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Journal of Industrial and Engineering Chemistry xxx (2012) xxx–xxx

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Journal of Industrial and Engineering Chemistry


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Review

Factors affecting CO2 absorption efficiency in packed column: A review


L.S. Tan, A.M. Shariff *, K.K. Lau, M.A. Bustam
CO2 Management MOR, Universiti Teknologi PETRONAS, 31750 Tronoh, Perak, Malaysia

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

Article history: Carbon dioxide (CO2) is a major greenhouse gas that results in the climate change. Hence, efforts are in
Received 13 December 2011 place to control CO2 emissions into the atmosphere. CO2 removal is also an essential step in many
Accepted 23 May 2012 industrial processing operations such as coal gasification, natural gas processing and hydrogen
Available online xxx
manufacturing. Thus far, absorption is the widely used process in industrial for capturing CO2. This paper
presents a review on the factors affecting the absorption efficiency for CO2 capture in packed column.
Keywords: Challenges related to the absorption efficiency improvement and the impacts to real application as well
CO2 capture
as future directions are highlighted.
Absorption
Packed column
ß 2012 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights
Amine reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
2. Current technologies for CO2 removal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
3. Overview on solvents commonly used for CO2 capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4. Factors affecting absorption efficiency in packed column . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.1. Physical properties of solvent . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.2. CO2 partial pressure/total system pressure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.3. Gas flow rate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.4. Liquid flow rate. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.5. Absorbent concentration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.6. Liquid temperature . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.7. CO2 loading of solvent . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
4.8. Packing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
5. Major challenges and future prospects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
6. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 000

1. Introduction shows that the world has been heating up since 1980s. It was
reported that greenhouse gases are the glaringly obvious
The recent few years’ simultaneous weather-related cata- explanation for the rise in average global temperatures over the
strophes worldwide show the horrendous effects of global past 50 years [2]. Carbon dioxide, methane, and nitrous oxide are
warming. The United Nation’s network of climate scientists – all long-lived greenhouse gases [3]. However, carbon dioxide (CO2)
the Intergovernmental Panel on Climate Change (IPCC) – has long is well accepted as major greenhouse gas which results in climate
predicted that rising global temperatures would produce more change due to the high ratio of CO2 released to the atmosphere
frequent and intense heat waves as well as rainfalls [1,2]. compared to other greenhouse gases [1,4]. Hence, CO2 is usually
Meanwhile, a report compiled by the National Oceanic and used as a reference for global warming potential [5,6].
Atmospheric Administration (NOAA) in Unites States of America CO2 sources, associated with fossil-fuel energy usage namely
electricity and heat generation, industry and transport, account for
80% of the world’s total CO2 emissions [3,7]. Human activities are
* Corresponding author. Tel.: +60 5 368 7570; fax: +60 5 365 6176. primarily responsible for emissions of CO2 [8]. Based on estimation
E-mail address: azmish@petronas.com.my (A.M. Shariff). by International Energy Agency (IEA) [3], the global CO2 emission

1226-086X/$ – see front matter ß 2012 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.jiec.2012.05.013

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Table 1 Thailand. The Natuna field in the Greater Sarawak Basin in Indonesia
Global CO2 emissions by sector for year 2000–2005 [7].
is the largest gas field in south Asia, with estimated 46 trillion cubic
CO2 emissions by sector Emissions Emissions feet of recoverable reserved. Unfortunately, it remains unexplored
2000 2005 due to high CO2 content at 71% [7]. In Malaysia, CO2 content from
Gt CO2 Gt CO2
natural gas fields varies from 28 to 87%. Over 13 trillions cubic feet of
Electricity and heat production 8 9.6 natural gas reserves are undeveloped due to the presence of high CO2
Industry 6.3 6.8 contents [13]. High CO2 gas fields in Malaysia represent significant
Transport 5 5.2
CO2 capture and storage (CCS) opportunity.
Residential 1.9 2.2
Fuel transformation 0.7 0.9 While natural gas sweetening and post combustion CO2 capture
Commercial 0.7 0.9 technology is readily implemented in plants commercially, there is
Agriculture 0.6 0.7 also emerging pre-combustion technology employed in natural gas
Total 23.3 26.3 plants whereby the methane rich gas is converted into hydrogen
(H2) for combustion [14,15]. The by-product, CO2, produced during
the steam reforming of natural gas, needs to be separated from H2
has increased from approximately 21,000 Mt in year 1990 to before H2 could be fed into combustion turbine. The advantage of
28,000 Mt in year 2006. The CO2 emission rate in year 2010 was pre-combustion process is lower energy penalty compared to post-
estimated at 30,000 Mt and the amount was projected to double up combustion CO2 capture due to higher CO2 concentration and
over the next 50 years [9]. In Malaysia, as a developing country, the elevated pressure [16]. Kvamsdal et al. [17] conducted comparison
CO2 emission has significantly increased by more than 200% from on natural gas fired power plants net efficiency and emission of
approximately 49 Mt in year 1990 to 154 Mt in year 2006 [3]. The CO2 between post-combustion, oxy-fuel and pre-combustion
CO2 emission in Malaysia was projected to increase by more than capture concepts. They concluded that oxy-fuel technology could
100% in year 2030 [10]. Table 1 shows the world CO2 emissions by provide better net plant efficiency, but it has a distant future
sector for year 2000–2005. Recent IEA analysis in Energy perspective for realization.
Technology Perspective (ETP) 2008 projected that the CO2 Globally, there are 62 active or planned commercial scale
emissions attributable to energy sector will increase by 130% by integrated CCS projects, comprising capture, transport and
2050 in the absence of new policies or supply constraints, largely sequestration elements, sequestering of CO2. However, only seven
as a result of increased fossil fuel usage. projects are currently in the operational stage while the rest are in
With the increased awareness on the severity of the global the evaluation, definition, or execution stages [18]. As such, with
warming, concerted efforts are in place to control CO2 emissions more insight generated by continuous and intense research on CCS,
into the atmosphere [6]. The commonly accepted target is to avoid it is expected to accelerate the transition from evaluation to
an increase of the average global temperature beyond 2 8C. It is execution and operational stage.
regarded as the threshold to avoid severe negative impact for life
on mother earth [5]. 2. Current technologies for CO2 removal
CO2 removal is also essential process in sweetening of natural
gas from underground reservoir. Natural gas generally contains a Most attention is currently focused on absorption and
large quantity of methane along with heavier hydrocarbons such membrane separation for the time being due to maturity of the
as ethane, propane, isobutene, normal butane and considerable processes compared to the rest [7,19]. There are also emerging
amount of CO2 [11]. CO2 must be removed from natural gas before novel technologies for CO2 capture such as biotechnology i.e.
use. This is because CO2 is highly corrosive with presence of enzyme based system [7,20,21], electrochemical pumps and
moisture (water) and rapidly destroys pipelines and equipment. It chemical looping [22,23] but extensive research still needs to be
also reduces the heating value of a natural gas stream and wastes conducted to establish the strategy for its integration in industrial
pipeline capacity [12]. processes. Table 2 provides an overview of current CO2 capture
Natural gas in commercial operations includes varying amounts options, issues and their potential.
of CO2 ranging from CO2-free natural gas in Siberia to as high as 90% Notz et al. [24] compared the technologies available for CO2
of CO2 content in natural gas in the Platong and Erawan fields in capture and concluded that reactive absorption with aqueous

Table 2
CO2 capture technologies and its future directions [7,24–29].

Technology Industrial applications Critical issues for large scale application Future needs/emerging trends

Absorption Removal of CO2 from flue gas. Energy requirement for regeneration. Improved process design.
Purification of natural gas. Pretreatment of other acid gases. Solvents with high CO2 capacity and low
regeneration energy.
Rotating absorber.
Novel and improved contacting
equipment.

Membranes CO2 separation in H2 production. CO2 selectivity. Degradation/fouling issue. Ceramic facilitated transport.
Purification of natural gas. Cross-linking the mixed matrix
membranes to attain enhanced
permeability and selectivity.

Cryogenic distillation CO2 liquefaction from gas wells. Refrigeration <0 8C. Hybrid process.
Pretreatment for impurities that freeze Integration with sequestration
above operating temperature (e.g. H2S). processes.
Efficient refrigeration cycles.

Adsorption CO2 separation in H2 production. Adsorbents tend to have low capacity/selectivity. New adsorbents that adsorb CO2 in
Purification of natural gas. Energy penalty for regeneration. presence of water vapor.
Long cycle times. Carbon-based adsorbents.

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amine solutions is considered to be the only attractive option for widely used for years for removing entrained CO2 in raw gas [18].
post-combustion capture. The other technologies are currently less Low hydrocarbon loss is observed in amine system and it could
attractive either for economical reasons or because the technology meet the low CO2 specification required in processed natural gas
is still at a development stage that would only allow industrial [29].
application at a later date. Hence, based on the mature technology Absorption in a physical solvent relies on the solubility of CO2 in
of absorption process, it can be implemented on a large scale in the the solvent rather than a chemical reaction with the solvent. The
near future. solvent is regenerated by changing pressure or temperature.
However, since the CO2 concentration in flue gas from coal fired
3. Overview on solvents commonly used for CO2 capture power plant is typically up to 15% [4,7,25,30], chemical absorption
is generally preferred over physical absorption for CO2 capture in
Absorption processes with chemical solvents are currently the flue gas because of their higher absorption capacity at a low partial
most used technology for CO2 separation from natural gas and pressure of CO2 [31,32].
post-combustion CO2 capture commercially because they are the Among the solvents available, the most popular and widely
most efficient and have lower costs compared to other processes used solvent in industrial process for capturing CO2 is mono-
thus far [27]. In gas processing industry, amine systems have been ethanolamine (MEA) [30,32]. Table 3 summarizes the advantages

Table 3
Summary of solvents commonly studied in chemical absorption process for commercial implementation.

Solvent Advantage Disadvantage Ref.

Monoethanolamine (MEA) - High reactivity and fast absorption rate, - Limited CO2 loading capacity [14,32–38]
which allows absorption to take place due to formation of rather
in a shorter column. stable carbamates.
- Low absorption of hydrocarbon. - Degradation through irreversible
side reactions with CO2 and O2.
-Operational issue such as solvent
loss, foaming, fouling, increased
viscosity and corrosion.

Diethanolamine (DEA) - High reactivity and fast absorption rate. - Limited CO2 loading capacity. [33,34,39]
- The carbamate of DEA is not as stable - Prone to a certain extent of
as the carbamate of MEA. corrosion and solvent degradation.

Methyldiethanolamine (MDEA) - Higher CO2 loading compared to MEA - Slow absorption kinetics with CO2. [16,30,33,
and DEA due to formation of the 34,37,39–43]
bicarbonate ion instead of carbamates.
- Low heat of reaction with the acid gases
which leads to lower energy requirements
for regeneration.
- Lower solvent degradation rate compared
to MEA and DEA.
- Not corrosive to carbon steel.

Diisopropanolamine (DIPA) - Less corrosive than MEA or DEA solutions. - Have moderate rates of reaction [33,35,44]
- Requires less heat in the regeneration of with CO2 and are prone to a certain
the solution. extent of corrosion and solvent
degradation.
- Have a greater selectivity for H2S
over CO2.

2-Amino-2-methyl-1-propanol (AMP) - Higher CO2 loading capacity compared - Lower absorption rate compared [38,45–47]
to MEA. to MEA.
- Requires relatively low energy consumption
for solvent regeneration.
- Induces less corrosion.
- Higher degradation resistance.

Piperazine (PZ) - Higher CO2 loading capacity compared to MEA. - High concentration in solution is not [42,48–53]
- The reaction of CO2 with piperazine is much possible due to its solubility limitation
faster than with conventional carbamate-forming in water. Hence, it is usually used as
amines such as MEA and DEA. promoter for amine systems to improve
- Resistant to thermal degradation up to 150 8C. CO2 mass transfer rates.
- Resistant to oxidative degradation.
- Less volatile than MEA.

Ammonia - High absorption capacity and fast absorption rate. - Temperature in absorber must be lower [14,30,54–57]
- Salts formed from reaction with CO2 can be used than 60 8C to prevent decomposition of
commercially as fertilizers. ammonium bicarbonate (by-product
- Low energy requirement since solvent regeneration from reaction with CO2).
is required. - Highly volatile and often provides an
- Resistance to oxidative and thermal degradation. ammonia slip into the exit gas.

Potassium carbonate (K2CO3) - Significantly lower absorption enthalpy compared - Requires presence of promoting amines [11,24,58–61]
to amine solvent. such as piperazine/high temperature of
solvent up to 75 8C to significantly
increase the otherwise low mass
transfer rate.
- Corrosive to carbon steel; required
corrosion inhibitor.

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Table 4
Summary of CO2 absorption in packed column experimental studies/pilot tests.

Absorbent(s) Type of Name of packing Column inner Variables studied Ref.


packing diameter (mm)

Ammonia Random Pall Rings 597 Configuration of absorbers, packing height, solvent concentration, [62]
CO2 loading of lean solvent, gas flow rate, liquid flow rate
MEA Random Raschig Ring, Not disclosed Gas flow rate, liquid flow rate, type of packing [63]
Intalox Saddle
and Pro-Pak
MEA Random Super Mini Ring 76 Type of packing [64]
(SMR) and Pall Rings
MEA Random Pall Rings Not disclosed Gas flow rate, liquid temperature [65]
MEA Random Raschig Rings 250 Liquid/gas ratio, pressure and packing size [66]
Mixture of Random Raschig Ring 20 CO2 partial pressure, weight ratio of absorbents mixture [67]
MDEA and PZ
Novel amine Random Ring-shaped stainless Not disclosed Liquid flow rate [68]
based solution steel packing
AMP Structured Mellapak 250Y 150 Liquid flow rate, absorbent concentration, CO2 loading in solution, [69]
CO2 inlet concentration
NaOH Structured Mellapak 250Y 427 Surface tension [70]
Mellapak 500Y
NaOH Structured Mellapak 250Y 427 Viscosity and surface tension [71]
Mellapak 500Y
Flexipac 1Y
NaOH, MEA, AMP Structured Sulzer EX 19 Gas flow rate, CO2 partial pressure, liquid flow rate, liquid [72]
Gempak 4A temperature, solvent concentration, solvent type and structured
Sulzer BX packing type
MEA Structured Mellapak 250Y 150 Liquid temperature, gas temperature [73]
NaOH Structured HelieR, Mellapak 38 and 100 Geometric arrangements of packing, packing size, gas flow rate, [74]
250Y, Montz B1-200 liquid flow rate
KOH Structured Mellapak 350Y 100 CO2 loading of lean solvent [75]
AMP Structured Sulzer EX 19 CO2 partial pressure, gas flow rate, liquid flow rate, and solvent [76]
concentration
MDEA Structured Sulzer EX 25 CO2 loading of lean solvent [77]
MEA and blended Structured Sulzer DX 20 CO2 loading of lean solvent, alkanolamine concentration, CO2 [78]
MEA/MDEA partial pressure, temperature, liquid flow rate
MEA, AMP Structured Intalox Saddle, 76 Packing type, solvent type, presence of organic diluents [79]
and random BX gauze, Flexipac
MEA Structured Pall Rings, IMTP, 101 Solvent concentration, packing type, liquid flow rate, gas flow rate, [80]
and random A4-structured packing inlet gas composition, CO2 loading of lean solvent
TS-1, MEA, AMP Not disclosed Not disclosed 160 Type of solvent [81]

and drawbacks of the solvents commonly used/studied in chemical reaction rate constant, k2, and surface tension for NaOH and MEA
absorption process. aqueous solution. Although MEA has lower reaction rate constant
compared to NaOH, the overall mass transfer coefficient, KGav, for
4. Factors affecting absorption efficiency in packed column MEA was higher due to its lower surface tension as indicated in
Fig. 1. Lower surface tension resulted in increased capability of
In recent years, various experimental works have been carried spreading and this behavior tended to maximize the effective area
out to further investigate on efficiency of packed column in CO2 of the packing [72].
removal. Packed column is commonly used as a means of However, the magnitude of impact depends on type of packing.
promoting efficient contact between gases and liquids because Tsai et al. [70] found that reducing surface tension from
it could offer high mass transfer efficiency with low pressure drop approximately 72 mN/m to 35 mN/m minimally impacted the
[61]. The list of researches and pilot tests examining the effect of effective mass transfer area of Mellapak 250Y but yielded
operating condition and column packing structure experimentally substantially higher areas for Mellapak 500Y. It was deduced that
are summarized in Table 4. Insight from factors affecting this was due to the inhibition of capillary phenomena by the
absorption performance in packed column is further discussed reduced surface tension. This indicated that packings with higher
in the following subsections.

4.1. Physical properties of solvent

While viscosity was found to have no effect on the mass transfer


parameter [71], the influence of surface tension could sometimes
prevail over influence of reaction rate in certain cases. Such
behavior was observed by Aroonwilas et al. [72]. Table 5 shows the

Table 5
Second order reaction rate constant, k2, and surface tension for NaOH and MEA
aqueous solution [72].

Parameter NaOH aqueous solution MEA aqueous solution

k2 (m3/(kmol s)) 13,190 at 20 8C 5545 at 25 8C


Surface tension 70.9  103 at 2 kmol/m3 61.8  103 at 3 kmol/m3
at 30 8C (N/m) Fig. 1. KGav comparison between aqueous solutions of NaOH and MEA [72].

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surface area are expected to experience a greater improvement in


effective mass transfer area than packings with lower surface area
under low surface tension conditions.

4.2. CO2 partial pressure/total system pressure

CO2 partial pressure is defined as [82]:

CO2 partial pressure ¼ mole fraction of CO2


 pressure of system (1)

As such, the effect of CO2 partial pressure and total system pressure
is discussed together since the variation of CO2 partial pressure
could be due to concentration of CO2 in inlet gas and/or variation of
the total system pressure itself.
According to Bailey and Feron [83], higher CO2 content in gas
stream resulted in a higher driving force for absorption. Zhang et al.
[67] found that the absorption rate of CO2 in MDEA + PZ was
Fig. 3. Effect of gas flow rate on the overall mass transfer coefficient using AMP [76].
enhanced at elevated CO2 partial pressure while Godini and Mowla
[66] observed similar increased absorption efficiency with increasing
of pressure for MEA system. At high CO2 partial pressure, there was an aqueous solution as shown in Fig. 3. The authors expected that an
increase of the interfacial tension resulting from the concentration increase in the gas load allowed more CO2 molecules to travel from
increase in the interface. This condition would increase the instability gas bulk to the gas–liquid interface, which would result in higher
of the gas/liquid-phase interface and lead to the interfacial mass-transfer performance. Nevertheless, it was deduced that the
disturbance, which is called the Marangoni effect. Buzek et al. [84] mass transfer process in the study was primarily controlled by the
also observed that Marangoni effect significantly enhanced mass resistance residing in the liquid phase. Hence, diffusion of solvent
transfer rate but it could easily be damped by a surface active agent. molecules within the liquid phase was restricted, causing a
Therefore, it was suggested that amine solutions used for absorption constant amount of CO2 absorbed regardless of the gas load values.
should not be contaminated by traces of surfactants. Aboudheir et al. [80] observed increase of CO2 removal
The inability of primary and secondary amine to load up with percentage with reducing the gas feed rate as shown in Fig. 4.
CO2 much beyond 0.5 mol of CO2/mol of amine can be attributed to Higher CO2 removal efficiency using 30 wt% MEA was also
the rather stable carbamates formed. However, a certain amount of observed by Park et al. [63] at lower flue gas flow rate under
carbamate hydrolysis can occur with all amine, particularly at high constant absorbent flow rate. The authors deduced that this was
pressures, and loading for MEA and DEA may exceed 0.5 under this due to shorter gas–liquid contact time with the increase of gas flow
condition [38]. Nevertheless, more investigation on kinetic at high rate.
pressure condition needs to be carried out to confirm this matter. Recently, Yan et al. [4] found that the overall mass transfer
However, Aroonwilas and Tontiwachwuthikul [32] found that coefficient, KGav, showed two distinct behaviors in two regions of
the overall mass transfer coefficient for NaOH increased when the gas flow rate. In the first region where gas flow rate was below
partial pressure of CO2 decreased from 10.0 to 1.0 kPa as shown in 37.5 kmol/(m2 h), KGav was less sensitive to the change in gas flow
Fig. 2. Although the effect was not significant in AMP [32,76], rate. However, in the second region whereby gas flow rate was
further studies on impact of CO2 partial pressure need to be above 37.5 kmol/(m2 h), the KGav values decreased significantly
conducted to establish deeper understanding on the effect of CO2 with the increase of the gas flow rate. The high gas velocity in the
partial pressure. packed column could possibly entrain the solvents because of
the direct contact between liquid and gas phases and resulted in
4.3. Gas flow rate the decrease of liquid flow rate spreading on the packing surface.

Aroonwilas et al. [32,72,76] observed no significant effect of


gas flow rate in the range of 46–97 kmol m2 h1 (0.29–
0.61 m3 m2 s1) for overall mass transfer coefficient using AMP

Fig. 2. Effect of CO2 partial pressure on the overall mass transfer coefficient for (a)
CO2–NaOH; (b) CO2–AMP [32]. Fig. 4. Effect of gas flow rate on the CO2 absorption [80].

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However, balanced consideration between absorption efficien-


cy and cost involved should be taken when increasing the
concentration of absorbent. Aboudheir et al. [80] experimented
with extra high concentration of MEA solutions and found that as
the MEA concentration was increased from 18 wt% to 30 wt%, the
CO2 removal efficiency increased from about 91% to 96%, with 5% of
enhancement achieved. It was observed that only 2% of enhance-
ment was achieved when MEA concentration was further
increased from 30 wt% to 54 wt% even though at a higher MEA
concentration, the net CO2 absorption per mole of MEA is less. The
authors deduced two reasons for the trend observed. First, the
acid-gas vapor pressure was higher over more concentrated
solutions at equivalent acid-gas/amine mole ratio. Second, the
higher heat of reaction in the more concentrated solution resulted
in a greater increase in temperature. This increase in temperature
would increase the CO2 vapor pressure over the solution.
According to Setameteekul et al. [78], the increasing viscosity of
Fig. 5. Effect of liquid load on the CO2 absorption performance [33]. the solutions from with increase of absorbent concentration also
possibly hindered the ability of the liquid to spread, which offset
the positive effect of increased availability of absorbent molecules.
4.4. Liquid flow rate
4.6. Liquid temperature
In absorption operation, it was well agreed in various studies
that higher solution/liquid flow rate led to higher CO2 removal In general, temperature is an important parameter influencing
efficiency [32,33,62,63,68,72,80,85]. Fig. 5 shows that the CO2 reaction kinetics. For CO2 absorption kinetics, the reaction rate
removal efficiency for 5 different types of amine increased with the constant normally is based on the Arrhenius expression [86]:
increase of liquid load/flow rate. The improvement was especially
obvious for MEA. This increasing trend was because the wetted k ¼ AeEa =RT (2)
surface of the packing material for gas–liquid contact increased
with increase of solution flow rate [68]. Hence, there was an The natural log of the equation results in the following expression:
increase in the effective area for mass transfer process [33,72].
According to Aroonwilas and Tontiwachwuthikul [76], there was Ea 1
also higher liquid-side mass transfer coefficient and higher lnðkÞ ¼ lnðAÞ  (3)
R T
availability of absorbent molecules reacting with CO2 per unit
time with increase of liquid flow rate. This indicates that the reaction rate constant is temperature
However, it should be noted that during operation at industrial dependence and increasing temperature leads to a greater reaction
stage, higher steam flow rate would be needed to regenerate the rate constant, k. It was confirmed in several studies that higher
higher flow rate solvent. Otherwise, there would be higher CO2 temperature contributed to higher mass transfer efficiency [49,51].
loading in the regenerated lean solvent and it would subsequently However, Aroonwilas et al. [72,85] observed that too high of a
lower the absorption performance as observed by Arashi et al. [68] temperature induced efficiency deterioration. Fig. 7 shows that
in Fig. 6. when the temperature of MEA was increased from 25 to 36 8C, the
mass transfer coefficient increased. Nevertheless, when the
4.5. Absorbent concentration temperature was further increased to 45 8C, the removal efficiency
dropped. This was due to the thermodynamics of the exothermic
An increase in absorbent concentration generally leads to an CO2 absorption system which could cause reversible reactions
increase in mass transfer coefficient [32,62,72,78]. This was due to when the temperature was too high. The increase in temperature
higher amounts of solvent molecules per unit volume available for could also increase the CO2 vapor pressure over the solution which
absorbing more CO2 at the gas–liquid interface and it increased the leads to decrease of the physical solubility of CO2 in solvent [30,80].
chance for CO2 to contact and react with the active absorbent. Hence, there is a need to strike a balance between physical

Fig. 6. Relationship between solution flow rate (L/h) to (a) CO2 removal; (b) CO2 loading in lean solution at constant steam flow rate of 250 kg/h (for stripping process) [68].

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Table 6
Properties of structured and random packing.

Type of Name of packing Surface Void Ref.


packing area fraction
(m2/m3) (%)

Structured Flexipac 1Y 453 91 [87]


Flexipac 2Y 223 95 [88]
Flexipac 3Y 115 96 [88]
Gempak 1A 115 95 [88]
Gempak 2A 223 96 [88]
Gempak 4A 446 92 [89]
Mellapak 500Y 500 91 [89]
Mellapak 500X 500 91 [89]
Mellapak 350Y 351 95 [90]
Mellapak 250Y 250 95 [91]
Mellapak 250X 250 95 [91]
Sulzer-BX 492 90 [91]
Sulzer-DX 900 78 [92]
Sulzer-EX 1710 86 [93]
Fig. 7. The overall mass transfer coefficient in CO2–MEA system at various liquid Optiflow 210 98 [85]
temperature [85]. Montz-Pak B1-200 200 98 [94]
Montz-Pak B1-250 245 98 [88]
solubility and reaction kinetics while increasing temperature to Montz-Pak B2-300 300 93 [94]
enhance the absorption efficiency. Random 1 in. Pall Rings 205 94 [91]
1.5 in. Pall Rings 130 95 [91]
4.7. CO2 loading of solvent 2 in. Pall Rings 115 96 [91]
Raschig Super-Rings 0.5 236 96 [95]
Raschig Super-Rings 0.7 176 97 [95]
Increase of CO2 loading in solvent reflected lower available active Raschig Super-Rings 1 156 98 [95]
absorbent concentration in the solution and this condition could IMTP #25 230 97 [91]
significantly reduce the mass transfer coefficient for 30 wt% MEA IMTP #40 154 97 [91]
and ammonia as depicted in Fig. 8 [30]. It is noted that the operating IMTP #50 98 98 [91]
1 in. Intalox Saddles 256 72 [32,96]
temperature of ammonia is much lower than MEA since ammonia is
1.5 in. Intalox Saddles 194 73 [32,96]
highly volatile and the low temperature is necessary to prevent 2 in. Intalox Saddles 118 75 [32,96]
ammonia slip (as explained in Table 3). Arashi et al. [68] observed 1 in. Raschig Rings 190 68 [94]
that when CO2 loading in the lean solution was high, the driving 1.5 in. Raschig Rings 121 72 [32,96]
2 in. Raschig Rings 95 83 [94]
force of mass transfer from gas to solution became small and the
1 in. Berl Saddles 250 68 [91]
decrease in CO2 removal efficiency could not be compensated even 1.5 in. Berl Saddles 150 71 [91]
with the increase of solution flow rate. The strong influence of CO2 2 in. Berl Saddles 105 72 [91]
loading to the mass transfer coefficient was also discovered by
Setameteekul et al. [78]. Among the process parameter of
alkanolamine concentration, CO2 partial pressure in feed gas, mass-transfer coefficient than random packing [72,79,80]. Aroon-
temperature, CO2 loading of solvent and liquid circulating rate, wilas et al. [72] found that Gempak 4A provides almost two fold
the authors observed that CO2 loading of the solution was the most mass-transfer performance (KGav) superior to #25 and 1 in. Pall
influential process parameter on overall mass-transfer coefficient. Rings. This was perhaps due to a considerably higher geometric
surface area per unit volume of the structured packing in
4.8. Packing comparison with those of random packings as indicated in Table
6. A study conducted by Marcia et al. [97] indicated that structured
Packing is instrumental in creating longer gas–liquid contact packing provided more evenly distributed flow of solution
time during CO2 absorption process. Table 6 lists the properties of throughout the column packing compared to the Pall Rings
commercial packing. random packing.
In recent years, there are increasing findings that structured Generally, the volumetric mass transfer coefficient increased
packing in an absorber can provide a much higher overall with increase of surface area [98]. However, surface area of packing
should not be the only judging criteria for higher mass transfer
coefficient estimation as there are also other influencing factors
such as pattern of packing arrangement, corrugation angle and
crimp height in the case for structured packing [89]. According to
Aroonwilas et al. [85], for arrangements of successive packing
elements, the 908 and 458 rotation around the column axis
provided better efficiency compared to 08 rotation.
Meanwhile, higher void fraction generally indicates lower
pressure drop. Nevertheless, liquid holdup could cause reduction
of void space in small-size packing. Hence, careful consideration on
shape and size of packing should be taken into account as larger-
size packing could minimize the liquid entrainment capacity [96].

5. Major challenges and future prospects

Fig. 8. Overall mass transfer co-efficient for CO2 absorption with aqueous ammonia Although MEA is an effective and popular solvent, strong bonds
and 30% (w/w) MEA solvents as a function of CO2 loading [30]. are created between the solvent and CO2 and the breaking of these

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8 L.S. Tan et al. / Journal of Industrial and Engineering Chemistry xxx (2012) xxx–xxx

Fig. 9. (a) Woven carbon fibers which were braided into tubes; (b) the final structure after the tubes were fitted together [106].

bonds requires large amounts of energy [31]. Alternative solvents need to be done to confirm the efficiency when it is scaled up, but
which could overcome the problem are being sought after. these innovative structures could pave way for new generation of
Ultimately, improvement in the performance of current amine- packing evolution.
based system and reduction in energy penalty can reduce the There are efforts on enhancing mass transfer rate between gas
future cost of CO2 capture [99]. Ideally, the newly developed and liquid via rotating packed bed (RPB) in which liquid and gas are
solvent should have high reactivity, low vapor pressure in order to contacted in the presence of a high centrifugal field. Lin et al. [109]
reduce the loss of solvent in desorption, low degradation with time, found that the CO2 removal efficiency in a rotating packed bed was
low-cost and as harmless as possible [27,31]. In recent years, new comparable to packed tower while Tan and Chen [110] observed
chemical absorbents such as sterically hindered amines are being more effective mass transfer in RPB than that in a packed tower.
examined since the bonding between the solvent and CO2 is Although usage of RPB could provide saving in size and space
weaker and subsequently, the recovery energy could be reduced [49,111,112], further study needs to be conducted in order to
[7]. overcome the mechanical maintenance issue if it were to be
Eimer identified three alternative solvents which have about applied commercially. Recently, there are emerging studies on
30% lower energy consumption and significantly lower degrada- using spray column for CO2 removal and it was observed to be
tion rates compared to MEA i.e. Mitsubishi’s KS-1, Universiti of capable of removing CO2 from gas streams at a higher rate than the
Regina’s PSR and Praxair’s solvent [26]. KS-1 is already imple- packed column due to greater interfacial area provided [113,114].
mented commercially at a fertilizer plant in Malaysia [7,27] while Besides, there is opportunity for alternative form of CCS
PRS and Praxair’s solvent is still in testing stage but they could soon whereby CO2 is captured in solid formation after reacting with
be available commercially [26]. KS-1 solvent is also not a corrosive solvent [115,116]. Currently, the strategy for CO2 storage is to have
substance in contrast to MEA. Hence, it does not require a corrosion the CO2 dispersed in pores in a geological formation, eventually
inhibitor [14,100]. Meanwhile, integrated projects supported by dissolved in formation water and reacted with rocks. However,
European Commission have so far developed several versions of there is a need for suitable selection of storage location, injection
new solvent such as CASTOR1, CASTOR2, CESAR1 and CESAR2 system design and monitoring during and after injection process
[101,102]. The pilot plant study on the solvents indicated that [117,118]. CO2 could be captured in bicarbonate salts form using
CESAR1 could provide reduction of about 20% in the regeneration amino acids and it is optional to degas it outside the column [116].
energy and 45% in the solvent flow rate compared to MEA [103]. CO2 could also be captured in the form of calcium carbonate after
CASTOR2 also showed significantly lower energy requirement than reaction with aqueous MEA containing calcium nitrate while stable
MEA [104]. While various researches are intensively conducted to salts formation could be produced from reaction between CO2 and
produce new solvents with low regeneration heat duty, it should ammonia which could be used commercially as fertilizers [55,119–
be noted that the sensible heat needed to raise the solvent from 121]. This kind of solvent would require a different post-
absorber to desorber temperature and the heat of evaporation absorption process strategy such as filtration and sedimentation
required to produce the stripping steam in the reboiler should also instead of the conventional stripping process. Nevertheless, this
be taken into consideration on top of the heat necessary to desorb alternative form of CO2 storage, i.e. chemically bonded, offers a
the CO2 from the solution (heat of absorption) [83,105]. great potential for bulk CO2 storage as opposed to the current deep
Cost-effective and energy-efficient process is also important in sea sequestration option which requires substantial cost for the
order to reduce the cost of CO2 capture. Hence, the development of implementation [24,122]. In addition to that, direct injection of
novel generation of column internals which can provide enhanced CO2 into the mid-water oceanic column requires consideration for
mass transfer performance and relatively low pressure drop is an the environmental impacts such as lowered pH of the exposed
area of study which is worth exploring. Recently, there are waters and associated ecological impact [123]. This kind of post-
emerging researches on development of novel packing. A novel absorption strategy could also be considered for offshore applica-
structured packing which had high effective area, low density, tion whereby regeneration process is not a feasible option due to
significant structural cohesion and provided low pressure drop limited space and unavailability of huge heating utility system.
was developed using the corrosion-resistant and inert carbon
fibres (Fig. 9) [106]. There was also development of ‘honeycomb’ 6. Conclusion
and straight strips of packing manufactured from porous PVC
which could increase the volumetric mass-transfer coefficient for With the increase of weather-related catastrophes occurring, it
extremely low liquid flow rate [107,108]. Tremendous studies still is of utmost importance to consolidate all the available resources

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