Journal of Membrane Science 377 (2011) 191–197
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Journal of Membrane Science
jo u rn al hom epa ge: www.elsevier.com/locate/memsci
Simultaneous separation of H
2
S and CO
2
from natural gas by hollow fiber
membrane contactor using mixture of alkanolamines
Mahdi Hedayat, Mohammad Soltanieh
∗
, Seyyed Abbas Mousavi
Department of Chemical and Petroleum Engineering, Sharif University of Technology, Tehran, P.O. Box 11365/8639, Islamic Republic of Iran
a r t i c l e i n f o
Article history:
Received 12 February 2011
Received in revised form 22 April 2011
Accepted 24 April 2011
Available online 30 April 2011
Keywords:
Hollow fiber membrane contactor
Hydrogen sulfide
Carbon dioxide
Mixed alkanolamines
Natural gas sweetening
a b s t r a c t
In the present work we studied the use of a membrane contactor system for simultaneous absorption
of H
2
S and CO
2
from a gas mixture similar to natural gas. MDEA solution and mixtures of MDEA/DEA
and MDEA/MEA were used as absorbent liquid. PVDF and PSf hollow fiber membranes were used in the
membrane contactor modules. Design of experiments were carried out by Taguchi method in a manner
that a systematical investigation of the effect of operational parameters (temperature, pressure, gas and
liquid flow rates, absorbent concentration and acid gas content of the feed), in addition to the effect of
membrane material and absorbent liquid, was implemented on process performance parameters includ-
ing removal efficiencies, overall mass transfer coefficients and H
2
S to CO
2
selectivity. The results indicate
that liquid side resistance is negligible in comparison with membrane and gas side resistances. Both
membranes were wetted by the liquid, but PSf suffered more. The presence of a dense layer in mem-
brane side adjacent to the liquid, changes the influence of operational parameters. It was observed that
increasing absorbent concentration had a different effect in the presence or absence of CO
2
. Addition of
MEA enhanced the removal efficiencies while DEA had no significant effect.
© 2011 Elsevier B.V. All rights reserved.
1. Introduction
Many industrial gas streams contain acid gases, e.g., CO
2
and
H
2
S. An important example is crude natural gas. These acid gases
are impurities which lower the quality of the gas and cause corro-
sion problems. In addition, H
2
S is a very toxic agent which must
be removed before application of the gas. Removal of acid gases
from natural gas is a well-known process in the industry. Usually
the gas stream is contacted directly with a liquid solvent stream in
a conventional packed bed column.
Contacting gas and liquid streams via a microporous membrane
is an effective alternative for traditional separation processes. In
a membrane absorption system (contactor), the membrane is just
a fixed interface (medium) between gas and liquid streams and
does not offer any selectivity between the gases. This technology
has many advantages over packed columns, e.g., high specific mass
transfer area, modularity of the system with easy scale-up and
independent control of gas and liquid streams which eliminates
operational problems such as flooding and entrainment [1].
Qi and Cussler studied membrane absorption of acid gases for
the first time [2,3]. Since then the majority of studies have been
done on the removal of CO
2
, particularly from combustion gases
∗
Corresponding author. Tel.: +98 21 6616 5417; fax: +98 21 6602 2853.
E-mail address: msoltanieh@sharif.edu (M. Soltanieh).
which are the major sources of greenhouse gas emissions [4]. Few
experimental studies on simultaneous absorption of H
2
S and CO
2
by membrane contactors have been reported. Kreulen et al. [5]
studied selective removal of H
2
S from gas streams containing CO
2
and N
2
. They used MDEA solvent and polypropylene and nylon
66 flat sheet membranes as non-wetted and wetted membranes,
respectively. They found that non-wetted membranes decrease the
H
2
S selectivity. Wang et al. [6] continued their work by using tailor
made poly vinylidene fluoride hollow fiber membrane and sodium
carbonate solution. They found that gas to liquid flow ratio and
CO
2
concentration have significant effect on removal efficiencies
and H
2
S selectivity.
Mathematical modeling of simultaneous absorption of CO
2
and
H
2
S was carried out in recent years. Keshavarz et al. [7] performed
their modeling with DEA as absorbent and investigated wetting
and operational parameters. They found that wetting has a great
influence on CO
2
removal, comparing with H
2
S. Also, decreasing
of DEA concentration mostly decreases the CO
2
removal. Faiz and
Al-Marzouqi [8] performed a modeling with MEA as the solvent.
They found that low concentration of MEA is efficient in complete
removal of H
2
S, but increase of MEA concentration enhances CO
2
removal efficiency.
Wetting of micro pores in membrane absorption of CO
2
has
been a major field of interest for researchers [9–12]. Kreulen et al.
[9] determined mass transfer rates in wetted and non-wetted
microporous membranes. They found that the thickness of the wet-
ted membranes, reduces mass transfer significantly and thus they
0376-7388/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.memsci.2011.04.051