remains nearly constant
and can be used for packed bed design. For a known volume adsorbed of a given gas, the weight of GAC needed
for packed bed adsorption can be calculated using kd. With
the GAC weight known, the volume of GAC, as well as the
packed bed geometry, can be calculated.
GAC adsorbers were widely used for the adsorption of
radioactive noble gases produced by nuclear power stations, where kd was the main discussed quantity [711]. It
is not simple to know how to evaluate the packed bed
properties from the literature mentioned above, so the
depths of the bed were chosen randomly [10]. Fortunately,
the evaluation quantities of the packed bed, such as LMTZ
and LUB, can be found in other literatures. The quantity
LMTZ is related to premature solute breakthrough [12] and

C. Zhou et al.

100
95
90
85
80
75
70
65
60
55
50
45
40
35
30
25
20
15
10
5
0
40

50

60

t0.05 70 t0.50

80 t0.95

tx(min)

Fig. 1 Breakthrough curve

90

100

110

120

Behavior of xenon dynamic adsorption on GAC packed bed adsorber

curve is necessary to get the quantities kd, LMTZ, LUB and

q.
The curve has three characteristics: steepness, geometric
midpoint, and shape. From these characteristics, the
breakthrough times, equilibrium (midpoint), and saturation
are found [15, 16]. Combined with the flow rate, gas
concentration, packed bed volume, and GAC mass, the
quantities mentioned above can be calculated.
Adsorption isotherms
Langmuir equation can be used to depict adsorption isotherms. One form of Langmuir equation can be described
as following,
C0
1
C0

bqm qm
q

where b is the constant corresponding with both adsorption

and desorption rates, and qm is the amount adsorbate
adsorbed for a single monolayer.
At low concentrations, Eq. 1 can be shortened as
q kd C 0

This is the form of Henry equation.

Dynamic adsorption coefficient and amount adsorbed
kd and q are both affected by the GAC properties, the
temperatures, the flow rates, the pressures, the gas components, etc.
kd can be derived from mass balance of a packed bed
adsorber [5]. The GAC adsorption capacity is described by
kd, which can be expressed as [68, 17, 18],
kd

F  t0:50
W

where F, t0.50, and W are the inlet gas volumetric flow rate,
the equilibrium time (defined as the time when the outlet
concentration is at 50% of the inlet concentration), and
GAC mass in grams, respectively. The traditional
description of adsorption capability involves the quantity
q. As for a breakthrough curve, combining with Eq. 1, the
approximately method to calculate is,
q

F  t0:50  C0
kd  C0 :
W

where A0 is called pre-exponential factor, Q adsorption

heat, T absolute temperature, and R gas constant.
Length of mass transfer zone and length of unused bed
LMTZ is the length of the packed bed pertinent to the
breakthrough curve. This quantity is used to judge if the
depth of the packed bed is reasonable. After the mass
transfer zone is formed, its length remains constant for
constant velocity and it moves forward in the direction of
the gas stream. In practical engineering design, the depth of
the packed bed is chosen to be over twice LMTZ [19].
According to Pota and Mathews [12], LMTZ is calculated as
LMTZ

2t0:95  t0:05 h
:
t0:95 t0:05

LUB is the part that adsorption is not occurred and a

principle component of packed bed adsorber design. LUB
is used to account for the spreading of the concentration
front. Because LUB is affected by flow rate but not
affected by bed length, so it is used to scale up packed bed
from experimental size to real application [20]. LUB may
be approximated by


t0:05
LUB 1 
 h:
7
t0:50
Normally, for a symmetrical breakthrough curve, the
following equalities hold.
t0:95 t0:05 2t0:50
t0:95  t0:50 t0:50  t0:05

In this case, the relationship between LMTZ and LUB is

2t0:95  t0:50 t0:50  t0:05  h
t0:95 t0:05
2t0:50  t0:05  h

2LUB
t0:50

LMTZ

where t0.95, t0.05, and h are the saturation time (defined as

the time when the outlet concentration is at 95% of the inlet
concentration), the breakthrough time (the time when the
outlet concentration is at 5% of the inlet concentration),
and the bed depth, respectively.

Here, we obtain q by multiplying kd by the inlet gas

equilibrium concentration (C0). Compared with Henrys
Law, kd can also be called as Henry constant.
Xenon adsorption on GAC is a type of physical
adsorption, so temperature plays an important role. The
effect of temperature on kd and q can be expressed by
kd or q A0 eRT

611

Experimental
Equipment
We used an HP6890 gas chromatograph (GC) equipped
with a thermal conductivity detector (TCD) to analyze the
xenon concentration eluted out of the packed bed. A
stainless steel tube packed with Porapak Q (6080 mesh)

123

612

C. Zhou et al.

was used in the GC column. The carrier gas was purified

helium (99.999%) and the minimum detectable limit for
xenon was 1 9 10-6 V V-1. The operating conditions of
the GC used for analyzing xenon are given in Table 1.
The experiment also required the use of Humonics 650
digital flow meter, which was manufactured by Humonics
Inc., USA, CYG1003 absolute pressure transmitter, Baoji
Sensor Factory, China, and DC-2006 low temperature
thermostatic water bath, Shanghai Balance Instrument
Factory, China.
GAC

FI
2

P
2

V-1

V-3

exit

V-2

5
V-4

V-5

Set-up and operation

He

The GAC packed bed was placed in a thermostatic water

bath. The xenon mixed gas transiting the GAC packed bed
was adjusted by Rota meters and mixed with purified He
and 490 9 10-6 V V-1 (in He) stored in their respective

FI

A coconut shell GAC (Type KSO5, 1428 mesh or

1.650.59 mm) was procured from the Shuangxiong
Industrial and Trading Co., Ltd., Hainan Province, China.
The GAC was used directly as provided by the factory
without sieving, and the indices are listed in Table 2.
The GAC was oven dried at approximately 473 K for at
least 2 h to remove moisture. After cooling in the desiccator, the GAC was weighed and packed into the packed
bed. The packed bed depth was 60 cm and the inner
diameter was 0.80 cm. The volume of the bed was 30.1 mL
and the mass of the packed GAC was 13.4 g. Before performing the adsorption experiment, the packed bed was
wound and heated to 573 K in a muffle furnace for 2 h, and
the He gas was supplied at a volumetric flow rate of
50 mL min-1 from the beginning of heating until the bed
had cooled to room temperature. After each adsorption
experiment the bed was regenerated by the procedure
above described.

cylinders. The xenon concentration eluted from the fixed

bed was monitored sequentially once every 5 min by the
GC. When the adsorption experiment finished, the packed
bed was regenerated. The setup and operation of the
experiment is shown schematically in Fig. 2. The pure
xenon (99.99%) gas and the 490 9 10-6 V V-1 standard
xenon in He equilibrium gas used for calibrating the GC
and for the adsorption experiment were procured from
Beijing AP Beifen Gases Industry Company, Ltd., China.
T, C0 and DP (or F) are the factors that affect the performance of a packed bed. To determine their affect, three
series of experiments were performed. Each series contained at least six experiments, where one factor was varied
and the two others were kept constant. The T, C0 and
DP (or F) values used in the experiments are listed in

V-6

49010-6 VV-1
Xenon (in He)
1 Pressure Gauge
3 Pressure/Vacuum transmitters
5 Digital flow meter

2 Rota meter
4 GAC packed bed adsorber
6 HP6890 GC

Fig. 2 The diagram of the adsorption experiment

Table 1 GC operating conditions

Item

Volume of the
sample loop (mL)

Oven
temperature (K)

Front detector
temperature (K)

Column
flow (mL min-1)

Front detector
ref flow (mL min-1)

Front detector
makeup flow (mL min-1)

Index

0.5

363

478

10.0

35.0

2.0

Table 2 Indices of the GAC

Item

Mesh
size (mm)

Bulk
BET
Pore
density
surface volume
area
(cm3 g-1) (g cm-3)
(m2 g-1)

Index 1.650.59 C 90% C1100

123

Specific
heat (J
K-1
g-1)

0.380.55 0.420.50 -1.00

Hardness
(%)

Moisture
(%)

Ash
(%)

Methylene
pH
Iodine
value number blue
(mg g-1) number
(MI)

Carbon
tetrachloride
(CTC)
number (%)

C95

B10

B5

C7

C55

C1030

C13

T (K)

DP
(kPa)

F
(mL min-1)

C0 (9 10-6 V V-1)

298

298

298

298

298

23.1

18

13.3

9.3

8.2

6.5

369

270

184

109

76.7

48.4

278

288

298

308

318
328

10

11

12

13
14

Average

276

13.8 0.8

14.5
14.8

14.5

13.9

13.3

12.8

12.8

183 2

184
182

183

186

183

184

181

Condition 3: Different temperature

Average

298

52.1 4.8

51.4
46.9

52.1

59.3

49

58.1

48.1

466 6

466

474

470

464

465

455

1
298
14.2 0.7 184 2
18.4470
Condition 2: Different pressure drop or flow rate

Condition 1: Different xenon concentration

No.

24.8
17.2

36.9

54.5

92

145

164

27.6

37.9

55.8

95.7

135

213

56.0 0.9

t0.05
(min)

Table 3 Operating conditions and experimental results for kd, q, LMTZ, and LUB

30.4
21.3

45.4

65.9

108

169

190

33.8

45.2

64.6

108

151

238

66.1 1.1

t0.50
(min)

36.7
26.4

53.8

77.4

128

191

216

41.1

54.3

74.4

122

169

268

76.9 1.6

t0.95
(min)

0.417
0.289

0.619

0.916

1.48

2.32

2.56

0.889 0.028

0.931

0.911

0.887

0.879

0.863

0.86

0.906 0.011

kd
(L g-1)

0.0214
0.0136

0.0323

0.0543

0.0724

0.135

0.123

0.414 0.018

0.434

0.431

0.417

0.408

0.4

0.392

0.01680.417

q
(mL g-1)

23.2
25.3

22.3

20.8

19.8

16.4

16.7

23.6

21.3

17.2

14.4

13.4

13.9

18.9 1.3

LMTZ
(cm)

11
11.6

11.2

10.4

9.04

8.53

8.31

11

9.69

8.22

6.73

6.21

6.43

9.16 0.90

LUB
(cm)

2.10 0.08

2.11
2.18

1.99

2.00

2.19

1.92

2.01

2.15

2.20

2.09

2.14

2.16

2.16

2.06

LMTZ/LUB

Behavior of xenon dynamic adsorption on GAC packed bed adsorber

613

123

614

C. Zhou et al.

Table 3. In conditions 1, 2 and 3, the corresponding variable was T, C0 and DP (or F), respectively.

Results and discussion

Data
The experimental results for kd, q, LMTZ, and LUB are
shown in Table 3. We processed the experimental data
according to the equations mentioned above and found that
the kd average value is around 0.90 L g-1 (at 298 K),
which was consistent with the previously reported kd value
of 1.0 L g-1 [9]. For all data, the ratio h/LMTZ falls within
the range 2.374.48 and that range of h/LUB is 5.179.66.
The LMTZ/LUB ratio is 2.10 0.08, indicating that the
breakthrough curve is almost symmetric.
Effect of pressure drop on the flowrate
As shown in Fig. 3, in order to increase the F, the frontal
pressure should be high enough. Their effect of DP on
F was shown in Fig. 3. The DP and F are in conformity
with each other and we are going to discuss the effect of
DP on the quantities when they are the variables.

concentration in the gas stream must be enhanced to be

above the detection limit. Another difficulty is that the
xenon concentration in the desorption gas will be higher
than in the adsorption gas, so if the desorption gas is
readsorbed the adsorption concentration will become
higher. In all, the effect of the xenon concentration should
be known.
Because of the large specific area of GAC, the adsorbed
particle is far less probable to occupy the adsorption site
provided by GAC because the xenon concentration is low.
According to this logic, the xenon concentration will affect
none of the quantities except q. To experimentally verify
the effect on the quantities of the xenon concentration, the
volumetric flow rates and temperatures were kept constant.
We found that the inlet xenon concentration had no affect
on kd, LMTZ and LUB. q, however, was affected, indicating
that neglecting the effects of concentration on all the
quantities except q is justified.
The relationship between C0 and q is shown in Fig. 4,
where q is linear in C0 with a positive slope. This indicates
that the specific surface area of the GAC is sufficiently large
to allow it to provide enough sites for adsorption. Thus, the
adsorption rate is rapid, and there is negligible interaction
between xenon molecules adsorbed on neighboring sites.
The linear fit to the data shown in Fig. 4 yields
q 9:03  104 C0 9:12  104

Effect of xenon concentration on the quantities

In practical terms, the ultimate goal is to concentrate xenon
on the GAC, so the xenon concentration should be considered in these experiments. However, two difficulties
exist in regards to detection of the xenon concentration.
One is that the xenon concentration in air is well below the
TCD detection limit for GC. In order to study the dynamic
adsorption property of xenon on GAC, the xenon

10

When C0 [ 10, the intercept in Eq. 10 may be

neglected, so Eq. 10 reduces to the form of Eq. 2. It can
be known that the lowest experimental concentration is
18.4 9 10-6 V V-1 (that is C0 = 18.4), so the effect of
intercept in Eq. 10 can be neglected and then that is the
case of Eq. 2.
Here, the value of Henry constant equals to
0.903 L g-1.

400

0.500

350
F= 19.3 P - 75.9
R2 = 0.999

-4

q= 9.0310 C0 + 9.1210

0.400

250

-1

q(mL g )

F(mL min -1 )

300

200
150

0.300
0.200

100

0.100

50

0.000
0

0
5.0

10.0

15.0

20.0

25.0

-4

R = 0.9997

100

200

300
6

400

500

-1

C0 (10 V V )

P(kPa)

Fig. 3 Effect of the pressure drop (DP) on the flow rate (F) for the
packed bed

123

Fig. 4 The fitted line between the different xenon concentration (C0)
and the adsorbed amount (q) of GAC (temperature 298 K, flow rate
184 2 mL min-1, pressure drop 14.2 0.7 kPa)

Behavior of xenon dynamic adsorption on GAC packed bed adsorber

615

Effect of the pressure drop on the quantities

28.0

To operate the packed bed adsorber, it is necessary to know

how the DP (or F) affects adsorption. The dependence of
kd, q, LMTZ and LUB on DP is shown in Fig. 5, where the
temperatures and concentrations were kept constant. All
four of these quantities increase to varying degrees with the
DP (or F) values. The adsorption capacity thus is increased
with increasing DP.

LMTZ , LUB(cm)

LMTZ

24.0
20.0
LMTZ = 0.163T - 28.2
R2 = 0.9687

16.0

8.0
270

30.0

1.00
kd

L MTZ , LUB(cm)

0.80

k d = 4.29 10 -3 P + 0.832
R2 = 0.981

LMTZ = 0.656 P + 8.73

R2 = 0.975

0.70

15.0
10.0

0.60

LUB = 0.302 P + 4.10

R2 = 0.982

0.50

5.0

q = 25310 -3 P + 0.381
R2 = 0.930

0.0
5.0

10.0

15.0

k d(L g -1 ), q(mL g -1 )

0.90

25.0
20.0

P(kPa)

Fig. 5 Effect of pressure drop (DP) of the packed bed on the values
of dynamic adsorption coefficient (kd), length of mass transfer zone
(LMTZ) and length of unused bed (LUB) (temperature 298 K, flow rate
48.4369 mL min-1, xenon concentration (466 6) 9 10-6 V V-1)

0.00

1.50
lnq

-0.50
-1.00

lnk d = 3.80/T - 12.8

R2 = 0.9998

-1.50
-2.00
-2.50

0.00

-3.00
-0.50

-3.50

lnq= 3.91/T- 16.2

R2 = 0.9910

lnq(mL g -1 )

lnk d(L g -1 )

1.00
0.50

-4.00

-1.00

-4.50
-1.50
3.00

3.10

3.20

3.30

3.40

3.50

290

300

310

320

330

340

3.60

Fig. 7 Effect of the operational temperature (T) on the values of the

length of mass transfer zone (LMTZ) and the length of unused bed
(LUB) for the packed bed (flow rate: 183 2 mL min-1, pressure
drop: 13.8 0.8 kPa, xenon concentration: (52.1 4.8) 9 10-6
V V1)

The vant Hoff equation for kd is



3:80  103
6
kd 2:76  10 exp
:
T

11

The adsorption heat for xenon on GAC is

31.6 kJ mol-1, which agrees well with the value of
Strong and Levins [17], who found 29 kJ mol-1 for
radon adsorption on activated carbon.
It is clear that high temperature degrades the adsorption
efficiency because the adsorption force weakens, causing
LMTZ and LUB to lengthen, as shown in Fig. 7.

Conclusions

0.40
0.30
25.0

20.0

lnkd

280

T(K)

Adsorption is an exothermal process and the adsorption

capacity is much higher at low temperatures than at
ambient temperatures.
q and kd follow a vant Hoff equation [20]. Figure 6
shows the logarithm of kd and of q plotted versus inverse
temperature. LMTZ and LUB are proportional to temperature, as shown in Fig. 7.

LUB

LUB= 0.0657T- 9.65

R2 = 0.9244

12.0

Effect of temperature on the quantities

LMTZ

LUB

-5.00
3.70

T-1 (10 3 K-1 )

Fig. 6 Effect of the reciprocal of operational temperature (T) on the

values of dynamic adsorption coefficient (kd) and adsorbed amount
(q) for the GAC (flow rate: 183 2 mL min-1, pressure drop
13.8 0.8 kPa, xenon concentration (52.1 4.8) 9 10-6 V V1)

To use GAC to adsorb xenon, it is necessary to design and

evaluate breakthrough for a packed bed adsorber. In this
publication, we present a method of calculating the relevant quantities; i.e., kd, q, LMTZ, and LUB. For practical
situations, the dependence of these parameters on factors
such as temperature, flow rate, and concentration, were
discussed.
The length of the packed bed for this experiment is
60 cm and the ratio h/LMTZ is within the range of
2.374.48, which is above the required value of 2 for the
packed bed design. This means that the packed bed length
chosen is reasonable. The breakthrough curve of xenon
adsorption on GAC is almost symmetric by the value of
LMTZ/LUB = 2.10 0.08 and kd, which can be used to
design packed bed, is about 0.90 L g-1 at 298 K. kd can
also be called as Henry constant.
The main factors to affect the behavior of packed bed
are pressure and temperature. LMTZ and LUB increase with
the increasing of pressures or temperatures; kd and
q increase with the increasing of pressures, but decrease
with the increasing temperatures. The adsorption heat for
xenon on GAC is 31.6 kJ mol-1.

123

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