Journal of the Taiwan Institute of Chemical Engineers 43 (2012) 428–432

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Journal of the Taiwan Institute of Chemical Engineers

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Packed bed redistribution system for Cr(III) and Cr(VI) biosorption by

Saccharomyces cerevisiae
Margarita E. Ramı́rez Carmona a,*, Mônica A. Pereira da Silva b, Selma G. Ferreira Leite b,
Oscar H. Vasco Echeverri a, Carlos Ocampo-López a
a
Universidad Pontificia Bolivariana, Facultad de Ingenierı´a Quı´mica – CIBIOT, Circular 1a, No. 70-01, Medellı´n, Colombia
b
Escola de Quı´mica, Universidade Federal do Rio de Janeiro, Brazil

A R T I C L E I N F O A B S T R A C T

Article history: Saccharomyces cerevisiae yeast was immobilized on residual pumice for trivalent and hexavalent
Received 3 May 2011 chromium solution adsorption inside a PVC column of 4.3 cm diameter, 140 cm length by using a novel
Received in revised form 13 September 2011 redistribution system. Metallic solutions were fed through the packed bed column in order to establish
Accepted 5 December 2011
breakthrough curves, inlet solution conditions were 300 mg/L and 200 mg/L for Cr(III) and Cr(VI)
Available online 2 January 2012
respectively, pH value for Cr(III) was 4.3 and 1.66 for Cr(VI), the effluent solution was analyzed at equal
time intervals, obtaining breakthrough points of 240 min for Cr(III) and 300 min for Cr(VI). It was found
Keywords:
that redistribution system for chromium removal by Saccharomyces cerevisiae increases contact sites
Packed bed Column
Breakthrough curve
between yeast and metallic ion due to liquid flow ability through the column and the results were better
Chromium if compared with a fixed column without redistribution. Removal percentages of 53.7% and 60% for Cr(III)
Redistributor and Cr(VI) respectively were obtained.
Saccharomyces cerevisiae ß 2011 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Biosorption

1. Introduction in terms of energy and chemical products consumption, especially

The presence of heavy metal ions in wastewater is one of the most
critical environmental impacts of present time [1]. Chromium and
its compounds are released into natural environment from a variety
of anthropogenic sources, including electroplating, leather tanning
processes, chromite ore processing, wood preservation, alloys
making, corrosion control, pigment and dyes, and metal industries.
Chromium exists principally in hexavalent and trivalent forms [2].
Hexavalent form is more toxic than trivalent and it requires
more concern. Cr(VI) is found more toxic and highly soluble in
water, whereas Cr(III) is less toxic and less soluble. Strong exposure
to Cr(VI) causes cancer in digestive tract and lungs and may cause
epigastric pain, nausea, vomiting, severe diarrhea and hemorrhage.
Trivalent form is absorbed inside the digestive tract to generate
toxic complex compounds with proteins affecting both human and
animal health. Due to that fact, chromium removal from
wastewater before disposal is an essential factor [3,4].
Conventional physiochemical methods for metals remediation
include precipitation, filtration, coagulation, evaporation, ion
exchange, membrane separation and solvent extraction. However,
application of these processes is always expensive and ineffective
* Corresponding author. Fax: +57 4 411 87 79.
E-mail address: margarita.ramirez@upb.edu.co (M.E. Ramı́rez Carmona).
at low metal concentrations between 1 and 100 mg/L [5].
Furthermore, besides a strong metallic affinity, the study of a
low-cost and easily available adsorbent has led to the investigation
of agricultural materials as potential metal adsorbents [6].
Wastewaters with low concentrations of Chromium are usually
treated with ion exchange resins, but the high cost of resins limits
its industrial application [7]. Biosorption is a popular and effective
technique for metal recovery from wastewaters, it utilizes the
potential of dead biomass to remove heavy metal ions from
aqueous solution by physicochemical mechanisms [8].
The process engineering advantages of a packed bed adsorption
column with immobilized biomass offer an easy scale up, which is
an important aspect of the biosorption processes [9]. Packed bed
column studies include the effect of bed height, flow rate and initial
metal ion concentration on biosorption of chromium(VI) [10]. The
efficiency of a packed bed is highly dependent on liquid
distribution; it implies that if a packed bed does not operate
satisfactorily, a faulty design or incorrect installation of the
distribution system could be the cause [11].
Liquid streams inside the packed bed columns tend to channel
themselves and flow through columns walls, where minor flow
resistance is reached [12,13]. That fact causes unfavorable
operational conditions and it increases requirements of redistri-
bution systems which could be located at the initial part of the
column or through bed’s length.

1876-1070/$ – see front matter ß 2011 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.jtice.2011.12.002
 M.E. Ramı́rez Carmona et al. / Journal of the Taiwan Institute of Chemical Engineers 43 (2012) 428–432 429

2. Materials and methods

Nomenclature
2.1. Biosorbent
A area under breakthrough curve [MQ/L]
C0 final metallic ion concentration [M/L3] Heavy metal biosorbent used for biosorption process was
Cad adsorbed metallic ion concentration [M/L3] residual brewery Saccharomyces cerevisiae, supplied by ‘‘Cervecerı́a
Cdin dynamic capacity of the column. Metal adsorbed Unión S.A.’’ in Medellin Colombia. It consists in a viscous liquid
until breakthrough time/biosorbent mass [M/M] composed by 155 g/L of yeast in dry weight.
Ceq equilibrium concentration inside the column
((amount of metallic ion fed into the 2.2. Preparation of heavy metal solution
column  amount of adsorbed metallic ion)/efflu-
Cr(III) and Cr(VI) solutions were prepared from
ent total volume) [M/L3]
KCr(SO4)212H2O and K2Cr2O7 salts respectively, with an approxi-
Ci initial ion concentration [M/L3] mated concentration of 300 mg/L and 200 mg/L, these concentra-
De equivalent diameter [L] tion values were set according to concentration values of the
L column’s length [L] effluents in local leather tannery industry. Solutions pH were then
Lmin minimum bed’s length [L] set to 4.34 and 1.66 for Cr(III) and Cr(VI) respectively according to
Lsat saturated bed’s length [L] previously optimization study of biosorption [14]. Solutions
LUB unused bed’s length [L] standardization were carried out by using atomic absorption
mal/tb metal fed into the column until breakthrough time spectroscopy (Perkin Elmer, 3100).
[M]
2.3. Biosorption operation in packed bed column
mnad/tb non-added metal [M]
mad/tb absorbed metal until breakthrough time [M]
For biosorption operation it was used immobilized yeast inside
mtotal total amount of metallic ion fed into the column
a PVC column of 4.3 cm of diameter (f) and a 140 cm of length (L).
[M] The mechanical support used for the packed bed column was
Q volumetric flow [L3/Q] residual pumice from textile industry, with a void fraction of 0.67.
qeq equilibrium metallic ion captation. Amount of Bed particles diameter were 0.53 cm, and redistributor particles
absorbed metallic ion/biosorbent mass [M/M] diameter were 0.3 cm, corresponding approximately to a 1/8 and
qtotal amount of absorbed metallic ion [M] 1/14 of column diameter respectively, Fig. 1 shows the column
SP particle specific surface [L2] specifications. Bed and redistributor length was determined by
T residence time. bed’s volume/volumetric flow
[L3Q/L3]
tb breakthrough time [Q]
ts saturation time [Q]
ttotal total operational time of the column [Q]
Veff effluent total volume. Volumetric flow  total
operational time of the column [L3]
f column diameter [L]
X biosorbent mass [M]
e void fraction (porosity). Empty volume/Bed’s
volume [L3/L3]

The column system consists in two sections, in the superior part

is installed a column distributor in order to divide homogeneously
the inlet flow and assure an effective contact between the fluid and
the packed bed. The second is the packed section where
biosorption occurs. Additionally there is a redistribution system
which function is to retain the liquid that is flowing through
column walls and direct it over the cross section of the column.
Redistributor is made of a section of smaller particles inside the
packed bed by using the same packing material.
The aim of the present work is to study the removal of chromium
in both Cr(III) and Cr(VI) oxidation states. To achieve that,
breakthrough curves were established by using Saccharomyces
cerevisiae immobilized in residual pumice as the biosorbent, due to
its low cost and mechanical resistance, pumice is a volcanic rock
employed during the jeans fabric wash in order to obtain a desirable
textile finishing. Furthermore, redistribution systems were used
through the columns length to upgrade biosorbent immobilization
on the mechanical support, achieving a better contact between the
metallic solution and the biosorbent through the column. The
characteristic breakthrough s-shaped curves were obtained in the
range of validity according to operational flow value. Fig. 1. Distributor and redistributors scheme.
430 M.E. Ramı´rez Carmona et al. / Journal of the Taiwan Institute of Chemical Engineers 43 (2012) 428–432
Table 1
Bed, redistributor and particle calculations.
Parameter Diameter and length calculations
Relation Diameter Relation
with f (cm) with f
Column 1 4.30 1 140
Bed particles 1/8 0.53 3 13
Redistributor particles 1/14 0.30 0.35
Fig. 2. Breakthrough curve construction arrangement.
using operational conditions of packed bed columns, according to
Rhodes [13]. All these values are show in Table 1.
Immobilized microorganisms were pumped and recycled into
the column as a suspension with a biomass concentration of 155 g/
L for a period of 8 days; during that period, yeast is adhered
strongly on the interstices of pumice. The amount of immobilized
biomass was determined by quantifying the biomass concentra-
tion each day by dry weight during the 8-day of immobilization
process until the amount of biomass in the samples remain
constant.
After biosorbent immobilization, a continuous biosorption
process was started. The inlet flow to the column was made
downwards by using a peristaltic pump (Cole Palmer, model
77201-60) at a volumetric flow of 15 ml/min. Samples were
collected at the inferior part of the column by using a sample
collector, in posterior analysis samples were used to determine the
final metallic ion concentration (CF). Simplified scheme of
experimental arrangement is shown in Fig. 2.
3. Results and discussion
Changes in particle size inside the packed bed, with smaller void
fraction, provides higher flow resistance to the inlet flow through
the column, as a result of this mechanical phenomena flow is been
obligated to change its behavior through the cross section of the
column.
One explanation for such behavior consists in the assumption
that liquid flowing inside packed bed flows downwards through
little straight channels of equal diameter (De) [11].
e of chromium removal inside continuous systems. Experimental
De ¼
S p ð1  eÞ
Channel diameter (De) is a function of particles properties, e.g.
DeA (for bigger particles) is different from DeB (for smaller
particles). At a smaller particle diameter, bed’s void fraction
would be smaller. B particles have a smaller bed’s void fraction
than A particles. Furthermore, the particles specific surface (Sp)
Length increases with the decrement in particle diameter, which SpA < SpB,
(cm) this implies that hypothetical De decreases in proportion with
particle size decrement. For B particles void fraction (e) decreases
in relations with an increment of A and SpB and increases in relation
1.5 with SpA in this order ½1=e  1 will increase and the term S½1=e  1
will also increase, decreasing De (Fig. 1).
The Cr(VI) concentrations in the effluent, were higher than zero,
this could be attributed to the initial flow rate conditions that could
have been too high. According to Treybal [15] and Aksu et al. [16]
the flow rate is an important factor involved in the biosorption
process.
Breakthrough point observed for Cr(III) ions was early than that
for Cr(VI) ions, possibly the chemical properties of Cr(VI) and Cr(III)
are different. Cr(VI), considered the most toxic form of chromium,
is usually associated with oxygen as chromate (CrO24) or
dichromate (Cr2O27) ions. In contrast, Cr(III) in the form of
oxides, hydroxides or sulfates, is much less mobile [17]. Most cells
are impermeable to Cr(III) probably because it forms water
insoluble compounds in non-acidic aqueous solutions, similar
validation was exposed for Leite et al. [18].
Kogej and Pavko [19], finding out that lower metal uptake
efficiency is a consequence of the packed bed non-uniformity, the
formation of channels and zones of unexploited biomass within
the bed was inevitable. Besides this disadvantage, channeling is
another inconvenience that commonly occurs because of clogging
of the biomass. Flow inappropriate distribution leads to unwanted
residence time distributions over and above that occurring due to
axial mixing [20].
The target here consists in achieve a uniform flow distribution
in the catalyst bed, with the flow predominately in a radial
direction. In brief, the internal design was such that flow entered
the column across the entire cross section and proceeded
downwards near the wall of the column, then radially inwards
through the bed of 3 mm particles, and finally outwards in a
downwards direction via an axial collector [20].
According to Mark et al. [11], the ideal flow distribution is one
that is radially and angularly invariant so that the entire bed is
exposed to a uniform temperature and treatment time is
minimized. Because fluid flow through a packed bed is extremely
sensitive to even small variations in local void fraction, a uniform
porosity distribution is essential to minimize an inappropriate flow
distribution. For this reason, packed bed chemical reactors are
often loaded using methods and devices that assure consistent and
minimum bed porosity usually called a dense loading.
Studies of packed-bed structure are numerous; most have
focused on porosity variations near walls. Other than those
comparing dense and loose loading, there are comparatively
few treatments of the effect of loading method on bed’s void
fraction variations and flow distribution throughout the result-
ing bed. In addition the majority of theoretical work has deal
with spherical particles whereas extruded shapes are more
common in commercial practice. Mark et al. [11], show a
difference between free pouring and rainy filling, the latter
created by a horizontal distributing grid, by radio gauging local
bulk densities in a flat vertical model filled with 3 mm
cylindrical pellets.
After yeast immobilization with the help of the redistribution
system, breakthrough curves were plotted to observe the behavior
(1) data can be plotted using several relationships among them: final
metal concentration versus time (C0 vs t); relation between final
metal concentration and initial metal concentration versus time
(C0/Ci vs t) or final metal concentration versus effective volume (C0
 M.E. Ramı́rez Carmona et al. / Journal of the Taiwan Institute of Chemical Engineers 43 (2012) 428–432 431

Fig. 3. Breakthrough curves for Cr(III) and Cr(VI) with redistribution system.

vs Veff) [21]. Normalized plotted data (C0/Ci vs t) is needed to obtain The methodology employed in a packed bed adsorption process
models that describe the process or to scale-up processes. Fig. 3 determines the breakthrough curves shape and breakthrough
illustrates breakthrough curves for Cr(III) and Cr(VI) biosorption at time. Breakthrough time or breakthrough point, the point where
process conditions before mentioned. the slope ascends, for both of trivalent and hexavalent chromium

Fig. 4. Breakthrough curves for Cr(III) and Cr(VI) without redistribution system.

Table 2
Cr(III) and Cr(VI) continuous system biosorption process parameters.

Parameter Expression Cr(III) Cr(VI)

Length diameter relation L/D 32.6 32.6

Bioadsorbent mass (g) X 61.4 61.4
Breakthrough time (min) tb 240 300
Saturation time (min) ts 1260 2700
Saturated bed’s length (cm) Lsat = L  LUB 44 33
h i
t
Unused bed’s length (cm) LUB ¼ L 1  tb 68 79
h i
t
Minimum bed’s length (cm) Lmin ¼ L 1  tbs 90.7 99.6

QA
R t¼ttotal
Amount absorbed metal ion (mg) qtotal ¼ 1000 ¼ t¼0 C ad dt 2956 3691

C 0 Qt total
Total amount of metal ion fed to the column (mg) mtotal ¼ 1000 5509 6156
q
Total removal percentage (%) % ¼ mtotal  100 53.7 60
total

qtotal
Equilibrium metal ion concentration (mg/g) qeq ¼ X 48 60

mtotal qtotal
Equilibrium concentration inside the column (mg/L) C eq ¼ Ve f f  1000 135 61

metalad=tb
Dynamic capacity of the column (mg/g) C dinamica ¼ X 4.5 1.7

Amount of metal adsorbed until tb (g) metalad/tb = met . alim/tb  met . noad/tb 277.2 106.9
Effluent total volume (L) Veff = Qttotal 18.9 40.5
Residence time (min) t ¼ V Lecho
Q 108.4 108.4
432 M.E. Ramı´rez Carmona et al. / Journal of the Taiwan Institute of Chemical Engineers 43 (2012) 428–432
ions was determined according to Treybal [15], breakthrough time
decreases with the bed length increment, adsorber particle size
increment, rise on the volumetric flow through bed’s length and
with increment in the initial solute concentration at columns feed.
These values were of 4 h for Cr(III) and 5 h for Cr(VI). Similar
breakthrough curves are show by other authors and researchers
Pentchev et al. [22], Volesky and Prasetyo [23], Kratochvil et al. [24]
and Antunes et al. [14]. Breakthrough curves constructions is
important for industrial scale-up of their equipment, but some
authors Muraleedharan et al. [25], Huang et al. [26], Monser and
Adhoum [27] and Kratochvil et al. [24], do not study the influence
of pressure loss through column length, physical–mechanical
behavior of the supports, once column size does not exceed a
length of 50 cm an a diameter of 2.5 cm.
The Cr(VI) effluent concentration in biosorption process were
higher than zero, it is believed that the initial solute concentrations
at the inlet feed of the reactor were very high for the type of system
used. Comparisons between breakthrough curves obtained for
trivalent and hexavalent chromium with redistribution system
and without redistribution systems (Fig. 4), show that packed bed
gets saturated at 3 h of operation, meanwhile, the present study
reports column saturation times of 21 and 25 h for Cr(III) and
Cr(VI) respectively. It is demonstrated that redistribution systems
increases in an efficient way the contact of immobilized biomass
with heavy metal solution through the column, increasing global
removal efficiency.
Chromium solutions breakthrough curve parameters are shown
in Table 2, calculated from the equations revealed in Aksu and
Gönen [28], Geankoplis [29] and Slejko [30].
Biosorbent dynamic capacity of the column to adsorb metallic
ions was, 4.5 mg/g and 1.7 mg/g for Cr(III) and Cr(VI) respectively,
i.e. the amount of metallic ions removed by 1 g of biosorbent.
Removal percentages for both metallic ions was, 53.7% and 60%
for Cr(III) and Cr(VI) respectively, results obtained for hexavalent
chromium removal percentage were higher than the ones obtained
with immobilized activated sludge and activated coal, 22.4% and
42.2% respectively [16], nevertheless we cannot compare this two
works, because the biosorbent, column and conditions are not the
same.
Metallic ion adsorbed, total metal concentration fed into the
column, equilibrium metal concentration inside the column and
residence time were higher values that the ones found in different
researches, Zulfadhly et al. [31], Zhao et al. [32], Huang et al. [26]
and Yang and Volesky [33], demonstrating the pertinent redistri-
bution system.
4. Conclusions
The proposed redistribution system for chromium removal by
Saccharomyces cerevisiae increased the contact sites for yeast–
metallic ion, due to the flow ability of the liquid through the
column, because of the uniform porosity distribution of the packed
bed essential to minimizing flow inappropriate distribution
through the cross section of the column.
Biosorbent dynamic capacity of the column to adsorb metallic
ions was, 4.5 mg/g and 1.7 mg/g for Cr(III) and Cr(VI). In contrast
removal percentages for both metallic ions was, 53.7% and 60% for
Cr(III) and Cr(VI) respectively.
Acknowledgement
Margarita Enid Ramı́rez Carmona, Oscar Hernán Vasco Eche-
verri and Carlos Ocampo López express their gratefulness to
COLCIENCIAS (Colombia).
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