Process intensiﬁcation for post-combustion CO 2capture with chemical [628926]

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Process intensiﬁcation for post-combustion CO 2capture with chemical [628926]

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Review
Process intensiﬁcation for post-combustion CO 2capture with chemical
absorption: A critical review
Meihong Wanga,⇑, Atuman S. Joela, Colin Ramshawa, Dag Eimerb, Nuhu M. Musaa
aProcess/Energy Systems Engineering Group, School of Engineering, University of Hull, HU6 7RX, UK
bTelemark Technological Research and Development Centre (Tel-Tek), Norway
highlights
/C15Assessment of main barriers for deploying post-combustion CO 2capture (PCC) process.
/C15Evaluation of different process intensiﬁcation technologies for use in PCC process.
/C15Rotating packed bed attracted great interest due to high mass transfer capability.
/C15Process ﬂow diagram for intensiﬁed carbon capture using solvents process proposed.
/C15Preliminary technical and economic analysis for the intensiﬁed capture process.
article info
Article history:
Received 12 September 2014
Received in revised form 15 July 2015
Accepted 17 August 2015Available online 29 August 2015
Keywords:
Post-combustion CO
2capture
Chemical absorptionRotating packed bed (RPB)Process intensiﬁcation (PI)SolventsIntensiﬁed heat exchangerabstract
The concentration of CO 2in the atmosphere is increasing rapidly. CO 2emissions may have an impact on
global climate change. Effective CO 2emission abatement strategies such as carbon capture and storage
(CCS) are required to combat this trend. Compared with pre-combustion carbon capture and oxy-fuel
carbon capture approaches, post-combustion CO 2capture (PCC) using solvent process is one of the most
mature carbon capture technologies. There are two main barriers for the PCC process using solvent to becommercially deployed: (a) high capital cost; (b) high thermal efﬁciency penalty due to solvent regener-
ation. Applying process intensiﬁcation (PI) technology into PCC with solvent process has the potential to
signiﬁcantly reduce capital costs compared with conventional technology using packed columns. Thispaper intends to evaluate different PI technologies for their suitability in PCC process. The study shows
that rotating packed bed (RPB) absorber/stripper has attracted much interest due to its high mass transfer
capability. Currently experimental studies on CO
2capture using RPB are based on standalone absorber or
stripper. Therefore a schematic process ﬂow diagram of intensiﬁed PCC process is proposed so as to moti-vate other researches for possible optimal design, operation and control. To intensify heat transfer in
reboiler, spinning disc technology is recommended. To replace cross heat exchanger in conventional
PCC (with packed column) process, printed circuit heat exchanger will be preferred. Solvent selectionfor conventional PCC process has been studied extensively. However, it needs more studies for solvent
selection in intensiﬁed PCC process. The authors also predicted research challenges in intensiﬁed PCC
process and potential new breakthrough from different aspects.
/C2112015 Elsevier Ltd. All rights reserved.
Contents
1. Introduction . . . ………………………………………………………………………………………… 2 7 6
1.1. CO
2emissions and climate change. . . . . . . . . ………………………………………………………………. 2 7 6
1.2. CCS technologies . . . . . . . …………………………………………………………………………….. 2 7 6
1.3. Different technical options in the context of PCC . . . . . . . . . . . . . . . . ……………………………………………… 2 7 7
1.4. Current status of PCC using solvent and its commercial deployment ……………………………………………… 2 7 7
1.5. Motivation for using PI in PCC with solvents process. . . . . . . . . . . . . ……………………………………………… 2 8 0
http://dx.doi.org/10.1016/j.apenergy.2015.08.083
0306-2619/ /C2112015 Elsevier Ltd. All rights reserved.⇑Corresponding author. Tel.: +44 01482 466688; fax: +44 01482 466664.
E-mail address: Meihong.Wang@hull.ac.uk (M. Wang).Applied Energy 158 (2015) 275–291
Contents lists available at ScienceDirect
Applied Energy
journal homepage: www.elsevi er.com/locat e/apenergy

1.6. Introduction to PI and evaluation of different PI technologies for PCC . . . . . . . . . . . . ………………………………….. 2 8 0
1.7. Aim and novelty of the paper. . . . . . . . . . …………………………………………………………………. 2 8 1
2. RPB absorber: Current status of experimental rigs and experimental studies . . …………………………………………… 2 8 1
2.1. RPB absorber experimental rigs . . . . . . . . …………………………………………………………………. 2 8 1
2.1.1. Newcastle University in the UK. . . . . . . . . . . . ……………………………………………………….. 2 8 1
2.1.2. BUCT in China. . . . . . . . . . ……………………………………………………………………… 2 8 1
2.1.3. Taiwan (National Tsing Hua University, Chang Gung University and Chung Yuan University) ……………………… 2 8 1
2.1.4. India . . . . . . . . . . . . . . . . . ……………………………………………………………………… 2 8 1
2.2. Experimental studies on intensified absorber . . . . . . . . . . . . . …………………………………………………… 2 8 2
3. RPB stripper: Current status of experimental rigs and experimental studies. . . …………………………………………… 2 8 2
3.1. RPB stripper experimental rigs. . . . . . . . . …………………………………………………………………. 2 8 2
3.1.1. Newcastle University, UK. ……………………………………………………………………… 2 8 2
3.1.2. Taiwan. . . . . . . . . . . . . . . . ……………………………………………………………………… 2 8 2
3.2. Experimental studies on intensified regenerator. . . . . . . . . . . …………………………………………………… 2 8 3
4. Intensified heat exchanger. . . . . …………………………………………………………………………….. 2 8 3
4.1. Technologies available to choose . . . . . . . …………………………………………………………………. 2 8 3
4.1.1. Printed Circuit Heat Exchanger (PCHE) . . . . . . ……………………………………………………….. 2 8 3
4.1.2. Formed Plate Heat Exchanger (FPHE) . . . . . . . ……………………………………………………….. 2 8 3
4.1.3. Hybrid Heat Exchanger (H2X )…………………………………………………………………… 2 8 3
4.1.4. The Marbond heat exchanger . . . . . . . . . . . . . ……………………………………………………….. 2 8 3
4.1.5. Spiral heat exchanger (SHE). . . . . . . . . . . . . . . ……………………………………………………….. 2 8 3
4.2. Recommendation for intensified Heat Exchanger for PCC application. . . . . . . . . . . . . ………………………………….. 2 8 4
5. Solvents used for intensified PCC process. . . . . . . . . . . . ……………………………………………………………. 2 8 4
5.1. Factors to consider . . . . . . . . . . . . . . . . . . …………………………………………………………………. 2 8 4
5.2. Solvents used. . . . ………………………………………………………………………………….. 2 8 4
5.2.1. Alkanolamine . . . . . . . . . . ……………………………………………………………………… 2 8 4
5.2.2. NaOH. . . . . . . . . . . . . . . . . ……………………………………………………………………… 2 8 5
5.2.3. Ionic liquid (1-n-butyl-3-methyllimidazolium hexafluorophosphate) ………………………………………. 2 8 5
5.2.4. Potassium Carbonate (K 2CO3) …………………………………………………………………… 2 8 5
5.2.5. Benfield solution (Amine-promoted hot K 2CO3solution). . . . . . . . . . . ………………………………………. 2 8 5
5.2.6. Piperazine (PZ) . . . . . . . . . ……………………………………………………………………… 2 8 5
5.3. Proprietary commercial solvents . . . . . . . …………………………………………………………………. 2 8 5
5.4. Recommendations on solvent selection for PCC process . . . . …………………………………………………… 2 8 5
6. Modelling/simulation for CO 2capture process using RPB . . . . . . . . . . . . . . . . . . …………………………………………… 2 8 6
6.1. Correlations for mass/heat transfer . . . . . …………………………………………………………………. 2 8 6
6.2. Modelling/simulation of intensified absorber . . . . . . . . . . . . . …………………………………………………… 2 8 6
6.3. Modelling/simulation of intensified stripper . . . . . . . . . . . . . . …………………………………………………… 2 8 6
6.4. Modelling and simulation of the whole plant . . . . . . . . . . . . . …………………………………………………… 2 8 6
7. Prospective of applying PI technology into PCC using solvents. . . . . . . . . . . . . . …………………………………………… 2 8 6
7.1. Fundamental study regarding Marangoni effect and enhanced mass transfer . . . . . . ………………………………….. 2 8 7
7.2. Proposed schematic PFD for whole intensified PCC process. . …………………………………………………… 2 8 7
7.3. Experimental rigs and experimental studies . . . . . . . . . . . . . . …………………………………………………… 2 8 7
7.4. Selection of solvents . . . . . . . . . . . . . . . . . …………………………………………………………………. 2 8 7
7.5. Modelling and simulation of intensified CO 2capture process …………………………………………………… 2 8 7
7.6. Scale-up . . . . . . . . ………………………………………………………………………………….. 2 8 7
7.7. Evaluation of technical, economical and environmental performance. . . . . . . . . . . . . ………………………………….. 2 8 7
8. Conclusions. …………………………………………………………………………………………… 2 8 8
Acknowledgements . . . . . . . . . . …………………………………………………………………………….. 2 8 8
References . …………………………………………………………………………………………… 2 8 8
1. Introduction
1.1. CO 2emissions and climate change
Global energy demand is expected to continue to rise due to the
increasing world population, in addition to economic development
of nations such as Brazil, Russia India and China. Dependence on
renewable energy alone such as solar, wind and tidal power to
meet the projected demand is not feasible due to their intermittent
nature. Therefore, fossil fuel remains the very attractive options in
meeting future energy demands. But power generation using fossil
fuel is estimated to be the largest source of worldwide carbon
emissions [1].
Combustion of fossil fuels (e.g. petroleum, coal and natural gas)
accounts for the majority of CO 2emissions. Globally most fossil-
fuelled electricity production is from coal (63%), followed by natu-
ral gas (29%) and oil (9%) [2]. For instance about 85.5% of its coal(produced and imported) is used for electricity generation in the
UK in 2011 [3]. Albo et al. [4]stated that among the greenhouse
gases, CO 2contributes to more than 60% of global warming. Statis-
tics from World Metrological Organisation (WMO) showed that the
amount of CO 2in the atmosphere reached 393.1 ppm in 2012. The
WMO report also showed that the amount of CO 2in the atmo-
sphere has increased on average by 2 ppm per year for the past
10 years, this increased atmospheric concentration of CO 2affects
the radiative balance of the Earth [5].
1.2. CCS technologies
Intergovernmental panel on climate change (IPCC) [6]has set
ambitious goal to reduce CO 2emission by 50% in 2050 as compared
to the level of 1990 so as to overcome the foreseen environmental
challenges. In order to achieve the required emission reductions in
the most cost-effective manner, carbon capture and storage (CCS)276 M. Wang et al. / Applied Energy 158 (2015) 275–291

will need to contribute around one-ﬁfth of total reductions in
emissions by 2050 [7].
CCS consists of three basic stages: (a) separation of CO 2; (b) CO 2
transportation and (c) CO 2storage. There are three major
approaches for CCS: post-combustion capture, pre-combustion
capture and oxy-fuel process [8].
1.3. Different technical options in the context of PCC
PCC technologies are at various stages of development. Aba-
nades et al. [9]reviewed the technological readiness level for dif-
ferent CO 2capture technologies in the context of PCC including
chemical looping, calcium looping, PCC using solvent, PCC using
adsorbent and PCC using membrane. The most matured process
is PCC using solvent [9,10] .
However, the PCC using solvent process has several drawbacks
including: (1) low CO 2loading capacity; (2) high equipment corro-
sion rate; (3) amine degradation by SO 2,N O 2, and O 2in the ﬂue
gases which induces a high solvent makeup rate; (4) high energy
consumption during solvent regeneration; (5) large equipment size
[11–14] (in whole PCC process, absorber and stripper account for
55% and 17% of the total capital cost respectively [15]). This process
is introduced in more detail in Section 1.4andTable 1 gives its per-
formance indicators and status for chemical absorption compared
to adsorption and membrane technologies.
Chemically modiﬁed adsorbents have proved to be applicable
for PCC process because of large CO 2adsorption capacity, high
adsorption and desorption rates, high tolerance to moisture, and
high selectivity towards CO 2over other gases [24]. In terms of
regeneration energy, Zhao et al. [25] reported that solid sorbent
does not have any obvious advantage over the matured MEA pro-
cess in terms of energy consumption in the ﬁrst design (i.e. two
reactor used, one for adsorption and the other for regeneration).
But the novel (second) design (i.e. using three reactors, one for
adsorption, one for regeneration and another one for formationof K
2CO3.1.5H 2O), the regeneration energy can be reduced by uti-
lizing the waste heat from the process, however this design is dif-
ﬁcult to control because the reactors operate at different pressures.
A lot of researchers have focused on new adsorbent development,
process optimization, and equipment innovation [26–50] .
Abanades et al. [9]shows that membrane process for PCC is at
almost the same level of technological readiness as adsorption.
Therefore, more study in this area is needed in order to get detailed
technical performance at large scale condition. Many researchers
have developed new membranes that offer better performance in
term of selectivity. The recent key projects developing membranes
and modules for CO 2capture include Membrane Technology and
Research (MTR) in the USA, NanoGLOWA in Germany, the carbon
capture project (CCP) and the CO2CRC in Australia [9]. Membranes
process for PCC is beneﬁcial because of relatively small footprint,
no phase change, simple mechanical system, steady-state operat-
ing conditions (usually), easy scale-up and ﬂexibility [51–53] .The major challenge for membranes comes from the potential foul-
ing of the membrane surfaces from particulate matter, uncertainty
about the performance and cost of large-scale efﬁcient vacuum
pumps and compressors required for PCC, and the ability to inte-
grate the process into a power plant. Technological outlook of
membrane system is reported in Abanades et al. [9]and high-
lighted that for the technology to be competitive with other PCC
technology, the membrane needs to be of high CO 2permeance
(around 1000 gas permeance units (GPU)) to be economical.
The technological readiness (maturity) level of PCC based on
chemical absorption and the ﬁrst commercial deployment of PCC
using solvents plant in 2014 motivate the authors to write this
paper and highlight the process design option that will improve
the chemical absorption PCC process using the RPB technology.
1.4. Current status of PCC using solvent and its commercial
deployment
Fig. 1 shows a simpliﬁed PCC process. Flue gas from CO 2sources
such as power plant is contacted counter-currently with lean sol-vent solution in the absorber. Solvent chemically absorbs CO
2in
the ﬂue gas. This leaves a treated gas stream of lower CO 2content.
The solvent solution (now rich solvent) is regenerated in the strip-
per. CO 2from the top of the stripper is compressed and transported
while the lean (regenerated) solvent solution is returned to the
absorber column passing through a cross exchanger to recover heat
with rich solvent from the absorber.
Studies on PCC with chemical absorption process were reported
mainly for fossil fuel-ﬁred power plants. Dugas [55] carried out
Table 1
Status of post-combustion CO 2capture development [15–23] .
Absorbent Adsorbent Membrane
Commercial usage in chemical process
industriesHigh Moderate Low/Niche
Operational conﬁdence High High, but complex Low to moderate
Primary source of energy penalty Solvent Regeneration
(thermal)Solid sorbent Regeneration
(thermal/vacuum)Compression on feed and/or vacuum on
permeate
Regeneration energy (MJ/kg-CO 2) 2.2–6 0.5–3.12 0.5–6
Efﬁciency penalty (%) 8.2–14 5.4–9.0 6.4–8.5Development trends New solvent, thermal
integrationNew sorbent, process conﬁguration New membrane, process conﬁguration
Fig. 1. Simpliﬁed process ﬂow diagram of chemical absorption process for post
combustion carbon capture [54].M. Wang et al. / Applied Energy 158 (2015) 275–291 277

Table 2
Summary of different PI technologies.
PI equipment Description Mechanism for
intensiﬁcationArea of application
at presentSuitability to
CO2captureLimitation
Static mixer A static mixer or motionless mixer is a
device inserted into a housing orpipeline with the objective ofmanipulating ﬂuid streams. Differentdesigns are available, typicallyconsisting of plates or bafﬂes positionedin precise angles in order to direct ﬂow,
increase turbulence and achieve mixing
and reactions [90].
Static mixer functions to
divide, recombine,accelerate/decelerate,spread, swirl or formlayers of ﬂuid streams asthey pass through themixer. mixture
components are brought
into intimate contactthereby enhancingreaction processes [90]Mostly this equipment is
used for liquid system. e.g.Waste water treatmentprocess (Formosetreatment) [91]Because of its high mass
transfer capability, thiscan be used for CO
2
capture by combining theﬂue gas stream and thesolvent streamThe challenge would be
the high volume of ﬂue gasto be treated (For example,500 MWe coal-ﬁred powerplant releases 8,000tonnes/day of pure CO
2)
At the exit, a ﬂash drum
can be used to separate
the treated gas and therich solvent
Spinning disc Spinning disc reactor consists of a
cylindrical housing with a rotating discin the middle between the top andbottom plates of the cylinder, therotating disc is connected to a motor
[92–94]
Gas and liquid are fed
together through the inletin the centre of the topstator, close to the rotatingaxis. A liquid ﬁlm is
present on top of the rotor,
and a gas–liquid bubblydispersion is locatedbetween the rotor and thebottom stator. Thecombined ﬁlm ﬂow on therotor and the dispersed
ﬂow in the remainder part
of rotor–stator reactorlead to higher gas–liquidmass transfer rate [92]It is used for gas–liquid
and liquid–solid masstransfer process such asdesorption of oxygen fromoxygen saturated water,
polymerization,
crystallization [92–97]It has the potential for CO
2
absorption, either as an
absorber because of itshigh mass transfercapability or as a stripper
because of its high heat
transfer ability. It can alsobe used as a reboilerIt may result in additional
unit such as ﬂash drum toseparate the rich solventfrom treated gas streamsince the ﬂow is co-
current
Mop fan Mop fan is a device that uses ﬂexible
ﬁbre needle impeller instead of bladeimpeller within a centrifugal fan casing.The ﬂexible ﬁbre needle impeller is
connected to a motor [98]
Dirty air enters the mop
through its centrecontacting the solventwhich is sprayed on the
ﬁbre needle impeller. The
rotating mop leads toincrease in interfacial areafor captureMop fan is used for
removal of air-borneparticulates [99]The system uses a ﬂexible
ﬁbre needle impeller (mopfan) device to increase theheat and mass transfer in
the absorber for CO
2
capture [98–100]Huge volume of ﬂue gas to
be treated from powerplants means there needsto be many mop fans for
CO
2capture. It may also
result in additional unitsuch as ﬂash drum toseparate the rich solventfrom treated gas streamsince the ﬂow might beco-current
Loop reactor Advanced BUSS Loop
/C210reactor is made
up of a reaction vessel, a circulationpump, a heat exchanger with a highperformance gas/liquid ejector toachieve high mass transfer rates [101] .
A gas–liquid ejector
consists of four mainsections. Optional swirldevice, nozzle thatprovides a high velocity jet
of ﬂuid to create suction of
the gas in the gas suctionchamber and entrain gasinto the ejector. Liquid jetattaches itself to themixing tube wall resultingin a rapid dissipation ofkinetic energy. This
creates an intensive
mixing where the highturbulence produces a ﬁnedispersion of bubbles[101]Loop reactor is used for
hydrogenation,phosgenation, alkylation,amination, carbonylation,oxidation and other gas–
liquid reactions [101,102]Because of high mass
transfer and heat transferit may be applicable toCO
2capture [101–103]Design modiﬁcation will
be required for it to be usefor CO
2capture also huge
volume of ﬂue gas thatwill be treated is another
challenge278 M. Wang et al. / Applied Energy 158 (2015) 275–291

Table 2 (continued )
PI equipment Description Mechanism for
intensiﬁcationArea of application
at presentSuitability to
CO2captureLimitation
Microreactor Schematic representation of a 2nd
generation microreactor based on a platedesign for performing mixing, gainingvolume (e.g. to increase residence time)and integrating heat exchange [104] .
There are many designs
for Microreactor, but theplate design offers anadvantage of good mixing,longer residence time andbetter temperature controlusing cooling or heating
plate [104] . Two ﬂuid
streams ﬂow co-currentlyinto the reactor wherethere are static mixersinside the reactor toenhance mixing before theﬁnal product comes outThe technology is mostly
applied to ﬁne chemicaland pharmaceuticalindustries for productionof specialized drugs andhazardous chemicals[104–106]Because of high mass
transfer and heat transfer,and its ability to operate atcontrolled temperature, ithas good potential for CO
2
capture [105,106]The expected challenge of
using this technology forcarbon capture is the hugevolume of ﬂue gas to betreated
Chamber’s
centrifugal
absorberThis centrifugal absorber was
introduced by Chambers and Wall in
1954. The lower plate is rotating whilethe upper plate is static. Mass transferoccurs in the intermesh of concentricrings as the lean solvent contact the ﬂuegas. No packing was utilized [107] .
The rotation of the lower
plate makes the liquid
coming into the chamberto splash as it is thrownout while the ﬂue gascontact the liquid counter-currently leading to masstransfer in the concentricregions of the abzsorber
[107]It is used for CO
2capture
as reported by Chambers
and Wall [107]With more modiﬁcations
in design (to incorporate
packing in its bed so as toincrease surface area ofcontact) and constructionmaterial (e.g. corrosionresistance materials), itcan be used for CO
2
captureMaximum CO 2recovery
was reported to be 85%,
this is below the standardfor CO
2capture above 90%
Podlbieiniak’s
deodorizerThe contactor is basically a cylindrical
rotor mounted on a shaft withcontacting material [108] .
Gas and liquid meet
counter-currently with thehelp of contacting materialas the contactor rotates[108]Used for stripping out
odour and ﬂavoursubstances fromtriglyceride oil usingsteam [108]Has the potential for CO
2
capture especially as
stripperDesign modiﬁcation will
be needed when using itfor CO
2capture
Rotating
Zigzag bedThe RZB is characterised by a rotor
coaxially combining a rotating disc witha stationary disc [109–111] .
In the interior of rotor, the
gas ﬂows along a zigzagpath and the liquidexperiences repeateddispersion andagglomeration. There aretwo types of gas–liquid
contact. The ﬁrst step is
cross-current contact oftwo phases when theliquid is thrown by therotational bafﬂes. Thesecond step is counter-current contact of two
phases when the liquid
falls down along thestationary bafﬂes[109,110]RZB can function without
liquid distributors,eliminate one dynamic-seal, and easilyaccommodate andaccomplish intermediatefeeds in continuous
distillation processes
[109–111]It has the potential for CO
2
absorption because of its
high mass transfercapability [109–111]No known limitation to
CO
2capture
Rotating
Packed BedThe HiGee machine was constructed
using a doughnut-shaped rotor, which ismounted on a shaft, and ﬁlled with highspeciﬁc area packing [85]
This technology takes
advantage of centrifugalﬁelds as stimulants forprocess intensiﬁcation.
Increasing the centrifugal
acceleration improves theslip velocity, which in turnimproves the ﬂoodingcharacteristics andinterfacial shear stress,and consequently booststhe mass transfer
coefﬁcient [85]Many studies such as
Jassim et al. [85], Joel et al.
[87,89] , Cheng and Tan
[112] , Cheng et al. [113] ,
Cheng and Tan [114]
showed its application toCO
2capture was success-
fulRPB has the potential for
CO2capture [85,87–
89,112,114–118]No known limitation to
CO2captureM. Wang et al. / Applied Energy 158 (2015) 275–291 279

pilot plant experimental studies of PCC in the context of fossil fuel-
ﬁred power plants. Mangalapally et al. [56–59] reported pilot plant
studies of PCC for gas ﬁred power plant. Lawal et al. [11,60–62] ,
Biliyok et al. [63], Kvamsdal et al. [54,64–66] , MacDowell and Shah
[67–69] , MacDowell et al. [70], Lucquiaud et al. [71,72] , Errey et al.
[73], Agbonghae et al. [14,74] carried out steady state and dynamic
modelling of CO 2absorption for PCC using solvents for fossil-fuel
ﬁred power plants. Asendrych et al. [75], Sebastia-Saez et al. [76],
Raynal et al. [77], Raynal and Royon-Lebeaud [78] studied PCC
for fossil fuel ﬁred power plant using CFD.
There is also good progress in commercial deployment of PCC
using solvent technology. SaskPower’s Boundary Dam Integrated
Carbon Capture and Storage (ICCS) Demonstration Project (that
comes online on 2nd October, 2014) captures over one millionmetric tons of CO
2per year, reﬂecting a 90% CO 2capture rate for
the 139 MWe coal-ﬁred unit. This is the ﬁrst commercial CCS plant
in the world [79],
The demonstration plant of Southern Company’s 25 MWe Plant
Barry CCS project in Alabama, USA using Mitsubishi Heavy Indus-
tries (MHI) technology has been operational since June 2011 and
it reached full-scale capture of 500 tonnes a day in September
2012 [80].
Petra Nova/NRG 240 MWe W.A. Parish project using the MHI
technology is the largest commercial PCC using solvent project in
the world. It is located in southwest of Houston, Texas, USA. It is
installed on an existing coal-ﬁred power plant and is expected to
be operational in 2016 [81]. The plant is expected to capture
1.6 million tons of CO 2annually for use in enhanced production
at mature oil ﬁelds in the Gulf Coast region [81].
However, there are two main barriers for the PCC using solvent
process to be commercially deployed: (a) huge capital cost;(b) high thermal efﬁciency penalty due to solvent regeneration.
Therefore it is necessary to improve the technologies that can
reduce various costs in PCC.
1.5. Motivation for using PI in PCC with solvents process
It was reported that a 500 MWe supercritical coal ﬁred power
plant operating at 46% efﬁciency (LHV basis) releases over8000 tonnes of CO
2per day [82]. PCC using solvents based on the
conventional technology (i.e. using packed columns) requires very
large packed columns. Dynamic modelling and simulation study of
a 500 MWe sub-critical coal-ﬁred power plant by Lawal et al. [11]
showed that two absorbers of 17 m in packing height and 9 m in
diameter will be needed to separate CO 2from the ﬂue gas. These
huge packed columns translate into high capital costs. A signiﬁcant
amount of steam from power plants has to be used for solvent
regeneration. This translates into high thermal efﬁciency penalty.
It is reported that 3.2–4.5 MJ energy is required to capture per kg
of CO 2using MEA solvent [11,54,68,83,84] . Technical approaches
such as heat integration, inter-cooling among others can reduce
the operating cost slightly. However, they limit the plant ﬂexibility
and will make operation and control more difﬁcult [54]. On the
other hand, PI has potentials of signiﬁcant capital cost reduction
[85–89] , and also to improve process dynamics.
1.6. Introduction to PI and evaluation of different PI technologies for
PCC
According to Reay [86], process intensiﬁcation (PI) can be
deﬁned as: ‘‘Any engineering development that leads to a substan-
tially smaller, cleaner, safer and more energy efﬁcient technology. ”
There are general approaches to PI with the aim to improve process
performance [86]: (a) Reducing equipment size using an intensi-
ﬁed ﬁeld (e.g. centrifugal, electrical, microwave); (b) Simplifyingprocesses by integrating multiple process tasks in a single item
of equipment; (c) Reducing equipment size by reducing its scale
of structure.
PI technologies differ in functions and areas of application.
Some will be very good at intensifying mass transfer, whilst others
are good at intensifying heat transfer. Some typical PI studies are
presented in Table 2 to evaluate the most preferred option for
CO
2capture application.
Out of all the PI technologies studied, RPB proves to be the most
suitable for intensiﬁed PCC process because of its high mass trans-
fer performance. Fig. 2 shows the study done by BRITEST which
indicates that RPB technology gives the best mass transfer capabil-
ity compared to all other mass transfer technologies [119] . Ram-
shaw and Mallinson [120] reported enhancement in mass
transfer when using RPB. Zhang et al. [121] also reported that there
Fig. 2. Mass transfer capacity in various devices [119] .
Micromixing controlled
Nanopar/g415cles Syntheses Fast reac/g415on Polymeriza/g415on
Mass transfer limited
CO2 H2S/CO 2 SO2
Fig. 3. Summary of why PI for PCC [119] .280 M. Wang et al. / Applied Energy 158 (2015) 275–291

is at least one order magnitude improvement in liquid phase mass
transfer when compared to conventional packed bed.
Fig. 3 summarised why PI technology is necessary in capture of
carbon dioxide, ﬁrst because reaction between CO 2and its absor-
bent is a fast reaction which means it is a micromixing controlled
process. Secondly it falls in the category of processes that are mass
transfer limited [85,119] .
1.7. Aim and novelty of the paper
PCC using packed column (i.e. conventional technology) in the
context of power generation may result in increase of the electric-
ity cost by more than 50%. This has led to the need to search for
alternative technologies since heat integration, inter-cooling
among others limit the operational ﬂexibility and make control
of the technology more difﬁcult [54,63,64,66] . PI technology offers
the beneﬁt of signiﬁcantly reducing the size of columns without
compromising its production capacity [120] .
This paper aims to evaluate current status of intensiﬁed PCC
(based on chemical absorption) process regarding experimental
rigs, experimental studies, intensiﬁed heat exchanger, solvent
selection, modelling and simulation and to identify the knowledge
gap that exists in using PI for intensiﬁed PCC process with solvents.
It was found that all of the experimental rigs available in the world
operate as standalone intensiﬁed absorber or standalone intensiﬁed
stripper. Therefore no study on the integrated intensiﬁed PCC pro-
cess was presented in any open literature. New process ﬂow dia-gram (PFD) of the integrated intensiﬁed PCC process is proposed
in Section 7.2of this paper. Preliminary technical and economic
analysis for intensiﬁed PCC process compared with conventional
PCC process is presented in Section 7.7. Other areas that needs
research efforts on use of PI for PCC process are study of Marangoni
effect, systematic experimental studies, selection of suitable sol-
vents, dynamic modelling and simulation, CFD study for scale-up,
optimization, techno-economic analysis and life cycle analysis (LCA).
2. RPB absorber: Current status of experimental rigs and
experimental studies
2.1. RPB absorber experimental rigs
Since Mallinson and Ramshaw [120] introduced RPB in late
1970s, interest has been continuously increasing in the use of
RPB as an absorber for PCC.
2.1.1. Newcastle University in the UK
The group at the School of Chemical Engineering and Advanced
Materials, Newcastle University carried out studies on CO
2absorp-
tion and desorption in aqueous monoethanolamine (MEA) solu-
tions in RPB. CO 2was captured at two solvents ﬂow rates of 0.66
and 0.35 kg/s having different MEA concentrations of 30 wt%,
55 wt%, 75 wt% and 100 wt%. The ﬂue gas is at a ﬂow rate of
2.86 kmol/h [85]. The RPB rig has internal diameter of 0.156 m,
outer diameter 0.398 m and axial height of 0.025 m. Presently
the RPB rig have been changed as reported by Lee et al. [122] ,
the new RPB rig has outer diameter of 1 m, internal diameter of
0.19 m and axial depth of 0.05 m. Newcastle team is also looking
at using different packing types (Expamet and Knitmesh) in the
RPB bed. Expamet in the inner section of the RPB packing while
Knitmesh at the outer section of the packing to reduce or avoid
the problem known as the end effect.
2.1.2. BUCT in China
Counter-current ﬂow RPB was reported by Yi et al. [123] using
Benﬁeld solution (amine-promoted hot potassium carbonate
solution). The experimental rig has the following speciﬁcations:inner and outer radius of the packing 0.040 m and 0.100 m respec-
tively, and axial depth of 0.031 m. Zhang et al. [121] reported RPB
absorber using ionic liquid with the following rig speciﬁcations:
inner diameter of 0.020 m, outer diameter 0.060 m and axial pack-
ing depth of 0.020 m. Luo et al. [124] proposed correlation for gas–
Liquid effective interfacial area in a RPB using NaOH solvent to
absorbed CO 2. Luo et al. [124,125] reported the following rig spec-
iﬁcations: inner and outer radii of the rotor were 0.078 m and
0.153 m respectively, and the axial height of the rotor was
0.050 m. The static casing had an inner radius of 0.248 m and an
axial height of 0.098 m. Zhang et al. [121] found that liquid side
volumetric mass transfer coefﬁcient for RPB has been improved
to around 3.9 /C210/C02s/C01compared with 1.9 /C210/C03s/C01for the con-
ventional packed column under the same operating conditions.
2.1.3. Taiwan (National Tsing Hua University, Chang Gung University
and Chung Yuan University)
The group in National Tsing Hua University in Taiwan studied
CO2capture using counter-current ﬂow arrangement. Yu et al.
[126] studied CO 2capture by alkanolamine solutions containing
diethylenetriamine (DETA) and piperazine (PZ) in an RPB. Cheng
and Tan [114] studied removal of CO 2from indoor air by alka-
nolamine in RPB, the experimental rig used is the same as for Tan
and Chen [127] and Yu et al. [126] . The diameter of the static casing
of the RPB was 0.228 m, the inner and outer diameters of the pack-
ing in the RPB were 0.076 and 0.16 m respectively, and the height
was 0.02 m. The total volume of the packing in the RPB was of
0.0003114 m3. Stainless wire mesh with a speciﬁc surface area of
803 m2/m3and a void fraction of 0.96 was packed in the bed acting
as packing. In all these studies, there is signiﬁcant improvement in
overall mass transfer and height of transfer unit (HTU) demonstrat-
ing the performance superiority of an RPB compared to conven-
tional packed bed. Overall mass transfer coefﬁcient ( KGa) and HTU
corresponding to the most appropriate operating conditions in
RPB were found to be higher than 5.8 s/C01and lower than 1.0 cm
[114] . However HTU is around 40 cm for conventional PCC process.
The group in Chang Gung University in Taiwan studied RPB
absorber using cross-ﬂow RPB for CO 2capture which is believed
to have relatively small gas ﬂow resistance and unaffected by cen-
trifugal force. Another beneﬁt of cross-ﬂow is higher gas velocity
due to no critical gas velocity limitation. Lin et al. [128] and Lin
and Chen [129] found that cross-ﬂow RPB absorber is effective
for CO 2absorption process. In their study, the following rig speci-
ﬁcations were used: inner radius of 0.024 m, an outer radius of
0.044 m, and an axial length of 0.12 m, speciﬁc surface area of
855 m2/m3and a voidage of 0.95.
2.1.4. India
India Institute of Technology (IIT) Kanpur reported the use of
RPB as absorber in CO 2absorption process using split packing.
The two packing discs can rotate co-currently or counter-
currently. Their work shows that counter-current rotation of the
packing disc gives better performance. The technology improves
slip velocity to as high as 30 m/s [130] . It was also reported in their
study that this type of RPB shows good performance in gas phase
control processes by enhancing volumetric mass transfer coefﬁ-
cient on the gas side to about 35–280 times compared to those
of packed columns, the liquid side volumetric mass transfer coefﬁ-
cient enhances in the range of 25–250 times compared to the
packed column [130] . Agarwal et al. [131] stated that continuous
single block packing causes a signiﬁcant reduction only in the liq-
uid side mass-transfer resistance with little or no reduction in the
gas side resistance. Rajan et al. [130] studied RPB absorber in NaOH
solution and found that the split packing gives the highest volu-
metric liquid side mass transfer coefﬁcient as compared to conven-
tional packed column.M. Wang et al. / Applied Energy 158 (2015) 275–291 281

2.2. Experimental studies on intensiﬁed absorber
Signiﬁcant progress has been witnessed in the area of intensi-
ﬁed absorber, from the early work published by Chamber’s Wall
in early 1950’s to what we have at present. Newcastle research
team in the UK as reported by Jassim et al. [85] was able to estab-
lish that RPB has the potential to dramatically reduce the size and
cost of carbon capture units for power plants. Lee et al. [122]
reported that there are some uncertainties which need to be tack-
led such as (a) Power consumption; (b) Pressure drop; (c) Viscous
liquid distribution in a RPB, this leads to the modiﬁcation of the
experimental rig used by Jassim et al. [85] with the aim of address-
ing these challenges.
Research Groups in China and Taiwan also made signiﬁcant
progress towards the commercialization of this technology. The
early report of the technology based on counter-current ﬂow
has now turned to look at the other ﬂow geometries such as
co-current and cross-ﬂow arrangement to take the advantage of
lower gas phase pressure drop and eliminating the need for air
blower.
The research Group In India studies split packing RPB which has
been suggested to increase the gas-phase mass transfer coefﬁcient
as against continuous packing RPB which is said to have the same
gas phase mass transfer coefﬁcient as conventional packed column
[132] .3. RPB stripper: Current status of experimental rigs and
experimental studies
3.1. RPB stripper experimental rigs
Study on intensiﬁed stripper experimental rig for intensiﬁed
PCC process was published by just two research groups: Newcastle
University in the UK and National Tsing Hua University in Taiwan.
With both groups, reboiler is the same as that of conventional
packed column (i.e. big in size).
3.1.1. Newcastle University, UK
Jassim et al. [85] reported RPB stripper for desorption runs for
30 wt%, 54 wt% and 60 wt% MEA solution having ﬂow rate range
from 0.2 kg/s to 0.6 kg/s. The rich MEA solution is preheated to
the temperature range between 57 /C176C and 70 /C176C and at atmo-
spheric pressure before being sent into the intensiﬁed stripper.
The RPB stripper has internal diameter of 0.156 m, outer diameter
0.398 m and axial height of 0.025 m. The packed bed material was
stainless steel expamet with very high speciﬁc surface area
(2132 m2/m3) and a moderate voidage (0.76). Comparison between
RPB stripper and conventional stripper operating at the same per-
formance was done by Jassim et al. [85] which shows that the
intensiﬁed stripper height is reduced by a factor of 8.4 and its
diameter is reduced by a factor of 11.3.
3.1.2. Taiwan
With conventional packed columns, energy consumption in
capturing CO 2from a conventional coal-ﬁred power plant ranges
from 3.24 to 4.2 GJ/tonne CO 2[20]. Kothandaraman et al. [133]
noted that the majority (approximately 62%) of the energy con-
sumed during the CO 2capture process was required for the regen-
eration of solvent. Moreover, the consumption of steam is the most
important component of the operating costs of alkanolamine
absorption as reported in Chapel and Mariz [134] ; Tobiesen and
Svendsen [135] .
In order to regenerate CO 2-rich solvent solution at a tempera-
ture higher than 100 /C176C and a pressure higher than atmospheric
pressure, Cheng et al. [88] introduced a back pressure regulator,
this is the major difference between Jassim et al. [85] setup and
Cheng et al. [88] setup. Because of the back pressure regulator,
Fig. 4. Printed Circuit Heat Exchanger (Courtesy of Heatric Ltd): the big one at the
back is shell-and-tube heat exchanger; while the small one in front is PCHE.
Fig. 5. Summary of Technology of PCHE, H2X, and FPHE (Courtesy of Heatric).282 M. Wang et al. / Applied Energy 158 (2015) 275–291

the regeneration could be operated at various temperatures over a
ﬁxed pressure, and vice versa. Cheng et al. [88] rig speciﬁcations
are as following: the diameter of the static casing of the RPB was
0.228 m, the inner and outer diameters of the packing in the RPB
were 0.076 and 0.16 m respectively, and the packing height in
the RPB was 0.02 m. The total volume of the packing in the RPB
was 0.000311 m3. For the RPB packing, a stainless wire mesh with
a speciﬁc surface area of 803 m2/m3and a void fraction of 0.96 was
packed into the bed.
The use of an RPB apparatus instead of a packed bed not only
dramatically reduces the required stripper volume but also con-
sumes less regeneration energy [88].
3.2. Experimental studies on intensiﬁed regenerator
Intensiﬁed regenerator for CO 2capture was reported by Jassim
et al. [85] and Cheng et al. [88]. In both studies, they found that RPB
regenerator can signiﬁcantly reduce the size of column as com-
pared to conventional stripper, but the reboiler size is still as bigas before since it has not been intensiﬁed. Cheng et al. [88]
improved from Jassim et al. [85] by introducing a back pressure
controller, this will help in operating the regenerator at higher
pressure and temperature.
4. Intensiﬁed heat exchanger
In conventional PCC process, there is a cross heat exchanger.
This is huge in volume. In addition to this, the piping surrounding
the cross heat exchanger has high footprint. Therefore, the cross
heat exchanger has to be intensiﬁed.
4.1. Technologies available to choose
4.1.1. Printed Circuit Heat Exchanger (PCHE)
The PCHE was invented in 1980 in Australia and applied to
refrigerators in 1985 by Heatric (UK) [136] . The PCHE is a high-
integrity plate type compact heat exchanger in which ﬂuid ﬂow
channels are produced by chemical etching on ﬂat metal plates.
Etched plates are stacked to produce single block by diffusion
bonding [136–139] .
Because of the compactness provided by PCHE design, the vol-
ume of PCHEs are typically 4–6 times smaller and lighter than con-
ventional shell-and-tube heat exchangers designed for the same
thermal duty and pressure drop as shown in Fig. 4 [140,141] .
Low pressure drop in PCHE can be found based on design. Kim
et al. [138] compared air-foil ﬁn PCHE and zigzag channel PCHE
which have the same heat transfer performance but the pressure
drop of airfoil ﬁn PCHE is one-twentieth of zigzag PCHE. PCHE
effectiveness was reported to be more than 98% and can operate
at maximum allowable pressure of 600 bar and more than 800 /C176Cmaximum operating temperature (limited by material of construc-
tion). PCHE has multi-ﬂuid capability (intensiﬁcation achieved by
reducing the number of exchanger units) [141] .
4.1.2. Formed Plate Heat Exchanger (FPHE)
The FPHE uses the same concept as various ﬁn plate heat
exchangers, but adds the advantage of replacing the brazing pro-
cess with the diffusion-bonding process. This is shown in Fig. 5 .
Heatric Ltd reported that FPHE has bigger channels size (about
3m m /C23 mm) than the PCHE, this leads to lower pressure drop
than PCHE [141] . FPHE has effectiveness of more than 98%. Maxi-
mum allowable pressure for FPHE is 200 bar and can operate at
higher temperature of up to 800 /C176C, it has multi-ﬂuid capability
(Intensiﬁcation by reducing number exchanger units) [141] .
4.1.3. Hybrid Heat Exchanger (H
2X)
H2X technology developed by Heatric Ltd combines the etched
plates and the formed ﬁns to form what is known as Hybrid Heat
Exchanger [141] . The heat exchanger takes some of the advantages
offered by PCHE and FPHE. H2X has bigger hydraulic diameter than
PCHE because of the presence of FPHE and can also withstand
higher pressure than FPHE because of the advantage offered by
the presence of PCHE. Typical hydraulic diameter of PCHE is in
the range of 0.1–3 mm while that of FPHE is in the range of 1.2–
3.3 mm [141] .
4.1.4. The Marbond heat exchanger
The manufacturing procedures of Marbond heat exchanger are
similar to those of the PCHE. It is formed of slotted ﬂat plates which
have been chemically etched through. The plate pack is then
diffusion-bonded together [142,143] . In contrast with the PCHE,
several thinner, slotted plates are typically stacked to form a single
sub-stream, thus giving the potential for very low hydraulic diam-
eters [142] . In some applications, it has a substantially higher area
density than the PCHE. For example, a doubling of porosity, otherfactors being equal, results in a halving of the volume for a given
surface area [144] .
4.1.5. Spiral heat exchanger (SHE)
SHE refers to a helical tube conﬁguration. The term refers to a
circular heat exchanger with two long metal strips of plate rolledtogether to form a pair of concentric spiral channels of rectangular
cross-section, one for each ﬂuid. The passages can be either smooth
or corrugated, in some cases studs are welded onto one side of each
strip to ﬁx the spacing between the plates, to provide mechanical
strength and to induce turbulence that increases heat transfer
[145] .
The internal void volume is lower (less than 60%) than in a shell-
and-tube heat exchanger [145] , and this yields a compact and
space-saving construction that can be readily integrated in any
Table 3
Evaluation of solvent properties [151] .
Property Importance Potential show-stopper Evaluation methods
Reaction kinetics 10 Yes Literature, wetted-wall column (WWC)
Absorption capacity 10 Maybe Calculation from VLEHeat of absorption 10 Yes Literature, Calorimetry Measurement, Calculation from VLEToxicity 6 Yes Literature/material safety data sheet(MSDS)Volatility 4 Maybe LiteratureCorrosivity 6 Maybe Literature, Laboratory Test
Degradation 6 Yes Literature, Laboratory Test
Foaming 4 Maybe LiteratureViscosity 4 Yes Literature, Pilot TestSurface tension 4 Maybe LiteratureCost 2 Maybe VendorM. Wang et al. / Applied Energy 158 (2015) 275–291 283

plant and reduces installation costs. The heat transfer surface ranges
from 0.05 m2for refrigeration applications up to about 500 m2with
a maximum shell diameter of 1.8 m and the sheet metal thickness
range is 1.8–4 mm for industrial processes [146] . The surface area
requirement is about 20% lower than that for a shell-and-tube unit
for the same heat duty [145] . SHEs are often used in the heating of
high viscosity and dirty ﬂuids. It exhibits lower tendency to fouling
[147] . When a SHE requires cleaning, all heat transfer surfaces are
readily accessible by simply removing the heads.
4.2. Recommendation for intensiﬁed Heat Exchanger for PCC
application
To make a decision on best intensiﬁed heat exchanger to be
used for PCC application, many factors need to be considered. Someof them are listed as follows [140] : (a) Operating Pressure limits;
(b) Thermal performance (also known as the effectiveness of the
heat exchanger); (c) Expected working temperature range; (d) Pro-
duct mix to be used in the exchanger (liquid-to-liquid or gas-to-
gas); (e) Pressure drop desired across the expected heat exchanger;
(f) The expected ﬂuid ﬂow capacities over both sides of the heat
exchanger; (g) Method of cleaning employed, maintenance and
repair issues associated with heat exchanger; (h) Materials
required for construction; (i) Ease of expansion of exchanger when
it becomes necessary; (j) The cost of the heat exchanger.
Compromise would therefore have to be made in most cases
when selecting a heat exchanger. For instance, cost of the exchanger
is a paramount factor, but it should not be the determining factor. If
just for a cheaper heat exchanger, certain desired performance
demands of the heat exchanger would have to be forfeited.
The authors believe that the PCHE and the Marbond heat
exchanger look promising for use in intensiﬁed PCC process
because of its many beneﬁts such as high efﬁciency (>98%), Com-
pactness to improve safety and economics, weight saving, low
pressure drop, high temperature and retroﬁt options [141–143] .
PCHE has been reported to have additional advantage of being
multi-ﬂuid, meaning it can be used for preheating of rich-MEA
stream and also as a condenser for CO
2– stream.
5. Solvents used for intensiﬁed PCC process
There are extensive studies in solvent selection from both aca-
demia and industry trying to identify alternative solvents for con-
ventional PCC process. There are very few studies on PI using
different solvents [85,87,89,121,123–126,128,129,148–150] .
5.1. Factors to consider
Factors to consider when conducting solvent screening for con-
ventional PCC process and intensiﬁed PCC process is similar to
some extent but the major difference comes from residence time
of solvent in different technologies. In intensiﬁed PCC process,
the residence time is relatively short (less than 10% of the conven-
tional PCC process). Therefore the factors to consider are: (1) CO 2
absorption reaction kinetics, (2) CO 2absorption capacity, (3) heat
of absorption, (4) solvent toxicity, (5) solvent volatility, (6) solvent
corrosivity, (7) solvent degradation, (8) solvent foaming, (9)
solvent viscosity, (10) solvent surface tension and (11) cost.
(1) CO 2reaction kinetics: This determines the rate at which CO 2
will be captured. Fast reaction kinetics is essential for inten-
siﬁed PCC process since the residence time is very short.
(2) CO 2absorption capacity: This is related to the solvent ﬂow
rate required and the sensible heat requirement. HigherCO
2absorption capacity would require lower solvent ﬂow
rate and subsequent less regeneration energy demand.(3) Heat of absorption: This would be an important factor affect-
ing reboiler heat duty. Lower heat of absorption will require
less regeneration energy input to reverse the chemical reac-
tion and release absorbed CO 2.
(4) Solvent stability, operational issues and environmental
impact: These are the other factors to be evaluated when
selecting solvents. Solvent degradation (which may be con-
trolled by having high stability against oxygen and thermal
stress) and corrosion will cause an increase in operation
and maintenance (O&M) costs by making up solvent and
reducing the lifetime of the equipment. Higher solvent vis-
cosity would increase the pump work in circulating the sol-
vent between the absorber and regenerator. Cost and
availability of potential solvents in commercial scale could
contribute to limitations of the process feasibility. Environ-mental impacts such as solvent toxicity and volatility
deserve serious attention when judging the potential of a
solvent since causing secondary pollution while capturing
CO
2is not a scenario the public would be willing to take.
Other solvent characteristics such as surface tension and foam-
ing tendency are also important factors to consider when judging a
solvent’s potential. Table 3 gives evaluation of solvent properties
based on relative importance on a scale of 0–10, with 10 being
the most important property and 0 the least important property
[151] . These may provide insights for solvent selection in intensi-
ﬁed PCC process.
5.2. Solvents used
Different solvents were used for intensiﬁed PCC process by dif-
ferent research groups. Some researchers use one solvent while
others mix solvents so as to beneﬁt from properties each solvent
offers.
5.2.1. Alkanolamine
The use of MEA for CO 2capture in RPB was reported in Jassim
et al. [85]. MEA has high reactivity but is rapidly replaced by more
efﬁcient solvents because of its corrosive nature, toxicity and high
heat of reaction with CO 2. Diethanolamine (DEA) is much slower to
react with CO 2. It is not good for intensiﬁed PCC process itself.
Methyldiethanolamine (MDEA) has become an important alka-
nolamine because of its low energy requirement, high capacity
and high stability but has the disadvantage of low rate of reaction
with CO 2. Lin et al. [128] presents study on the evaluation of vari-
ous alkanolamine solutions for CO 2removal in cross-ﬂow RPB. The
reaction rate of these solvents with CO 2followed the order of
Piperazine (PZ) > MEA > 2-amino-2-methyl-1-propanol (AMP).
Yu et al. [126] reported study on CO 2capture by alkanolamine
solutions containing diethylenetriamine (DETA) and PZ in RPB.
They found that the CO 2capture efﬁciency of DETA in terms of
overall mass transfer coefﬁcient KGaand HTU was superior to that
of MEA in RPB. This is because DETA possesses higher CO 2absorp-
Table 4
Performance of proprietary commercial solvents [19].
Solvent Regeneration
Energy (GJ/t-CO 2)Efﬁciency
penalty (%)References
Econmaine FG+ 3.12 9.2 IEAGHG [169]
KS-1 3.08 8.4 IEAGHG [169]
KS-2 3.0 9.3 Gibbins and Crane
[170]
CANSOLV 2.33 8.2 Just [171] , Shaw [172]
H3 2.8 7.8 Wu et al. [168] , Stover
et al. [173]284 M. Wang et al. / Applied Energy 158 (2015) 275–291

tion capacity and reaction rate with CO 2than MEA. Higher boiling
point and lower vapour pressure of DETA will lead to lower energy
requirement and less loss of solvent in stripper compared with
MEA, suggesting DETA as a promising solvent to substitute MEA
for CO 2capture. The mixed solution DETA + PZ exhibited higher
CO2capture efﬁciency than DETA indicating PZ was a great
promoter for capturing CO 2. This was because the promoter PZ
possesses higher reaction rate with CO 2than DETA [126] .
5.2.2. NaOH
Munjal et al. [152] reported the use of NaOH for absorption of
CO2. Their study shows that the gas–liquid mass transfer could be
improved. Lin et al. [153] compared the overall volumetric mass-
transfer coefﬁcient ( KGa) of RPB for different solvents (i.e. NaOH,
MEA and AMP) and found that KGavalues for the CO 2-MEA system
were approximately 2–5 times higher than those for the CO 2-AMP
system also KGavalues for MEA were at least 20% higher than those
for NaOH at the same operating conditions. Therefore rate of reac-
tion for CO 2capture in RPB follows the order MEA > NaOH > AMP
[154] . But AMP has higher absorption capacity than MEA. Lin and
Chen [81], Luo et al. [125] studied chemisorption’s of CO 2
using NaOH in RPB. They found that NaOH has the potential for
use as solvent in RPB, but one of the major challenges is the forma-
tion of stable salt which make solvent regeneration difﬁcult.
5.2.3. Ionic liquid (1-n-butyl-3-methyllimidazolium
hexaﬂuorophosphate)
The use of ionic liquids for CO 2capture is gaining interest due to
their unique characteristics (i.e. wide liquid ranges, thermal stabil-
ities, negligible vapour pressures up to their thermal decomposi-
tion points, tunable physicochemical characters, and high CO 2
solubility) [121,155] . However, ionic liquids are commonly high
or superhigh viscosity liquids with poor ﬂuidities. A signiﬁcant
limitation for large-scale application of a continuous CO 2capture
process for conventional packed columns by ionic liquid is the
great resistance of mass transfer and low gas–liquid mass transfer
rate due to the high viscosity. As reported in Chen et al. [118] , the
dependence of kLaon liquid viscosity in RPB is less than that of
packed column.
5.2.4. Potassium Carbonate (K 2CO3)
The use of K 2CO3is receiving great attention because of its high
CO2absorption capacity. Firstly, K 2CO3is a more efﬁcient solvent
for CO 2than either MEA or DEA [156] . This means that for a given
amount of solvent, K 2CO3can absorb more than the other two sol-
vents. In addition, the cost of this solvent is lower because less is
needed and K 2CO3is cheaper than other traditional solvents
[156] . Secondly, this eliminates the need for cross heat exchanger
because the stripper runs at lower temperature than the absorber
[156] . Thirdly, K 2CO3increases the safety in CO 2removal by not
only absorbing CO 2but also small amounts of hydrogen. Hydrogen
possesses a safety threat. Flashing off hydrogen can cause ﬁres or
explosions if proper precautions are not taken. Lastly K 2CO3is not
volatile, which means minimal losses of the solvent with the exit
gas occur. Since K 2CO3is not prone to the degradation reactions
associated with MEA, there is no loss of solvent associated with
degradation [133] . However, one of the major drawbacks of using
K2CO3in RPB is its low rate of reaction. This necessitated the need
for promoter so as to increase its rate of reaction. Kothandaraman
et al. [133] reported regeneration energy (without energy recuper-
ation) of 3.2 MJ/kg for K 2CO3when treating ﬂue gas (12 vol% CO 2).
5.2.5. Benﬁeld solution (Amine-promoted hot K 2CO3solution)
Amine-promoted hot K 2CO3solution, which is called Benﬁeld
solution, is used in Benﬁeld process [157] . The amine promotercould signiﬁcantly enhance the reaction rate while the carbon-
ate–bicarbonate buffer offers advantages of large capacity for CO 2
capture and ease of regeneration [123,157] . Pilot plant studies by
Field et al. [158] shows that hot-carbonate system is particularly
effective for removing CO 2, especially when present at high partial
pressure. Steam consumption is one-third to one-haft that of etha-
nolamine. Therefore, Benﬁeld Process is known as an economic and
efﬁcient way of removing large quantities of CO 2from ﬂue gases
and can be effectively used in RPB [123] .
5.2.6. Piperazine (PZ)
PZ is a diamine solvent whereby one amine group is involved in
a fast reaction with CO 2to form the carbamate while the other
amine absorbs the released proton [159] . PZ reacts rapidly with
CO2and thus has attracted interest for usage in CO 2capture, partic-
ularly as a reaction rate promoter for CO 2absorption in carbonate
and tertiary amine solutions [148,159–162] . Chemical reactions
which describe the absorption of CO 2in PZ solutions are more
complex than MEA [159,160] .
Reaction rate between CO 2and aqueous PZ solution is high
[148,160–162] . However, the absorption has to take place at high
temperatures because its solubility in water is limited [161] . Free-
man et al. [160] suggested the use of concentrated PZ solution for
CO2capture because of its effective resistant to oxygen degradation
and thermal degradation. Despite its high reactivity with CO 2,i t
has some challenges such as limited solubility in water and more
volatile than MEA.
5.3. Proprietary commercial solvents
To avoid high thermal efﬁciency penalty due to high regenera-
tion energy, new solvents were developed and commercialised.
Econamine FG+ is MEA–based solvent with proprietary inhibitors
[163,164] . Sander and Mariz [163] reported resultant solution cir-
culation factor (m3solvent per m3Econamine FG+ solvent) for Eco-
namine FG+ solvent as 1 while 18 wt% MEA solvent has 1.7. The
Kansai Electric power Co. and Mitsubishi Heavy Industries, Ltd.
have developed new aqueous solutions of sterically-hindered ami-
nes designated as KS-1, KS-2 and KS-3 [165–167] . The world’s lar-
gest commercial PCC plant (Petra Nova/NRG 240 MWe W.A. Parish
project) planned to use KS-1 solvent when commissioning in 2016
[81]. The ﬁrst commercial CCS plant (SaskPower’s Boundary Dam
139 MWe project) uses Consolv solvent [79], the solvent is based
on tertiary amines, and probably includes a promoter to yield suf-
ﬁcient absorption rates for low pressure ﬂue gas streams. H3 sol-
vent is Hitachi’s proprietary solvent formulation which has much
lower regeneration energy compared with MEA [168] . Regenera-
tion energy and thermal efﬁciency penalty for different proprietarycommercial solvents were compared in Table 4 .
5.4. Recommendations on solvent selection for PCC process
Selection of solvents for CO
2capture process is a very important
design decision for both conventional and intensiﬁed PCC pro-
cesses. Firstly, the residence time in the intensiﬁed PCC process
is less than 10% of the conventional PCC process. Therefore solvent
for intensiﬁed PCC process should have fast kinetics to capture CO 2.
That is why most studies on RPB absorber uses primary or sec-
ondary alkanolamines due to their fast kinetics. Concentration of
the solvent in RPB is usually high in order to have high reaction
rate. High concentration solvent generally has high viscosity,
which prevents its use in conventional PCC process. However, this
is not a problem in RPB case. Secondly to achieve high CO 2absorp-
tion capacity and reaction kinetics fast, mixing solvents such as
amine-promoted K 2CO3will play a signiﬁcant role. Thirdly the
regeneration energy of solvents should be low in addition to fastM. Wang et al. / Applied Energy 158 (2015) 275–291 285

kinetics and high absorption capacity. Oexmann et al. [174]
reported mixing MDEA and PZ gives lower regeneration energy
of 2.52 GJ/t-CO 2. Lastly when an intensiﬁed PCC plant is to be built
in non-compliant area, volatility of the solvent will have a big
impact on whether or not the project will be permitted.
6. Modelling/simulation for CO 2capture process using RPB
Modelling and simulation can be used to circumvent the difﬁ-
culties with the experimental approach, and complement the
experimental studies.
6.1. Correlations for mass/heat transfer
Signiﬁcant progress has been noticed in the development of
correlations for mass/heat transfer in RPB. Tung and Mah [132]
developed correlations for liquid phase mass transfer coefﬁcient
based on the penetration theory. In developing Tung and Mah
[132] correlation, the effect coriolis acceleration and packing
material geometry were neglected. Chen et al. [175] developed cor-
relation that takes into consideration of those terms that were
neglected by Tung and Mah [132] . Chen [176] reported mass trans-
fer correlation for gas-phase mass transfer coefﬁcients which has
predicted experimental data reasonably well. The challenge of pre-
dicting accurately the interfacial area in RPB is another issue of
concern. Onda et al. [177] correlation for gas–liquid interfacial area
for conventional packed column was modiﬁed by replacing the
gravity term with centrifugal gravity term, but this does not take
into account different types of packing factors such as wire
diameter and the wire mesh opening. Luo et al. [124] developed
gas–liquid interfacial area correlation for wire mesh packing which
takes into account the effect of wire diameter and wire mesh
opening. Burns et al. [178] correlation predicts the liquid hold-up
for a high voidage structured packing in an RPB.6.2. Modelling/simulation of intensiﬁed absorber
Few open literature discussed modelling and simulation of
intensiﬁed absorber. The group in Taiwan modelled the RPB as a
series of continues stirred tank with contactors. Cheng and Tan
[114] reported that ﬁve CSTRs with a contactor can achieve the
set target for a given case through simulation study. The research
group at University of Hull, UK reported modelling and simulation
of RPB absorber using Aspen Plus/C210and visual FORTRAN [87,89] .
Their key ﬁndings include: (a) the packing volume can be reduced
52 times and the absorber size can be reduced 12 times; (b) there
is no temperature bulge observed so far inside the packing [87,89] .
6.3. Modelling/simulation of intensiﬁed stripper
Experimental studies of intensiﬁed regenerator were only
reported in Jassim et al. [85] and Cheng et al. [88]. No modelling
and simulation of intensiﬁed stripper was reported in open
literature.
6.4. Modelling and simulation of the whole plant
Open literature on modelling and simulation of whole intensi-
ﬁed PCC process was not available as at the time of this review.
7. Prospective of applying PI technology into PCC using solvents
With the high potential to reduce capital and operating costs for
carbon capture, the UK Engineering and Physical Sciences Research
Council (EPSRC) recently awarded a consortium project worth
£1.27 million to the universities of Hull, Newcastle, Shefﬁeld and
Imperial College London to apply PI technology into PCC with sol-
vents process.
Fig. 6. Simpliﬁed PFD of intensiﬁed chemical absorption process for PCC.286 M. Wang et al. / Applied Energy 158 (2015) 275–291

7.1. Fundamental study regarding Marangoni effect and enhanced
mass transfer
Interfacial turbulence (i.e. Marangoni effect) which is caused by
surface tension gradient have been analysed by Semkov and Kolev
[179] , Kolev and Semkov [180] , Sternling and Scriven [181] and
Buzek et al. [182] . The main reason for the phenomenon of instabil-
ity can be the local disturbances of temperature and /or concentra-
tion near the interface [182] . Marangoni effect can signiﬁcantly
enhance mass transfer rate by a factor of two or more, but it can
easily be damped by a surface active agent. Therefore, amine solu-
tions used for absorption should not be contaminated by even
traces of surfactants [182] . A future task is to use simple experi-
ments to observe whether interfacial turbulence exists in RPB
absorber.
7.2. Proposed schematic PFD for whole intensiﬁed PCC process
Since there is no pilot plant of whole intensiﬁed PCC process in
the world, we propose a simpliﬁed whole intensiﬁed PCC process.
Fig. 6 describes potential technologies (RPB, Spinning disc and
PCHE) proposed for the intensiﬁed PCC.
Comparing Fig. 6 (intensiﬁed PCC using solvent) with Fig. 1
(conventional PCC using solvents), there are three main differ-
ences: (1) Rich solvent is regenerated in the stripper which use
spinning disc reboiler incorporated outside RPB packing in order
to use the same motor for rotation; (2) the cross heat exchanger
in the conventional PCC technology is replaced with the intensiﬁed
heat exchanger based on PCHE. The intensiﬁed heat exchanger is
multi-ﬂuid which can be used as condenser for the CO 2stream
and also pre-heating rich solvent. Therefore this integration can
reduces or eliminate condenser cooling cost; (3) Intensiﬁed absor-
ber and stripper are driven by motors.
Checked against the deﬁnition of PI in Section 1.6, the proposed
PFD in Fig. 6 achieves PI in the following ways: (a) the size of the
intensiﬁed absorber and stripper is reduced signiﬁcantly due to
the centrifugal ﬁeld; (b) the reboiler and the stripper are merged
together into a single item of equipment. The condenser is also
merged into the multi-ﬂuid intensiﬁed heat exchanger.
7.3. Experimental rigs and experimental studies
For intensiﬁed absorber or stripper, conscious judgement on the
best ﬂow arrangement (i.e. counter-current, co-current or cross-
ﬂow) is necessary in RPB design of experimental rig so as to decide
which ﬂow geometry will have better RPB performance and at
minimum energy penalty (due to vapour phase pressure drop).
Currently, there are only standalone intensiﬁed absorber or
stripper worldwide. The experimental rig for the whole intensiﬁed
PCC process is necessary to build so as to understand the dynamic
behaviour of the whole capture process and to provide foundation
for studies in optimal design, operation and control.
Mass transfer performance of the intensiﬁed absorber has been
fully determined by experimental studies and modelling & simula-
tion. More studies are needed to understand the actual surface area
in the RPB which over the years not been fully determined.
Dynamic ﬂow behaviour in RPB is another aspect that needs to
be studied.
7.4. Selection of solvents
Studies in conventional packed column showed that solvent
with high viscosity affects its performance. Zhang et al. [121]
reported that the impact of high viscosity on CO 2capture process
is not so severe for intensiﬁed CO 2capture process. Therefore study
on ionic liquid solvent which has high absorption capacity andselectivity can be a good driver in improving the performance of
intensiﬁed PCC process. Again studies on mixed solvents in inten-
siﬁed PCC process should be emphasized in order to bring in bal-
ance during absorption and desorption so as to have high capture
performance in the absorber and less amount of regeneration
energy to be consumed in the stripper.
7.5. Modelling and simulation of intensiﬁed CO 2capture process
Thermodynamic and transport property data is central to any
modelling and simulation of intensiﬁed CO 2capture process and
these properties were readily available for up to 30 wt% aqueous
MEA solution. However higher MEA concentration is required for
RPB absorber or stripper due to low residence time. There is verylimited data for CO
2with high concentration MEA in literature.
Solubility (i.e. VLE) data for MEA concentration up to 60 wt%
and for temperature range of 40–120 /C176C were reported in Aronu
et al. [183] . Mason and Dodge [184] reported solubility for MEA
concentration up to 75 wt%. More solubility data at 80 wt% or even
100 wt% MEA concentrations is needed for intensiﬁed PCC process.
Therefore there is a need for more solubility studies for higher sol-
vent concentrations. This can be done by experiment or using
molecular simulation software to interpolate or extrapolate.
Other areas that require experimental or molecular simulation
study are reaction equilibrium constants and kinetic parameters
determination for higher solvent concentration with CO 2.
Most studies through modelling and simulation focused on
intensiﬁed absorber with few researches on intensiﬁed stripper
for PCC. Studies on steady state simulation of intensiﬁed absorber
were reported in Joel et al. [87,89] with main aim on process anal-
ysis for design and operation. However, these studies could not
check the dynamic behaviour of the absorber or the whole intensi-
ﬁed PCC process. Therefore future study on dynamic modelling is
necessary in order to meet such challenges. It is believed that if a
dynamic model is developed and validated, sensitivity analysis will
be done for optimal design, operation and control.
7.6. Scale-up
Commercial-scale capture on operating power plants has yet to
be undertaken, leading to uncertainty regarding scale-up and inte-
gration of existing technologies [185] . Harzog [186] reported that
the challenge for CCS commercial deployment is to integrate and
scale up these components (absorber, heat exchanger and the
regenerator). Shi et al. [187] and Yang et al. [188] use computa-
tional ﬂuid dynamic (CFD) to study ﬂuid ﬂow in RPB. But more
studies are required for scale-up of RPB columns. To be able to
carry out the scale-up study of an intensiﬁed PCC process, it is rec-ommended to couple process modelling software with CFD soft-
ware so as to accurately predict the hydraulic behaviour and the
mass transfer behaviour of the RPB.
7.7. Evaluation of technical, economical and environmental
performance
So far, no detailed and systematic studies were reported on the
technical, economical and environmental impact on the use of
intensiﬁed PCC process compared with conventional PCC process.
There are some operational beneﬁts when using RPB in intensi-
ﬁed PCC process. The ﬁrst is its ability to be operated at higher gas
and/or liquid ﬂow rates owing to the low tendency of ﬂooding
compared to the conventional packed bed [128] . The second bene-
ﬁt of using RPB is its better self-cleaning, avoidance of plugging in
the system, and being unaffected by a moderate disturbance in its
orientation [189] .M. Wang et al. / Applied Energy 158 (2015) 275–291 287

Joel et al. [87] carried out comparative study between conven-
tional absorber and intensiﬁed absorber, and found the size reduc-
tion factor of about 12 times. Jassim et al. [85] reported stripper
height reduction factor of 8.4 and stripper diameter reduction fac-
tor of 11.3 as compared to conventional packed column. Cheng
et al. [88] reported a reduction factor for RPB stripper of at least
10 times as compared to conventional stripper. Li et al. [190]
reported that for PCHE performing the same duty as shell-and-
Tube heat exchanger has size reduction factor of 4–6 times. From
the analysis above, the size of main components in intensiﬁed
PCC process can be signiﬁcantly reduced.
Because of much less gas–liquid contact time that occurs in RPB
absorber than in a conventional packed bed columns, the selection
of solvent with a fast reaction rate with CO 2is crucial [85,87,89,11
2,113,120,127,191] . This necessitates the use of higher concentra-
tion solvent (such as 55 wt% or 75 wt% MEA reported in
[85,87,89] ), but this comes with another challenge of corrosion as
reported by Barham et al. [192] . This corrosion problem can be man-
aged by the use of (a) more expensive construction material such as
stainless steel rather than the commonly used carbon steel; (b) coat-
ing with high performance polymer on the surface of stainless steel.
In addition to steam consumption for solvent regeneration,
electricity will be consumed to drive the intensiﬁed absorber and
stripper in the intensiﬁed PCC process. This means parasitic energy
consumption added to carbon capture in intensiﬁed PCC process.
Cheng et al. [88] reported that regeneration energy of RPB stripper
is smaller than that of conventional packed column (excluding the
energy for rotating the RPB stripper). This is caused by decrease in
the amount of vapour lean MEA required from reboiler to RPB due
to improved heat transfer zone inside RPB thereby decreasing its
reboiler duty. Only Agarwal et al. [131] studied electricity con-
sumption to drive the motors in RPB absorber using DEA solvent
for carbon capture. Generally the higher the rotating speed, the
higher the electricity consumption by the motor. The study in
Agarwal et al. [131] indicates that electricity consumption is quite
low at 900 rpm while the number increased signiﬁcantly at
1500 rpm. More experimental studies are required to quantify
the contribution of electricity used by motors to overall energy
consumption in intensiﬁed PCC process.
The authors have performed preliminary technical and eco-
nomic analysis for intensiﬁed PCC process compared with conven-
tional PCC process. The initial prediction is that the capital cost of
the whole intensiﬁed PCC process can reduce to 1/6 (i.e. 16.7%)
compared with the same capacity conventional PCC process. The
reasons behind this prediction are: (a) the average size reduction
is around 12 times; (b) Due to corrosion, stainless steel has to be
used instead of carbon steel. Unit material price will roughly dou-
ble. The initial prediction on energy consumption in capturing unitmass of CO
2will be similar between the two processes. The reasons
behind this prediction are: (a) the steam consumption (or the
regeneration energy) in intensiﬁed PCC process will be lower due
to higher concentration of solvent used; (b) electricity consumed
to drive the intensiﬁed absorber and stripper in the intensiﬁed
PCC process is highly related to rotating speed. The second item
can only be determined by speciﬁc design conditions.
In summary, it is necessary to quantify overall costs (capital &
operating costs) used for capturing unit mass of CO 2in intensiﬁed
and conventional PCC processes based on detailed and accurate
process models. Detailed life cycle analysis (LCA) for intensiﬁed
PCC process should be performed in order to compare with con-
ventional PCC process.
8. Conclusions
The paper presents a critical evaluation of current research
status in intensiﬁed PCC regarding experimental rigs (includingintensiﬁed absorber and stripper, intensiﬁed heat exchanger),
experimental studies worldwide, solvent selection, modelling and
simulation. It was found: (a) there is no experimental rig for whole
intensiﬁed PCC process apart from standalone intensiﬁed absorber
or stripper. There have been no efforts to intensify the reboiler and
the cross heat exchanger so far. (b) There is no systematic study on
solvent selection for intensiﬁed PCC process. (c) There are some
papers on steady state modelling and simulation of intensiﬁed
absorber. No modelling and simulation of intensiﬁed stripper
was reported in open literature. Future research efforts and poten-
tial breakthrough on different aspects of intensiﬁed PCC process
have been discussed. These include: (a) A schematic PFD for inten-
siﬁed PCC process has been proposed. (b) It is important to use
simple experiments to observe whether interfacial turbulence (i.
e. Marangoni effect) exists in RPB absorber. (c) It is vital to developdynamic models for the whole intensiﬁed PCC process for future
work in process control. (d) It is necessary to combine CFD study
and process modelling for scale-up study. (e) A preliminary techni-
cal and economic analysis for the intensiﬁed PCC process has been
carried out in comparison with conventional PCC process. More
detailed and systematic technical, economic and environmental
performance analysis should be performed.
Acknowledgements
The authors from University of Hull would like to acknowledge
ﬁnancial support from EPSRC Research Challenges in Carbon Cap-
ture for CCS (Ref: EP/M001458/1), UK Research Councils’ Energy
Programme (Ref: NE/H013865/2) and EU FP7 International
Research Staff Exchange Scheme (Ref: PIRSES-GA-2013-612230).
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