Renewable and Sustainable Energy Reviews 41 (2015) 13241350

Contents lists available at ScienceDirect

Renewable and Sustainable Energy Reviews

journal homepage: www.elsevier.com/locate/rser

A journey into the process and engineering aspects of carbon

capture technologies
B. Sreenivasulu a, D.V. Gayatri a, I. Sreedhar a,n, K.V. Raghavan b
a
Department of Chemical Engineering, BITS Pilani Hyderabad Campus, Shameerpet, Hyderabad 500078, India
b
Reaction Engineering Laboratory, Indian Institute of Chemical Technology, Tarnaka, Hyderabad, India

art ic l e i nf o a b s t r a c t

Article history: Atmospheric warming due to greenhouse gases has become a serious global concern. Extensive efforts
Received 5 March 2014 are being made to combat this phenomenon through Carbon Capture as carbon dioxide is its major
Received in revised form contributor. In this work, a comprehensive review has been made on various Carbon Capture
16 September 2014
methodologies including adsorption, absorption, membrane separation, Chemical Looping Combustion,
Accepted 19 September 2014
cryogenic separation with focus on their process chemistry, critical process parameters, contactor
Available online 10 October 2014
congurations, kinetics, thermodynamics, process development and scale-up. The challenges at the
Keywords: research and development stages have also been identied so as to provide the future directions for
CC methodologies research.
Kinetics and heat/mass transfer & 2014 Published by Elsevier Ltd.
Reactor engineering
Scale-up

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1325
2. Potential pre- and post-combustion CC options. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1327
2.1. Gasliquid absorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1327
2.1.1. Absorbent selection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1328
2.1.2. Contactors for Absorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1330
2.1.3. Modeling and kinetic studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1330
2.2. Gassolid adsorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1331
2.2.1. Pressure, thermal and electrothermal swings . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1331
2.2.2. Adsorbents and their selection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1332
2.2.3. Contactors for adsorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1332

Abbreviations: AAP, agglomeration and attrition of particles; Ac, adsorption cycle; Apl.F, application formulated; APOC, analytical proof of concept; AR, air reactor; ARR,
auto reduction reactor; BESs, bioelectrochemical systems; BFB, batch uidized bed; BN, boron nitride; BPOB, basic principles observed; BR-MPBR, biomass retention-
membrane photo bio reactor; BS, bench scale; BZX, binderless zeolite 13X; CASU, cryogenic air separation unit; CASU-PB, cryogenic air separation unit-packed bed; CC, CO2
capture; CCI, combined cycles integrated; CDCL, coal direct chemical looping; CLAS, chemical-looping air separation; CLC, chemical looping combustion; CLOU, chemical-
looping with oxygen uncoupling; CLP, calcium looping process; CMBS, circulating moving bed system; C-MPBR, carbonation-membrane photo bio reactor; CnC, counter
current; CnC-MBR, counter-current moving bed reactors; Con-O, continuous operation; CPDm, component prototype demonstration; CPDt, component prototype
development; CRS, condensed rotational separation; Dc, desorption cycle; DOCPB, dynamically operated cryogenic packed-bed; ESA, electric swing adsorption; FAC, ne
activated carbon; FBR, uidized bed reactor; Finlet, feed inlet conditions; FPSC, free piston stirling cooler; FR, fuel reactor; FRR, ber to resin ratio; FSCD, full-scale commercial
deployment; GP, gas permeation; HCM, honeycomb monolith; HTC, hydro talcite; ICC, inlet CO2 concentration; IFBR, interconnected uidized-bed reactors; IPA, isopropanol
amine; La, liquid ow area; LCT, laboratory component testing; LS, lab scale; MBA, moving bed adsorber; MCFC, molten carbonate fuel cells; MCR, max. compression ratio
(per stage); MEA, methyl ethyl amine; MECs, microbial electrolysis cells; MEDC, microbial electrodialysis cell; MOF, metal oxide framework; MS, microwave synthesis; MxOy,
oxidized form of metal oxide; MxOy
1, reduced form of metal oxide; N, absorption rate; NDC, non-dispersive contact; NPC10, nitrogen enriched porous carbons; OC, oxygen
carrier; OFC-I, 1st generation oxyfuel combustion; OFC-II, 2nd generation oxy-fuel combustion; OFC-III, 3rd generation oxy-fuel combustion; PBR, packed-bed reactor; PEG,
poly ethylene glycol; PEI, poly ethylene imine; Pexit, product exit conditions; Post-CCC, post-combustion CC; PP, partial pressures; Pre-CCC, pre-combustion CC; PSA, pressure
swing adsorption; PSD, pilot scale demonstration; RPBR, rotary packed bed reactor; SAFB, sound assisted uidized bed; SC, semi continuous; SLM, supportive liquid
membranes; S-P, selectivity and permeability; SPM, substituted polymer membranes; SSCD, sub-scale commercial demonstration; STCR, steam-to-carbon ratio; STS,
solvothermal synthesis; TSA, temperature swing adsorption; VPSA, vacuum pressure swing adsorption; ZIF, zeolitic imidazolate frameworks; ZX, zeolite 13X
n
Corresponding author. Tel.: 91 4066303512; fax: 91 4066303998.
E-mail address: isreedhar2001@yahoo.co.in (I. Sreedhar).

http://dx.doi.org/10.1016/j.rser.2014.09.029
1364-0321/& 2014 Published by Elsevier Ltd.
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350 1325

2.2.4. Kinetic and modeling studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1334

2.3. Membrane technology. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1334
2.3.1. Membrane separation and membrane materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1334
2.3.2. Membrane contactors and modeling studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1336
3. Chemical looping combustion (CLC) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1337
3.1. Signicant developments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1337
3.1.1. Oxygen carriers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1337
3.2. Reactor engineering aspects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1338
3.3. Kinetic and modeling studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1338
4. Cryogenic separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1338
4.1. Recent developments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1341
4.2. Engineering aspects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1341
5. Sustainability through CC and critical comparison of various CCTs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1342
5.1. Enhancing the sustainability levels of CC technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1342
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1343
Dedication . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1344
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1344
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1344

1. Introduction CO2 concentration is enhanced. It can be operated at high pressures

The rst meeting of United Nations Framework Convention on
Climate Change (UNFCCC) held in 1992 had triggered for global
concern on climate change due to GHG emissions. The global
warming due to carbon dioxide emissions has been receiving
worldwide attention to mitigate its adverse effect on the climate in
terms of temperature rise, continuous rise in sea level, increasing
occurrence of storms and oods. The main focus is on developing
novel processes for carbon dioxide capture (CC) [14]. It has been
predicted by the International Panel of Climate Change (IPCC) that
by the year 2100, the atmospheric content of CO2 shall reach
570 ppmv, rise in sea level of 3.8 m and a rise in global mean
temperature of about 2 1C with very serious consequences on
environment [58]. Coal continues to be the main fuel for power
generation worldwide and hence integrating CC with power
generation through pre and/or post-combustion options is on
the main agenda [9,10].
The relationship between the CO2 emissions (CD) with the
population (P), economic development (represented by gross
domestic product, GDP), energy production (E), carbon based fuels
used for energy production (C) and CO2 sinks (SCO2), expressed by
the modied Kaya's identity [11]:
GDP E C
CD P
SCO2
P GDP E
It shows that the three feasible ways to reduce the CO2
emissions viz., increase of energy efciency (E/GDP), change of
the fossil fuels to non-carbon forms of energy (for e.g., renewable
and nuclear energy) and to create CO2 sinks with the help of CC
technology [12,13]. It can be achieved through technological
options like pre-combustion removal of CO2 from the fuel, post-
combustion removal of CO2 from the ue gases, oxyfuel combus-
tion (OFC) to provide CO2 at a high concentration in the ue gases,
chemical looping and clatherate hydrate processes [1416]. The
presence of CO2 at a relatively higher concentration and at a higher
pressure in a pre-combustion option make them economically,
thermodynamically and kinetically more attractive. Post-combustion
CC though expensive is advantageous in that it can be successfully
integrated to the existing power generation plants to enhance their
efciency with simultaneous CC. Oxyfuel combustion (OFC) CC is the
latest of all technologies and is yet to be commercialized. By employ-
ing pure oxygen, the undesirable gases like NOx are minimized and
reducing the cost of CC. It, however, suffers from drawbacks like the
need for expensive cryogenic air separation unit, higher material
requirement and high temperatures for handling ue gases and their
recirculation [1719].
The post-combustion options for the CC are adsorption, absorp-
tion (physical and chemical), membrane and cryogenic separations
(Fig. 2). Absorption based CC employs physical or chemical inter-
actions between the CO2 and the absorbent. Solvents like rectisol,
selexol ,..etc. are employed for physical absorption [14]. For
chemical absorption, solvents like amines, alcohols and their
compatible blends, liquid ammonia and alkalies like NaOH,
K2CO3, and Na2CO3 are employed. Chemical absorption is widely
employed due to higher capture efciencies even at low concen-
trations of CO2 and higher selectivity's [2026]. Adsorption
attaches gas or liquid on solid adsorbents which then could be
regenerated by the application of temperature swing, pressure or
vacuum swing. Adsorbents like activated carbon, alumina, metal
oxides, zeolites and phosphates [14,2730], metal organic frame-
works [3134], microporous carbons and polymers [3539] and
modied amines [4042] are employed. CC could also be achieved
through membranes separation of CO2 from ue gases constitu-
ents due to its difference in permeability and selectivity. Organic
(polymeric) and inorganic (ceramic, carbon, zeolite, metallic, etc.)
membranes are employed for separation. Membrane also acts as a
1 contacting device for the gas and the solvent moving in counter-
current fashion with CO2 getting selectively absorbed on the
membrane matrix [15,43,44]. The advantages of the membrane
technology are high product purity, low cost, continuous proces-
sing with very low start up time while the disadvantages could be
non-attractiveness at low CO2 concentrations and high ue gas
temperatures and membrane fouling. Novel and effective mem-
branes can be developed by incorporating functional groups like
amines, combination of different and compatible membrane
materials and manufacture of biomimetic congurations [4547].
The fourth technical option of CC is cryogenic separation
involving the compression and cooling of gas mixture with CO2
at various levels to facilitate phase change of the CO2 along with
other constituents which can then be separated using distillation.
The advantages of this process are that no chemical absorbent is
needed, can be operated at atmospheric pressure and its compat-
ibility with both pre- and oxy-combustion CC with easy transport
of liquid CO2 formed. Its drawbacks are its feasibility at high CO2
concentrations (450%), formation of ice or solid CO2 clathrates in
the presence of water vapor leading to serious plugging, pressure
1326 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

Nomenclature M fCO2 mole fraction of CO2

MFgas mass of ue gas (g/g of CO2)
A absorbent concentration (kmol/m3) mt mass ux of CO2 deposition from ue gas to the
(A1,L1,T1 for NaOH & A2,L2,T2: for MEA) surface of cooling n
AC absorbent capacity (kg/kg) P pressure (MPa)
Ad-C adsorbent capacity (gCO2 =g ads ) PV pore volume (cm3/g)
AT activation temperature (1C) PVP vacuum pressure (Pa)
Bd bulk density (g/cm3) rc,inst instantaneous rate of conversion of the char
C CO2 concentration (v/v%) S solvent ow rate (kg/h)
CPs cycle periods (s) SA surface area of adsorbent (m2/g)
Cs specic heat of solids (J/(g K)) SFRR syngas feed rate to the reducer (L/min)
CT carbonization temperature (1C) SITC steam injection to combustor (g/min)
Dax axial mass dispersion coefcient SPECCA specic primary energy consumption for CO2 avoided
Dbed diameter of bed (m) (kJLHV =kgCO2 )
Dp particle size (m) SPL sound pressure level (dB)
Dpg size of spherical glass particles (mm) St synthesis time (h)
DT duration time (h) T temperature (oC)
EF enhancer ow (Ln/min) Tads adsorption time (s)
FF fuel ow (kg/h) Tdes desorption time (s)
FI inlet fuel (vol%) Tms microwave synthesis time (h)
Fsolids ow rate of solids (g/s) Trpt repressurization time (sec)
FT ue temperature (1C) Tsts solvothermal synthesis time (h)
G absorbent ow (m3/m2 h) ufuel feed velocity (m/s)
Ga gas ow area Umf minimum uidization velocity (m/s)
GTC gT/C(isentropic efciency)/gpump (%) V CH4 ow rate (kmol/h)
HCC higher cyclic capacity (%) Vf uidization velocity (cm/s)
HCE higher cyclic efciency (%) Vgas gas ow rate (m/s)
HCL higher cyclic load (%) V O2 =H2 O ow rate (kmol/h)
HEE heat exchanger efciency (%) Vvis viscosity of liquid
HR heat recovery (%) WC adsorbent working capacity (mol/kg adsorbent/cycle)
iC cell current density (A/m2) XOC chemical conversion of oxygen carriers (%)
ICC inlet CO2 concentration (%CO2) Xpth plate thickness (m)
KG,av volumetric overall mas transfer coefcient gs gas to solid heat transfer coefcient
(kmol m
3 h
1 kPa
1) Hr enthalpy of reaction
Ks thermal conductivity of solids (J/(m K s)) PRC pressure drop across the recycle chamber
L liquid ow rate (m3/m2 h) porous volume fraction
Lbed length of bed (m) eff effective axial heat dispersion coefcient
Lg inlet gas ow rate (L/min) OC/fuel ratio

build-up issues and reduction of heat transfer rates due to thick
CO2 layers formed on heat exchange surfaces [1416]. CLC is the
advanced version of OFC where the necessary oxygen for the
combustion of fuel is supplied from metal oxides avoiding the direct
combustion between air and fuel. The advantage of this process is the
inherent CC due to formation of CO2 with H2O as products thereby
requiring no additional separation step, minimal formation of NOx
gases, high capture efciency. It is yet to be commercialized since the
R&D is at the pilot plant level [9,43,48,49]. In CLOU the oxygen
required for combustion is released by the oxygen carrier in gaseous
phase thereby eliminating the gasication step while employing
gaseous fuels and also requiring smaller reactors reducing capital
costs when compared to CLC. This technology requires further
research before commercialization [50,51]. The Technology Readiness
Levels (TRLs) of all the above mentioned CC technologies are high-
lighted in Table 1 [5,6].
Table 1 shows that except gasication, oxyfuel combustion and
CO2 capture by absorption, other technological options need R&D

Table 1
TRL's of CC technologies.

TRL Scope Time (years) Pre-Combustion Post-Combustion Pre- & Post-Combustion

Gasication IGCC Abs. Ads. Mem.S MBFA OFC I OFC II OFC III Clatharites

9 FSCD 36
8 SSCD 25
7 PSD 25
6 CPDm 24
5 CPDt
4 LCT
3 APOC
2 Apl.F
1 BPOB
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
efforts on larger scale to prove their techno-economic viability.
TRL-4 is a typical end-point of R&D efforts at university level.
2. Potential pre- and post-combustion CC options
Fig. 1 shows the critical unit processes and operations involved
in pre and post-combustion CC technologies and their down-
stream applications in thermal power and fertilizer sectors. It
shows that both pre and post-combustion options can be
employed for coal and biomass. Gasication and reforming of
fuels can be used for achieving enhanced combustion rate and for
hydrogen production. Insitu ammonia and urea production will
minimize the energy penalties associated with CC [52]. The
oxyfuel combustion can be implemented in three modes and
two of them facilitate fuel combustion through a looping process.
The current status of the above technologies can be summarized as
 In pre-combustion technologies, the carbon in the fuel is
converted into synthesis gas upto 90% before combustion
through gasication or reforming processes. Employing inte-
grated coal gasication combined cycle (IGCC) concept, the
resulting gas can be further converted into a stream of H2 and
CO2 through a shift reaction. The pre-combustion technologies
can be applied to new power plants, their technologies are yet
to reach commercial maturity levels and they require high
capital investments due to major changes to be brought into
boiler and ue gas systems.
 In post-combustion technologies, CO2 is separated from com-
bustion ue gases by employing absorption, adsorption, mem-
brane separation and other options for coal, gas and other fossil
fuel based thermal power plants by retrotting. They are yet
to be commercially established except in the case of the
absorption option. The CO2 in the ue gases is in fairly diluted
concentrations (1015%) needing high recovery and capital
costs and 2530% additional energy for plant operation.
Fig. 1. Pre and post-combustion of CC technologies.
1327
 Oxyfuel, chemical looping and clatherate hydrate processes can
be employed in pre and post-combustion modes. The former
employs pure or enriched oxygen for combustion of fuel or ue
gases to obtain CO2 in higher concentration. The clatherate
process forms hydrate crystals from water and CO2, N2, O2, H2
and natural gas components. The process enables the max-
imum CO2 recovery of 42.5% at 8.5 MPa [53].
In all above options for CO2 capture and recovery, pilot experi-
mentation, modeling, validation tests and eld scale demonstrations
are essential to establish their commercial viability.
Post-combustion CC processes are well-suited for retrotting
into coal/gas red thermal power plants for CO2 removal from the
ue gases. They generally contain less than 15% of CO2 and smaller
concentrations of nitrogen, water vapor, SOx and NOx. Fig. 2 shows
a variety CC options based on gasliquid absorption, gassolid
adsorption and solid membrane facilitated separations. The main
factors impacting CC efciencies are ue gas composition and its
temperature and energy penalties associated with the desorption
process.
2.1. Gasliquid absorption
CC by absorption is a more widely employed technical option
than the other post-combustion CC options. It is a well-established
phenomenon which can be easily integrated/retrotted to any
power generation system as an end of the pipe technology.
Moreover, it is highly selective with very high CC efciency. Most
of the absorbents are very economical and can be easily regener-
ated. It has been widely used in coal gasication, petroleum
rening, syn-gas production, natural gas (sweetening) and hydro-
gen manufacture. The literature reports show that this technology
was the only commercially attractive option for CC until 2030
[5456]. Lower efcacies besides limited understanding of their
absorption process have made them relatively less popular [7,8].
1328 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

Fig. 2. Technical options of various CC methods from ue gases.

Fig. 3. The absorption system for CC.

The energy penalty for CO2 absorptiondesorption lies in the
range of 0.370.5 MWh/ton CO2. By employing more novel sol-
vents and their blends the energy penalty may be brought down to
0.190.2 MWh/ton CO2.
Chemical absorption can effectively remove acid gases from ue
gas by employing amine based solvents [10]. A reversible reaction
takes place during chemical absorption forming a weakly bonded
intermediate such that the reaction could be reversed by the
application of heat or pressure. Also, chemical absorption gives a
pure stream of CO2 after stripping the solvent [11]. Physical absorp-
tion obeys Henry's law (temperature and pressure dependent).
Organic solvents like selexol, rectisol, etc. were employed to physi-
cally absorb CO2 at higher pressure and lower temperature which
were regenerated later at reduced pressure and high temperature
[12]. Fig. 3 below shows the components of an absorption system
along with its type of contactors and solvents employed.
2.1.1. Absorbent selection
An absorbent should have high reactivity and absorptivity with
respect to CO2, low vapor pressure, easy regenerability, high thermal
and chemical degradation stability, low environmental impact
(green) and economical. Table 2 1.1 highlights the absorbent and
process options. Among various absorbents used for CC the earliest
and most commonly employed agent has been monoethanolamine
(MEA). It is relatively cheap, has high reactivity and higher absorption
rate. It can, however, degrade in oxidizing atmosphere, energy
intensive during regeneration, has limited CO2 loading capacity and
corrosive with foaming and fouling characteristics [13,43,5764].
Other alkanolamines like DEA have also been used for absorption
but they also suffer from similar drawbacks. A blend of MEA and DEA
i.e. Methyldiethanolamine (MDEA) has been employed with some
success with improved CO2 loading capacity, corrosion resistance,
degradation and reduced regeneration costs but with lower absorp-
tion rates [54,6569]. Diisopropanolamine (DIPA) has also been used
due to its high corrosion resistances and lower regeneration costs
though with similar drawbacks [59,61,70]. Sterically hindered amines
like AMP (2-amino-2-methyl-1-propanol) have been tried for CC
since they have high absorption capacity, higher selectivity, corrosion
and degradation resistances, easy regenerability though with low
absorption [64,7174]. Aqueous blends of AMP with DEA and DEA
with MDEA are also reported [75,76].
Piperazine(PZ)/cyclic diamines have been employed due to
their high loading capacity, low regeneration costs and high resis-
tance to corrosion and oxidative and thermal degradation. PZ is more
successful as a promoter due to its rapid formation of carbamates
with CO2. It was employed with MEA, diethylenetriamine (DETA),
and with AMP at various ratios. AMP-PZ blend is reported to be
Table 2
Summary of absorption based carbon capture.

Type Absorbent Reactive Operating CO2 Kinetics/mass transfer Remarks Ref

separator conditions capture (%), AC(kg/kg)
P,T,C,G

Single solvent Ammonia Sieve plate (CC) T:2555 1C C:1014 9599, 1.2 2NH 3 g CO2 g 3 NH 2 COONH 4 sNH2 COONH 4 s Temperature curve has a peak [161] [162]
H 2 Og 3 NH 4 2 CO3 s
(exo-endo)
h i
Spray (CC; pilot) P:0.1; T:2050;C:17 G:3 1020, NA G1
K G aV pH lnYY 12 Y 1
Y 2 KG av 0.17, increases with G and L/G [163]
T
7
MEA Flow (SC) T:1040; C:816; G:210 94, 0.4 C 2 H 4 OHNH 21 CO2g H 2 O1 NH3 regeneration heat 4MEA [161]


2C 2 H 4 OHNH 3aq HCO3aq

B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

2 3
Spray & packed T:25 A:37 G:10.3 100, 00.45 mol/mol hdY i Spray column offers superior CO2 [164] [13] [43]
K G ae 4  G1  5 CO2 ;G
(CC, pilot) dZ absorption than packed column [5764]
P yCO
ynCO HT
2;G
2 3
2

Tray (simulated P:0.1; T:15.2; A:30(w/w); 495, NA   X H2 OZ H CO2 MEAZ X CO2;Z H CO2 H 2 OZ
Theoretical study [103]
CC; pilot) G:0.1 mol/s H CO2;Z 100:152IZ 4 LZ
5

K2CO3 Fixed-bed (Con-O, T:60 G:40 ml/min 99.4, NA NA Reactivity decreases at 40200 1C [102] [93102]
bench scale)
Piperazine Stirred cell (SC, BS) T:42 P:0.032&0.042  100, 0.32 1st order partial reaction occurs promising promoter [165]
PZ CO2 k2 PZH COO

k
1
q

MDEA Batch mode w.r.t. T:25; A:01 G:0.0150.03 99, NA It doesn't polymerize unlike primary & [166]
N C nA a DA k2 C bulk st
B , pseudo-1 order reaction
liquid phase (BS) m3/hr secondary amines
AMP Double stirred cell T:47(ue gas); S:20350 90, NA Optimum L/G ratio(1.6 kg/kg) at reboiler [167] [64] [71
absorber (BS) T:40(solvent); L:28.5 duty 74]
of 3.4 GJ/tCO2; Linear decrease of
temperature with the height of the
desorber column.
3050
Ionic liquids Double stirred cell T:2550; P:0.1;A:0.51.2 99.11at 60 1C, NA k2 3:04  107 exp ; Density and viscosity increases with [168] [105107]
T
(BS) concentration & decreases with
temperature.
is a fast pseudo-rst order regime with
2nd order rate constant.
   
DEAB Packed laminar jet T:25 A:12 495, NA kDEAB 4:01  1013 exp
7527:7 Mass transfer depends on column height & [169] [54]
T
absorber (lab absorbent type. [6569]
scale)
Mixed Solvents MEA blends Packed (CC; pilot) T:2550 A:35 G:100  100, 00.59 K G ae K aminee eAAMP=MEA eB eCxCO2 LD
1e
EC s
eT Blend has [170]
(A1A2) L:2.55 better energy efciency
MEA-NaOH Packed (CC; pilot) A1:1.2; A2: 3 L1:3.829.3; NA, 00.5 C2 H4 OHNH2l CO2g H2 Ol Mass transfer increases with liquid [171]


L2: 3.822.9 T1:25; T2:25 2C2H4OHNH 3aq HCO3aq loading;
50 structured packing performs better
BDA-DEEA Packed (CC, BS) T:40(absorption) T:90 46(HCL), 48(HCC),11 Carbamate & Bicarbamate formations: Theoretical study validated with NMR [172]
(desorption) G: 24.78 m3/h (HCE) than MEA with studies.
5M
BDA CO2 H 2 O2BDACOO
H 3 O BDACOO

CO2 H 2 O2BDACOO22
H 3 OH
DEA-K2CO3 Split ow (CC, T:115 L:63.66 m3/h 99, NA Promoter selection is very critical. It is reversible Amine provides an efcient way of CO2 [173]
bench scale) exothermic reactions CO2 K2CO3 H2O22KHCO3 capture;
AMP-PZ Packed (pilot) L/G:2.9; packing 90,NA Regeneration energy is 3700 kJ/kg CO2 [7784]
height 10 m
PEI-SiO2 Packed (bech L:33.66 m3/h NA,NA qsensible
C p Tmsolution a high absorption efciency, a high [120,121]
mCO2
Alcohol/ scale) desorption
amine/water efciency, and a low regeneration energy

1329
penalty
1330 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
successful in achieving 20% reduction in regeneration energy and
45% in the absorbent circulation rate apart from showing a signicant
improvement in thermal and oxidative degradation resistances
[67,7783]. It has been recently reported by Dash et al., [84] in their
simulation studies that 90% CO2 capture could be achieved employ-
ing 22 wt% AMP8 wt% PZ. Aqueous ammonia has been employed
as a solvent due to its high CC efciency, high absorption capacity,
low regeneration costs, easy availability, ability to remove SO2, NOx
along with CO2 simultaneously and the value added salts that could
be used as fertilizers [43,8590]. Due to their distinct advantages, the
technology has been upgraded to pilot scale [91,92]. Aqueous
potassium carbonate has also been reported as an absorbent for CC
due to its low enthalpy requirements, low cost, less toxicity and high
degradation resistance. To offset its very low mass transfer rate,
promoters like inorganic salts of arsenites, vanadates, borates and
silicates; organics like amines and their derivatives, alkaline amino
acids like arginine and biological enzymes like carbonic anhydrase
have been reported [93102]. Potassium carbonate supported on
MgO is reported to achieve an efciency of 99.4% CO2 [103]. Studies
have also been conducted on tray absorption tower for CO2 capture
with 495% CO2 capture efciency by Mores et al., [104].
In the recent past, imidazolium ion based ionic liquids (ILs) have
been employed for their unique properties viz., non-inammablity
and non-explosivity, high thermal and chemical stabilities, almost
negligible vapor pressure, tunable physico-chemical properties, higher
reaction velocity and selectivity. They are also economical, efcient
and are compatible with membrane technology due to their non-
wettability [105107]. They are also blended with amines to derive the
advantages of both systems [108113]. Besides ILs, binding organic
liquids (BOLs) which too exhibit tunable physico-chemical properties
are being employed as they are highly energy efcient during the
solvent regeneration [114119]. Alcohol/amine/water blends and poly-
ethylenimine (PEI) immobilized on silica (SiO2) support have been
recently reported as novel absorbents for CC [120,121].
2.1.2. Contactors for Absorption
From operation angle, the precooled power plant ue gases enter
the absorption system at near atmospheric pressure. The CO2 lean
absorbent from the stripper is pumped into the absorber in a
countercurrent fashion. CO2 is absorbed to form carbonate or
bicarbonate and other compounds. Since, it is an exothermic reaction,
interstage cooling in contact towers is desirable for maintaining high
absorption efciency. The CO2 rich absorbent exiting the bottom of
the absorber is pumped to the top of the stripper operating at 100
150 1C under the inuence of a thermal swing operation. The reboiler
at the bottom generates stripping steam which meets CO2 rich
absorbent as it ows down the stripper. The temperature swing
reverses the CO2 absorption reaction and returns the same to the gas
phase. The CO2 thus released from the stripper is compressed and
sent for storage [9]. Extensive literature has been reported in the
development of efcient gasliquid contactor congurations, solvent
systems and stripper congurations. The main focus of energy
investigations is to achieve high capture efciency with minimal
energy penalty [122,123].
Various absorber congurations are employed for CO2 absorption
viz., packed bed, bubble column, rotating packed bed and tray towers.
Cousins et al., [124] has dealt with process ow sheet modications for
CO2 absorption to make it more energy efcient by employing
multiple columns in the pre-treatment stage, inter-stage temperature
control to achieve the desired temperatures of 4060 1C for optimal
CO2 absorption, heat integrated stripping to reduce the energy
requirement (by half or one third) in the regeneration process and
use of the split ow process to achieve energy requirements by 50%.
Other retrot options attempted are vapor recompression in the
stripping section, matrix stripping in which number of strippers
operate at different pressures in a matrix pattern and use of the
overall heat integration [69,125133]. The major factors that affect the
CO2 absorption CC by absorption in a packed column are physical
properties of the solvent, liquid and gas ow rates, CO2 partial
pressure/total pressure of the system, temperature, absorbent con-
centration, nature of packing and CO2 loading on the solvent [134].
Among the physical properties, the surface tension of the solvent has
inuence on mass transfer and increased effective packing area [135].
The CO2 partial pressure has a direct inuence on the CC efciency due
to the increase in the driving force for the mass transfer [136138].
Regarding the effect of gas ow rate, clarity is still required [135,138
140]. The liquid ow rate has been found to have a positive impact on
the CO2 capture efciency [135,141,142]. The absorbent concentration
has a direct inuence on CO2 capture efciency, heat of reaction,
temperature and the CO2 vapor pressure [135,138,143]. A high
absorption temperature leads to increase in viscosity, CO2 vapor
pressure and decrease in the solubility of CO2 [139]. In a packed
column, the nature of packing viz., structured or random has a vital
role in the capture efciency. The former provides much superior
performance due to higher geometric surface area per unit volume.
Apart from the nature of packing material, other factors like packing
arrangement, corrugation angle, crimp height can inuence the
absorbed performance [144,145]. Absorption studies have also been
reported employing rotating packed reactor (RPB) using PZ and a
blend of PZ and DETA for 10% CO2 with N2. RPB is found to be better
than PB in terms of enhanced gasliquid contact area and mass
transfer rate and a smaller size for achieving the same capture
efciency [146]. Gas ow rate and scavenger contents are the most
critical parameters inuencing the CC and dissolved oxygen [147].
Bubble column reactors have been reported for CC using ammonia as a
solvent. The contactor geometry (liquid column height to diameter
ratio) along with ammonia concentration and temperature have
positive inuence on the performance while inlet CO2 concentration
and the ue gas rate had negative inuence on the capture efciency
[148]. Recently mini-channel reactor which offers high surface area to
volume ratio has been employed for the absorption of CO2 from its
mixture with N2 using DEA to achieve 100% absorption efciency with
4 times increase in mass transfer coefcient and high specic
interfacial area [149].
2.1.3. Modeling and kinetic studies
Two main approaches are adopted for modeling CO2 absorption
viz., equilibrium stage and rate modeling concepts. The latter is
more extensively employed. Khan et al., [150] validated a rate
based model employing fast second order kinetics for the CO2
MEA system in a packed column considering the enthalpy changes
in both gas and liquid phases. Guo and Zhang [151] and Dash et al.,
[84] employed rate fraction in Aspen Plus for ammonia and AMP-
PZ blended absorbents. Chikukwa et al., [152] reviewed the models
employed for CO2 absorption and stripping using MEA as solvent.
Flue gas composition and ow rate, reboiler duty, CO2 capture
level and L/G ratio have been used for evaluating the dynamic
behavior. Models based on two lm theory have been found to be
more successful in predicting absorber performance as compared
to penetration theory. Software platforms like gPROMS, Aspen
Plus, Aspen HYSYS, ProMAx, Aspen Customer Modeler, Tsweet,
Aspen Plus Dynamics, MATLAB with ODE solver and Simulink have
been employed for the modeling studies [153]. CFD based models
have been employed to understand the hydrodynamic phenom-
enon in absorbers. Sarkar et al., [154] studied the uidized bed
regenerator design employing a multiphase CFD modeling using
solid absorbents under plug ow and well mixed ow conditions.
Sub-grid ltered CFD models have been reported for simulating
ow in larger absorbers besides incorporating desorption kinetics
[155,156]. Recently physical absorption by the rectisol process was
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
comprehensively reviewed by Gatti et al., [157] with respect to
various process congurations, simulation of staged regeneration
and auto-refrigeration via mechanical vapor recompression using
Aspen plus software platform.
Kinetic studies have been conducted by Shen et al., [158] for
absorption of CO2 with aqueous K2CO3 promoted by arginine in
wetted wall column at various temperatures. The kinetics was found
to follow pseudorst order regime with rate constants of 33,641
L/mol s and 85,367 L/mol s at 313 and 325 K respectively with activa-
tion energy of 71.9 kJ/mol. The reaction was reported to follow
zwitterion mechanism. Larachi et al., [159] employed emulsions of
amines (DEA) with ionic liquids for CO2 absorption in a stirred cell
contactor to understand the inuence of various parameters like
amine concentration, temperature, CO2 partial pressure, agitation
speed on CO2 absorption among which agitation speed was found to
have the most vivid impact. The techno economic and scale up aspects
of the post-combustion CC processes were reviewed by Saiprasad and
Raghavan [160]. Table 2 gives the summary of Technological options
for CC in terms of contactor, absorbents employed, CC efciencies
achieved along with relevant kinetic models.
From the above section on absorption, we understand its
critical role in CC and various developments of the technology
has witnessed in terms of development of novel absorbents, like
ILs, BOLs, amine blends, etc. and novel contactors like RPB, mini-
channel reactors for achieving process intensication besides
developing rigorous hydrodynamic and kinetic models to explain
the process effectively. The challenges posed by this technology
are the development of novel green cost-effective solvents to
reduce the regeneration costs and design of efcient contactors
with energy integration and process intensication employed.
2.2. Gassolid adsorption
Adsorption facilitated CC processes are promoted by gassolid
intermolecular forces. The kinetic diameter of molecules present
in ue gases varies between 2.65 and 3.75 with kinetic diameter
of CO2 being 33 . Wide differences exist in their electronic
properties viz., quadruple moment and polarization of gases in
the ue gas. CO2 has a large quadrupole moment of 13.4 
10
40 cm2 contributing to higher adsorptiondesorption efciencies
in the case of meso and micro-porous materials like zeolites,
molecular sieves, carbon nanotubes and metal organic frameworks.
Though a variety of adsorbents have been tried for post-
combustion CC, no adsorption based technology has been employed
on a commercial scale. However, future potential exists for their
commercialization since they have signicant energy savings as
compared to liquid absorbents. Their major challenges lie in
enhancing the thermal efciency of the sorbent materials, minimiz-
ing the physical attrition problems, improving their time on stream
performance and selection of appropriate contactors. It is found that
no absorbent is without technical demerits even though several
potential candidates are endowed with regeneration energies sig-
nicantly lower than the global benchmarks. Pressure, temperature
and electrothermal swings have been employed for effecting
adsorptiondesorption processes driven by physi or chemisorption.
Their rate and effectiveness are dictated by the polarity, surface area,
pore size and spacing of the selected adsorbents.
2.2.1. Pressure, thermal and electrothermal swings
2.2.1.1. Pressure and vacuum swing adsorption (PVSA). It was intro-
duced in early seventies by Turnock et al., [174]. Kao et al., [175]
employed PSA for signicant improvement in the selectivity of a
membrane possess for separations of a heliummethane mixture.
Dabrowski et al., [176] reviewed theoretical and experimental
applications of adsorption technology. VPSA technology is
1331
conventionally performed at higher pressures in feed (adsorption)
and atmospheric pressure in regeneration in PSA or less than
atmospheric pressure in VSA. Its operation is periodic (swings) in
nature. It is used for removal of bulk contaminants at comparably
higher concentrations. Simulation studies employing a two stage V-
PSA (Vacuum PSA) process with Zeolite 5A as adsorbent have been
recently reported by Zhen Liu et al., [177] to achieve a CO2 purity of
96% in a two bed and 70% purity for single bed process for 15% CO2
85%N2 mixture. Lopes et al., [178] and Grande [159] have reported
on a 10 steps PSA units with activated carbon adsorbent as well as
engineering approaches of PSA performance. Vacuum swing
adsorption has also been reported employing multilayered
adsorption system of 13X zeolite and activated alumina, F200 and
silica based Sorbead as protective pre-layers. Langmuir extended
BET and multi-molecular sorption equations for the simulation
studies to achieve 91% CO2 purity [179]. VSA has also been
employed to study the performance of the adsorbent of UiO66
(metal organic framework) for the capture of CO2 from dry and wet
ue gas containing 15% CO2. Around 70% capture efciency could be
achieved upto 50 cycles with a six step VSA cycle. Water vapor in
the ue gas has a negative inuence on the CC [180]. Hedin et al.,
reviewed the use of various micro- and mesoporous physical
sorbents and amine modied mesoporous silica using tem-
perature or vacuum swing adsorption and stressed the need for
more effective adsorbents and the energy integration in power
plants for better thermodynamic efciency [181]. Danga et al., [182]
employed the Dual Piston pressure swing adsorption (DP-PSA)
system for the characterization of novel adsorbents for Zeolite 13X
and isothermal model for cycle times greater than 10 s with
pressure ratios of 23. Gas ow pattern studies on the multistep
PSA process have been performed by Nathalie Casas et al., [183,184].
Recently Su et al., [185] reported the use of dual column
temperature/vacuum swing adsorption using amine loaded carbon
nanotubes as adsorbents to achieve 67% CO2 concentrations.
2.2.1.2. Temperature swing adsorption (TSA). The TSA is carried out
at moderate temperatures of around 40 1C and desorption occurs
at around 120 1C. It is used for the removal of contaminants at low
concentrations. Both TSA and PSA were commercialized in the
early sixties and were subsequently improved with novel,
effective, stable and recyclable adsorbents. While the con-
ventional adsorbents used for TSA and PSA were silica gel, activated
alumina, metal oxides and zeolites, the novel ones are metal organic
frameworks, activated carbon, graphite and porous polymers such as
honeycomb monolith [186]. The major drawbacks of TSA over PSA are
longer desorption times, higher energy requirements and rapid
adsorbent deactivation due to coking at high temperatures [187].
Pilot scale tests (1 kW) have been reported using carbon and amine
based adsorbents in a uidized bed contactor with TSA as the
regeneration strategy [188]. Veselovskaya et al., [189] employed a
composite K2CO3/Al2CO3 adsorbent to capture CO2 from air using TSA
for regeneration. It has been observed that with an increase in
regeneration temperatures from 150200 1C to 250300 1C increases
CO2 capture is increased upto 5 wt% and that the composite materials
exhibited high stability upto 80 cycles. Hedin et al., [181] identied
adsorbents suitable for rapid TSA viz., mesoporous materials like
zeolites, carbon molecular sieves, metal organic frameworks; other
microporous physi-sorbents like MCM41, silica and amine modied
mesoporous silica.
2.2.1.3. Electrothermal swing adsorption (ESA). It employs Joule
effect by passing electricity through a packed column [190].
Grande et al., [190,191] employed activated carbon honeycomb
monolith as an adsorbent separation of CO2 in low concentrations
in the ue gas streams. The desorption is not through resistive
1332 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
heating of the matrix, but through a direct electrical effect con-
tribution sorbatesorbent interactions [187,192]. The adsorbent to
be employed in this process has to be conducting to promote
electrical swing [187]. ESA is more economical than TSA and PSA
with suitable adsorbents like activated carbon ber materials are
employed. More lab and pilot studies have to be done on ESA
before its commercialization [193].
Pevida et al., [194] examined various regeneration strategies
employing TSA, VSA and VTSA employing activated carbon as an
adsorbent to capture CO2 from CO2N2 mixture. They found that
for single bed cycle congurations, the productivity and CO2
recovery followed the order viz., TSAoVSAoVTSA for achieving
a maximum CO2 recovery of 97%.
2.2.2. Adsorbents and their selection
An ideal adsorbent should have high CO2 capture capacity, easy
regenerability, stability, large pore dimensions and recyclability.
Carbon ber monoliths (poly acrylo nitrile (PAN) and Viscose
Rayon) and activated carbons are reported for ESA and PSA
[192,193,195]. Table 2 highlights the efciencies of various adsorp-
tion for CO2 capture. High temperature adsorbents like calcium
chabazite, 13X zeolites and K2CO3 based HTC zeolite, hydrotalcite-
like (clay minerals) compounds containing nickel and iron cations
with and without boehmite alumina have been employed as
adsorbents. Their adsorption capacity is found to be 2.5 mmol/g
and exhibited high thermal stability and activity over a wide range
of temperatures [196]. Pilot test results have been reported by
Sjostrom et al., [188] for hundred adsorbents in a xed bed
contactor. Amine and carbon based adsorbents were tried the
former exhibited high adsorption capacity whereas the latter has
shown the higher cyclic stability though with low CC capacity
[186]. Zeolite 5A and multilayered zeolite 13X with pre-layers of
F200 and silica based Sorbead WS have been employed for
adsorption of CO2 from a mixture of CO2N2 using VPSA regeneration
in a multi-bed column [177,179]. Nanoporous materials (1100 nm)
like zeolites, activated carbon, nano-hollow structured material
(110 nm) like carbon nanotubes, CaO nanopods and nanocrystal-
line particles like lithium silicate, Li2ZrO3 have been reported.
Future research efforts need to be directed towards the develop-
ment of novel and cost effective synthesis protocols followed by
scale-up [122]. Recently, amine modied TiO2 nanotubes, TEPA
modied metal organic frameworks (Mg-MOF-74) have exhibited
the highest adsorption capacity of 167.64 mg/g with good cyclic
stability [185,197,198]. Recently polyethyleneimine (PEI) incorpo-
rated metal-organic framework (MOF) adsorbents were able to
achieve selectivity of CO2 over N2 upto 770 at 25 1C and 1200 at
50 1C [199]. Its adsorption capacity for ue gas with CO2 concen-
tration of 15 vol% and 400 ppm was found to be 181 mg/g and
99.3 mg/g at 25 1C respectively [200]. To reduce the cost of
adsorbents, industrial wastes like slags, y ash, lter cakes,
foundry sands, dusts from cyclone, furnace and cement kiln are
employed for CC [201,202]. Among these, y ash derived adsor-
bents have shown good potential [203]. Alkaline paper mill waste
was also employed [204].
Various carbon based materials have been employed as adsor-
bents with appropriate modications. PEI loaded mesoporous
carbons with 65% loading have shown a sorption capacity of
4.82 mmol-CO2/g-sorbent [205]. Pitch based nanoporous carbons
activated with KOH showed good potential for CC with 203 mg/g
sorption [206]. The carbons doped with sulfur and N from a urea
formaldehyde resin have shown adsorption capacity of 8 mmol/g
at 0.9 MPa in case of former and 3.21 mmol/g in case of latter
with KOH activation [207,208]. Activated alumina modied with
sodium hydroxide (52 mg/g) and diethanolamine (56 mg/g); amine
grafted silica aerogels (2.61 mmol/g) and PEI immobilized on silica
(3.5 mmol/g) have also been reported [209212]. Linga et al., [213]
employed porous silica sand and silica gel as adsorbent in the
clathrate hydrate process. The former was found to perform better
than the latter in achieving higher conversions to hydrates. Of late,
the novel biomass based carbon adsorbents have been developed as
a greener option with advantages of low cost, high selectivity, easy
regenerability and high stability in humid conditions. Olive stones
and almond shells have been reported as used carbon adsorbents
with high adsorption capacity (4.8 mmol/g at 101 kPa and 0 1C)
[214]. Macadamia nut shell based carbon composites have been
used for Post-Combustion CC with 35% better efciency [215].
Recently Gao et al., [216] and Younesi et al., [217] have employed
bio-char from sugarcane bagasse and hickory wood and eucalyptus
wood based activated carbon modied by ammonia solution with
air adsorption of 73.55 mg/g at 600 1C. For selective adsorption of
CO2 over N2, CH4, CO and O2, porous synthetic hectorites (clay type
minerals made from LiF, MgO, SiO2) are employed with an adsorp-
tion capacity of 22.8 cm3/g and 18.7 cm3/g with and without
modiers respectively [218].
To summarize the developments, the microporous and meso-
porous solid adsorbents have the highest potential for large scale
CO2 capture. The SiO2/Al2O3 ratio and incorporation of cations in
their structure can enhance their adsorption capacity. The impreg-
nation of polyethyleneimine into MCM-41 is reported to enhance
CO2 adsorption 24 times. The selectivity and adsorption capacity
achieved so far are not attractive enough for large scale post-
combustion CO2 capture. Metal organic frameworks (MOF), which
are endowed with carefully sized cavities, have high CO2 capture
potential, low energy consumption for desorption and higher
impurity tolerance. On a comparative basis, the active area per
unit weight of MOFs is around 15004500 (m2/gm) as compared
to 4001000 (m2/gm) for activated carbon and 1500 m2/gm for
zeolites. Supporting liquid absorbents on porous solid substrates is
gaining momentum, the focus is on minimizing thermal instabil-
ities, fouling tendencies and SO2 induced degradations.
2.2.3. Contactors for adsorption
Fixed bed (single or multiple columns), normal, bubbling and
ultra-sound assisted uidized beds and moving bed contactors are
used for adsorption due to their relatively simple operation and
design. The critical parameters that affect the functioning of the
xed bed contactors are CO2 concentration in the feed, tempera-
ture, feed ow rate and the amount of the adsorbent used. Auta et
al., [209] observed an optimal CO2 at which adsorption capacity is
maximum (52 mm/g at 15%) since the available active sites would
become a limiting factor beyond certain concentration of the
adsorbate molecules. Adsorption capacity decreases with tempera-
ture. Low feed ow rate has a negative inuence on adsorption
capacity due to long residence times. The xed bed contactors
have been employed for the clathrate hydrate process (HBGS) for
pre-combustion CC due to lower power requirement and the
larger surface area available [213]. Moving bed adsorption (MBA)
with heat integration has been used for post-combustion CC with
one adsorption and two desorption beds [219]. The heat integra-
tion between adsorption and desorption beds contributes to
energy savings. A CO2 purity of 97%, recovery of 80% with degree
of heat integration of 57% have been achieved. Lab scale bubbling
uidized bed contactors have been employed by Sun et al., [220]
using PEI based silica adsorbent. An adsorption capacity of 11 wt/
wt% could be achieved over 60 cycles. The N2 was employed as
stripping gas which could be replaced with steam. The regenera-
tion heat was estimated to be 2360 kJ/mol which is signicantly
lower than the MEA scrubbing process. Recently Yong-Ki Park
et al., [221] employed the multi-stage uidized bed process with
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350 1333

inter-stage heat integration for improved energy efcacy using temperature is thermally integrated with a regenerator at lower
sorbents like K2CO3, Na2CO3 modied MgO and Li4SiO4. Each stage temperatures for necessary thermal balance. It is estimated that
contains an absorber, a regenerator and heat exchanger for intra- for a three stage process, a net electrical efciency of 32.8% was
stage heat recovery. Between adjacent stages, an absorber at high achieved in power plant of 500 MW capacity.

Table 3
Summary of adsorption based carbon capture.

Adsorbent Reactive Operating conditions CO2 capture Kinetics/mass transfer Remarks Ref
separator P,T,C,G (%), Ad-C
(gCO2/gads)

rayon HCM PBR (TSA) SA: 1873.9; AT:950; 97, 0.2 C

vZ
ch C
Dax ZC2
ap 1
mm kf C
C n
2
Ad-C is twice that of [232]
t
CT:650; FRR:0.5 conventional activated [243]
Langmuir Adsorption isotherm adopted
carbon & 1.5 times 4 ZIF.
 ai
Activated PBR(ESA,4&6- T:24; P:0.1; ICC:4.51; 4step cycle: 99.6,NA &21.7 % qni qn Decrease in electrical [236]
qmax;i K eq;i yi P 1
q i ;
carbon- step Cycle, LS) (purity) max;i
efciency with thermal
HCM load.
multi-site Langmuir model, energy saving 45 times [244]
enthalpy 25kJ/mole in 6step cycle
0.431; Md:99.2; 6step cycle : 81.4,NA 150 1C reaches in 45s
Mfco2:0.0451 &46.6 %(purity) at12V
Fly ash PBR(TSA,LS) T:70; P:0.11; St: 24 h 4.5 at 85 1C CO2 2RR0 NH2RR0 NCOO
RR0 NH 2 Higher Ad-C at lower [245]
PEI PEG CO2 2H2 O RR0 NCOO
22HCO3
temperature
RR0 NH 2 -higher performance with
lower m.wt polymers.
p p
ZX & K2CO3 PBR(VPSA,LS) T:120250; P:0.003; 95, NA & 97.2%(purity) p C q Operational Simplicity of [246]
s kC
C at 70% adiabatic
promoted 8x12 mesh; reactor, reduced cycle time [247]
compression.
HTC and Small bed sizing factor.
ZX MEA , PBR(PSA,LS) P:0.1;T:75; ICC:15; NA,0.0161(ZX); 2RNH2 CO2 -RNHCOO
RNH3 hybrid absorption- [248]
ZX IPA SA:14.9; NA, 0.01998(MEA); RNHCOO
H 2 O-RNH 2 HCO3
: adsorption [249]
:0.044 NA, 0.02278(IPA)
NPC10 PBR(TSA, LS) T:25,P:0.1, SA:639 NA, 0.041 Langmuir adsorption isotherm Selectivity over N2 is 425:1 [250]
Co-MOF-74 PBR(PSA, LS) SA:1314(MS);SA:1327 NA,0.288(MS)-CO2 Macropore channel density Synthesis with microwave is [251]
(MS) (STS) o 10 is for optimum performance. faster than conventional [252]
NA, 0.21(STS)-CO2 Molecular and Knudsen diffusion are heating.
NA,0.466(MS) -H2O chosen.
Co-MOF-74 Tms:1; Tsts:12 NA,0.605(STS)-H2O
(STS)
UiO-66-MOF PBR(VSA, LS) T:55; P:0.2; ICC:15; 6070,NA, 60%(purity) throughput TPD p gas_production  cycle 25% capacity decrease due [253]
cyclemads day
SA: 1260;; WC to water vapor after 50 [246]
Bd 0.45; Lg:0.26; specif ic productivity k cycles. [254]

Ac:900s; Dc:1620s
Activated PBR(1bed,3step, T: 60, Lg:50, P:0.113, 69.5,NA Dual-site Langmuir equation has been Increased energy penalty [253]
carbon VSA, LS) PVP 3, , Trpt:3;SA adopted and variation in
  2 
:921.7,PV:0.37, Q n
R ln1=T
lnP
RTP P hydrophobic nature of
n T n
Tads:35, Bd:0.493, activated carbon due to
ICC:11.2, TDes:100, water presence.
Vf:44; H2O vapor:4.6
mol%
ZX-APG, PBR(3-bed,8- T:35; P: 0.0070.008 8595, NA, 7382% CO2 Langmuir adsorption isotherm is adopted Higher capital cost with an [255]
5A zeolite step, VPSA , LS) purity energy consumption of
1.792.14MJ/kg of CO2
BZX, NaX, KX PBR(PSA, LS) Lg:00.1,Dp:0.50.75, NA, 0.21,912 Adsorption kinetics model has been Adsorption capacity [256]
& CaX SA: 931; x investigated by the Zero-Length Column increases with cation radius [257]
Crushing technique (ZLC) Ca2 o Na oK
strength:0.46 MPa
Xpth: 0.012
ZX MBA(PSA, LS) Bd:0.65,Cs :1.07, 80,NA, 97%purity Extended Langmuir Isotherm was used 54.4% of energy regenerated [258]
Dp:3420, :0.31, from Adsorber.
ks :0.275
Bed dimensions
(m): Xpth:0.012
L :1.5, W: 1.5;
Nm:36, 2b:0.03,
FAC SAFB(LS) SPL:140; Vf :1.5; 90,NA Langmuir isotherm is adopted, Increase of 1.78 MJ/kgCO2 than that of [259]
SA:1060 temperature is very small (23 K). amine based adsorption of [260]
ICC :10; Frequency 4.8 MJ/kgCO2
:80Hz;
Amine silica PBR(LS) Silane: silica 2.61 mmol/g with 100% CO2 N2 adsorption isotherm Adsorption capacity of 1.76 [211]
aerogels ratio 2:1 at 1 bar and 25 C, NA mmol/g
T 95 1C
TEPA-Mg- PBR(LS) Regeneration temp is 44.9 wt%, 8.31 mmol CO2/g N2 adsorptiondesorption isotherm Increase in Desorption [189]
MOF-74 250300 1C absorbent,NA temperatures [197,1-
98]
1334 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
2.2.4. Kinetic and modeling studies
Employ pseudorst and second order kinetics, intra-particle
diffusion models have been employed to simulate the adsorption
process. Yusup et al., [222] found that pseudo-second order model
tted the data best and the activation energy for the physisorption
process was found to be less than 42 kJ/mol. Erto et al., [223] have
investigated the kinetic, thermodynamic and regenerative studies
on adsorption using synthetic activated carbon (F50 from coal tar
pitch). They also found that the adsorption process is reversible in
nature with optimal desorption temperature at 100 1C being the
controlling parameter. The adsorption rate was found to increase
with inlet CO2 concentration and temperature. The sorbent was
found to be stable even after the 15 adsorptiondesorption cycles.
CFD modeling was employed to study the hydrodynamics and
adsorption process. Ryan al. [224] have tried various multi-phase
models and found that EulerianLagrangian model (FLUENT) has
successfully simulated the uidized bed contactor performance
with silica-supported amine sorbent. Daud et al., [225] have
various mathematical models to explain the complex phenomena
associated with CC in a xed bed contactors. The adsorption
equilibrium relationship can be explained by LangmuirFreun-
dlich, Ideal adsorbed solution theory (IAST), extended Langmuir
Freundlich, O'BrienMyers, multisite Langmuir, Virial, Toth and
dual site Langmuir isotherms mostly assuming plug or axial
dispersed ow [226242].
Table 3 summarizes the engineering aspects of the adsorption
process in terms of nature of adsorbents, contactors, mode of
operation, operating and critical parameters besides kinetic aspects.
Like absorption, adsorption is also a very established technol-
ogy for gassolid operations. It has been successfully employed for
both pre- and post-combustion carbon capture and signicant
improvements have been done in the identication of novel and
cost-effective adsorbents like nano-materials, biomass materials
and those from industrial wastes. To reduce the cost involved in
regeneration, a combination of vacuum and thermal swing adsorp-
tion cycles showed great potential. Many models have been
identied to explain the adsorptiondesorption processes among
which modied Langmuir isotherm was the most popular. The
contactors being employed for adsorption based CC witnessed
great improvements like multistage-uidized bed with energy
integration to reduce energy consumption signicantly.
2.3. Membrane technology
2.3.1. Membrane separation and membrane materials
The absorption adsorption processes for CC require contacting
towers of large diameter (1820 m) and length (2530 m). Mem-
branes with as much as 1000 times more surface area per unit
volume are much more effective in minimizing the size of contact
towers. An effective membrane system for CC has to be endowed
with high adsorption capacity without CO2 penetration into the
bulk, high reversibility, highly selective to CO2 with insignicant
sorption capacity to N2, CH4, H2 and others in ue gas, high
resistance to ue gas poisoning by Sox, NOx and H2S, ease of
fabrication, high stability at elevated temperatures and ability to
perform efciently at lower thicknesses.
Membrane technologies can be utilized both for pre-
combustion and post-combustion CC. In case of the latter, mem-
brane contactor has been successfully employed for gasliquid
absorption while they can be used for separation of CO2 from the
ue gases employing a wide variety of membrane materials.
Membrane separation is developing into a process intensication
tool for reactive absorption processes. Ceramic membrane con-
tactors are employed in cases where signicant absorption could
not be achieved with conventional absorbers.
CO2 permeation increases when there is a chemical afnity
with specic molecular groups present in the membrane. Several
CO2 selective membranes have been reported for CC from ue
gases. The Department of Energy, USA reviewed the membrane
development for CC, their stability, performance, interrelationship
of their properties and mechanisms applicable in different CO2
selective separation processes [261]. Cost savings upto 35% have
been reported to be achieved in a coal red power plant operated
under vacuum conditions [262264]. Membranes provide semi-
permeable barriers that separate substances by accordingly, three
general transport mechanisms viz., Knudsen-diffusion, solution
diffusion, adsorptiondiffusion, molecular sieving and ionic trans-
port mechanisms. They are available in various forms viz., organic
(polymeric) or inorganic (carbon, zeolite, ceramic or metallic) in
porous to nonporous forms. Membranes act as lters to separate
one or more gases from a feed mixture and generate a specic gas
rich permeate [43]. They offer various advantages like viz., no
ooding at high ow rates, no unloading at low ow rates [265],
high surface area per unit contact volume, independent control of gas
and liquid ow rates, compactness and scalability. The advantages
outweigh their fouling problem [266]. From operational point of
view they offer low maintenance cost with no moving parts,
relatively low capital cost and small physical footprint which makes
it favorable for platform and less energy intensive operations.
Cahn and Li [267] reviewed the liquid membrane process for
the separation of hexane from heptane. Ward III et al., [268]
reported silicone/polycarbonate membranes for on-board genera-
tion of nitrogen enriched air used as an inert gas. Karos and
Flemming [269] reviewed on material selection, membrane synth-
esis, and modular concepts in their scale-up and system charac-
teristics. Armor [270] highlighted the utility of catalytic inorganic
membrane reactors for renery products. Corti et al., [271] devel-
oped a methodology for the CO2 separation from membrane
reformed synthesis gas. Membrane based pre-combustion process
of integrated gasication combined cycle has been critically
analyzed by Colin a Scholes [272]. The major material develop-
ment challenges in membrane processes would be membrane
porosity and thickness, non-wetting characteristics, hydrophobi-
city, non-polar nature and pore size distribution. The critical
parameters are ue gas composition, temperature and ow rate,
high parametric sensitivity, selectivity to be achieved, need of high
quality energy, etc. [273].
2.3.1.1. Microporous membranes. Generally inorganic membranes
and facilitated transport membranes fall under this category [261].
The working principle of microporous membranes is indicated in
Fig. 4. The membrane support has an asymmetric porous structure
(except palladium-based membranes) to minimize ow resistance
[274]. They can be congured as modules of hollow-bres or at
plates. The different types of membranes employed CO2 capture
are given in Fig. 5. Hollow-ber polypropylene membrane
contactors are reported to give 97% capture efciency with
standard 3M MEA solutions [275]. The at sheet membrane
contactor was found to be better than that of hollow ber
Fig. 4. Microporous membran.
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
Fig. 5. Membranes for CO2 capture.
Fig. 6. Dense polymer membrane.
membrane contactors provide better CO2 absorption ux as
compared to hollow ber membrane contactors [276]. Various
membrane materials have been employed for above congurations
viz., PVDF (polyvinylidineuoride), PP (polypropylene), PTFE
(polytetrauoroethylene), PEI (polyetherimide), PSf (polysulfone)
and PMP (polymethylpentene) Teon-AF [277]. Among these, PP is
economical but has low chemical resistance but PVDF and PTFE
though chemically resistant are more expensive. Hence, the need
is to develop novel cost effective membrane materials and solvent
systems that facilitate good CO2 capture at low cost. Gas absorp-
tion occurs in the gas lled membrane pores. The membrane
support plays a key role in enhancing the system performance
with marginal inuence on selectivity. Hyper-cross-inked
networks consisting of aromatic rings connected to polymeric
matrices have been reported to form porous networks.
Modication of the network surface could be achieved through
functionalization of hyper-cross-linked layers [278]. Porous
inorganic membranes are high temperature CC processes. The
mechanisms of CO2 separation in inorganic membranes are based
on adsorption selectivity and surface diffusion with relatively low
separation factors. Microporous silica membranes containing
amine functional groups have been reported for CO2 separation
from ue gases [279]. The CO2 capture can also be achieved with
molecular sieve membranes in which CO2 separation occurs on
account of size discrimination within the channels of its porous
structure.
2.3.1.2. Dense membranes. CO2 permeation involves selective
passage of gas molecules through a dense membrane (generally
polymeric). Its permeability and selectivity would be critical
parameters in the process optimization. Their working principle
is given in Fig. 6. A solutiondiffusion or a molecular sieving
mechanism explains the process. Knudsen-diffusion mechanism
has also been reported to conform to this system. Dense polymeric
membranes are successfully used in CC due to their high
permeability and ux achieved [280]. Various materials viz., Tf2N,
ceramic, ceramic composite, PDMS (polydimethy siloxane), DMS
1335
Fig. 7. Supported liquid membran.
(dimethylsiloxane), PSf, Pebax, silicaalumina, polyuoroaniline
uoroaniline copolymer, zeolite Y, polyamide-imide, PES, PPO
(polypropylene oxide), PVAm (polyvinylamine), CNT (carbon
nanotube), POX (polyaryloxyphosphazene)-PDMS crosslinked, TM
(tetramethyl)-PSf, HF-PSf, imidazolium, LDPE (low density
polyethylene), PEEK (polyetherether ketone), PBI (polybenzimi-
dazole), polyurethane, carbon molecular sieves, etc. are employed
[278]. Wang et al., [281] achieved high CC with selectivities of above
100 and permeability of 743 Barrer (1 Barrer7.5  10
11 cm3 (STP)
cm/cm2 s kPa) at 10 bar employing hybrid membrane made of
Pebax-PEG-MWCNT (multiwalled carbon nano-tube). Mixed
matrix membranes of polyvinylalcohol containing amines with
MWCNTs dispersed as mechanical reinforcing llers demonstrated
high stability for gas separation at high pressures upto 1.5 MPa.
Selectivities and permeabilities of 43 and 836 Barrers have been
achieved even at such high pressures [282]. Marono et al., [283]
developed a novel hybrid membrane system based on potassium
carbonate doped hydrotalcite-catalyst, for pre-combustion CC and
H2 production.
2.3.1.3. Supported liquid membranes (SLM). In this system, the
liquid is dispersed on a porous or non-porous support. The CO2
in the ue gas is physically or chemically absorbed into the liquid
and passes through the membrane support. Viscosity of the liquid
is found to play a key role in the system design and the
performance. The SLM working is demonstrated in Fig. 7 below.
Typical examples are TEG liquid membranes modied by Na-Y
nano-zeolites, SLM with uoroalkyl-functionalized RTILs, DEA
supported on polyvinyl alcohol, ionic liquids [hmim][Tf2N],
[emim][CF3SO3], [omim][PF6], [H2NC3H6mim][Tf2N], enzyme of
carbonic anhydrase, etc. supported on polymer, all ionic ionic
liquids to be put together. Ionic liquids of [emim][BF4], [bmim]
[BF4], [hmim][BF4], [bmim][PF6], [bmim][Tf2N], [emim][Tf2N]
supported on polymer or PVDF, [bmim] [N(CN)2] [emim][B(CN4)],
etc. supported on PES, etc. [242]. Ionic liquids are used to eliminate
1336 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

the solvent evaporation step and as to achieve higher stability
(2012) [122]. Selection of the support was found to have marginal
inuence on the selectivity but it was found to be crucial in
determining the stability of the system. SLM is an upcoming
technology yet to be commercialized at an industrial scale
though promising results have been reported at lab scale
[273,284,285]. Fig. 7 shows the variety of membrane materials
employed for CC.
2.3.2. Membrane contactors and modeling studies
Packed columns have been the most commonly employed
contactors for membrane based CC. The critical design parameters
for scale-up are pressure drop, temperature and water condensa-
tion effects, ow rates and dispersion effects of gas mixture and
solvents and mechanical stability. An average volumetric CO2
absorption capacity of 1 mol/m3 s can be taken as a baseline
performance of packed columns to assess the intensication
effects of membrane contactors [286]. Favre et al., [287] found
that for a membrane contactor, a minimum effective mass transfer
coefcient of 2  10
3 m/s is required for achieving a condent
scale-up. For a hollow ber conguration, the external diameter
and thickness of membrane material are 0.001 m and 100 microns
respectively for a module length between 0.1 and 1 m.
Some interesting modeling studies have been reported. They
include modeling of a two stage contactor for CO2 separation from
a multicomponent gas mixture [288] and multi-stage cross and
counter-current membrane contactor for CC with various process
intensication and integration options with MEA as solvent [289].
Favre et al., [277] compared the performance of membrane
contactors employing 1D resistance in series and, 1D and 2D
convection-diffusion models for CO2 capture with MEA as solvent.
A 2D CFD model was employed to predict CO2 capture phenom-
enon using PTFE and dense composite membranes. A 2D CFD
model was employed [290] to predict CC phenomenon using AMP
PZ blended solvent and nanoporous membrane. Rode et al., [291]
compared the simulation results with a 1D transport model for
variable gas and liquid mass transfer resistances and a 2D model
considering convection, diffusion and reaction contributors for a
hallow ber membrane system with MEA as solvent. The potential
of N2 selective membrane for post-combustion CC was examined
[292] and optimization of energy consumption, membrane surface
area and energy consumption. Very recently a simulation model
was developed for CO2 transport through a zeolite membrane and
to understand the diffusion phenomenon [293]. Table 4 gives an
overview of membranes based CC w.r.t the types of membranes
employed, critical process parameters and major ndings of the
kinetic studies with challenges highlighted.

Table 4
Summary of cryogenic based carbon capture.

Process Membrane Reactive Operating parameters Kinetics/mass transfer Challenges Remarks Ref
separator

NDC Micro- Hollow P,T, Pore size and of Reaction kinetics depends on Wetting of the Membrane-solvent combination & [43]
porous Fiber and the membrane- solvent. membrane wetting are critical at high reaction
Membranes Flat- membrane wettability rates.
Sheet
Liquid ow area Pore diffusion depends on Limited long term High temp improves absorption. [276]
membrane support. stability & volatility of
solvent
Gas ow area Ko is controlled by the liquid Presence of other 20% higher performance in counter- [278]
lm resistance even at elevated compounds in the gas current mode than in co-current.
pressures. stream
Packing factor Ko can be given by Graetz Compatibility of Flat sheet is better than hallow [294
Leveque solution membrane and solvent. ber membrane. 296]
1
1
kmgd:d
0
kH:d 0 [313]
Koverall kg lm l :di :E

GP Dense Hollow S-P,T,P, La, Pressure Solution-diffusion, Knudsen Lower selectivity at Higher gas permeability is possible [43]
membranes ber and ratio of the permeate diffusion and molecular sieve higher permeability. with SPM.
Flat- side to the feed side, effect are a few mechanisms.
Sheet Pore size and porosity
Fick's law to govern gas Development of Membrane thickness affects the gas [297,298]
diffusion: novel, cheap and ux.
optimally selective
membranes is essential
Low driving force Plasticization effects should be [278]
after industrial scale-up. considered.
   
J i Pli P f :X i
P p :yi Dl i C i;f
C i;p Pre-Combustion High selectivity, permeability need [280
membranes were not to be addressed. 283]
proven

SLM Liquid in Flat T,P, VVIS, La ,Ga The overall mass transfer Stability of the Carriers and appropriate anion- [254]
the pores of Sheet coefcient, membrane reduces due cation pairs can enhance selectivity.
membrane only to solvent wash-out
H2/CO2 selectivity 1
1
kmgd:d
0
kH:d 0 Viscosity issues arise, The stability, permeability and [299]
Koverall kg lm l :di :E
and long-term stability though ionic liquids give selectivity can be improved by
at high T (400 1C) and P good capture changing the anion and cation
(950 psi). efciencies. composition of the ionic liquid used as
liquid phase.
Industrial scale [278]
literature is not available
Scale-up extreme [281
conditions and long- 283]
term stability tests are
needed for
commercialization.
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
Membrane technology is successfully employed for CO2 separa-
tion from ue gases and as a contacting medium in absorp-
tion based CC. The critical parameters of any membrane based
technology are selectivity and permeability and various novel
membrane like mixed matrix, ionic liquids based on polymeric
support are developed and used successfully in CC. Further
research needs to be focused in making this technology suitable
for large scale deployment.
3. Chemical looping combustion (CLC)
It is a promising energy efcient clean technology developed for
CC where dilution of CO2 with ue gases is minimized. It is a
ameless technology with low NOx formations. It can be treated as a
second generation technology for oxy-fuel combustion based on a
thermo-chemical capture process as shown in Fig. 8. The CLC is a
two-step cyclic process in which the fuel (gas/liquid/solid) is burnt in
the presence of metal oxides available as oxygen carriers in a fuel
reactor (FR). The reduced metal oxides are then oxidized in an air
reactor (AR). These metal oxides are again re-fed to the FR to
complete the loop. The notable feature of this process is its inherent
CC without CO2 separation. The absence of direct mixing of combus-
tion air with the fuel makes it highly energy efcient (zero energy
penalty for CO2 separation from H2O in ue gas mixture). Also, CO2
produced is not diluted with either N2 or O2. Oxygen carriers demand
a higher particle residence time for the reduction reaction than for
the oxidation [300,301]. The ameless nature along with its low NOx
formations at lower temperatures and more importantly its inherent
CO2 separation by condensation of water with minimum energy
penalty are the major advantages of this technology [302304]. The
block diagram of the CLC process is given in Fig. 9 below with the
working principle and the reactions involved.
Air reactor: MxOy
1 0.5O2-MxOy.
Fuel reactor: (2n m)MxOy CnH2m-(2n m)MxOy
1 mH2O
nCO2.
Fig. 8. Chronology of oxy-fuel combustion technology development.
Fig. 9. Schematic diagram of CLC.
1337
The net reaction of the CLC: CnHm (2n m) O2-n CO2
mH2Oheat.
CLOU (CLOU) is the 3rd generation technology of oxy-fuel
combustion which is a slight modication in the CLC process but
with same working principle. This concept was rst developed by
Lewis et al., [305] in early fties and was re-discovered by
Mattisson et al., in 2009 [306,307]. In CLOU, an oxygen carrier
such as CuO/Cu2O or MnO2/Mn3O4 releases gas-phase oxygen in
the fuel reactor and acts as an oxidizing agent in the air reactor. It
is reported to give improved performance with solid fuels (100%
capture efciency) at a faster rate and avoids char formation.
Various mixed metal oxide combinations, their synthesis protocols
and operating temperatures associated with CLOU are reviewed by
Mattisson et al., [308]. The enthalpy values of various metal oxides
employed in the CLOU process have been reported [309]. Rydn et
al., [310] employed a combination of manganese and calcium
oxides. The CLOU technology has the potential to signicantly
reduce the residence time, reactor size and the complexity in CC.
Signicant research efforts are being made in recent times in the
development of novel metal oxides, wide variety of fuels, reactor
congurations with various energy integration options to under-
stand the kinetics, reactor design and hydrodynamics aspects.
3.1. Signicant developments
Signicant developments in CLC have taken place in terms of
oxygen carriers, fuels and reactor congurations during the past two
decades [311316]. Solid, liquid and gaseous fuels have been most
extensively used. The gaseous fuels like syngas, natural gas, renery
gas, biogas, etc. have been employed in CLC. The critical issues of
gaseous fuels are due to the presence of sulfur and light hydrocarbon
impurities. They are also responsible for the reduction of the
reactivity of the metal oxides and CO2 concentration in the exit
stream. The selection of appropriate thermodynamically suitable
metal oxides and the reactor conguration are crucial for effective
operation [103,317]. CLC using solid fuels (coal, petroleum coke, solid
wastes, biomass, etc.) is being widely used in the recent past and
fossil fuels like coal will remain the main energy source in future too.
The mechanism of solid fuel combustion follows a two-step process
of gasication of solid fuel to form CO and H2 which then undergoes
combustion. Another approach is the direct combustion of solid fuel
with in-situ gasication by CO2/H2O [318320]. The sulfur content in
the fuel is a critical factor for solid fuels too and it can be tackled
by integrating a desulfurizing unit along with the CLC reactor
system besides selecting robust oxygen carriers that are sulfur
resistant [321]. A recent review on solid fuel based CLC shows that
high energy efciency can be obtained with appropriate contactor
design like ilmenite and mixed metal oxides have high reactivity,
low fragmentation and attrition characteristics with high oxygen
transport capacity [322]. Wood chips are also employed as solid
fuel in CLC and almost complete combustion to CO2 and H2O could
be achieved with 60 wt% CuO as oxygen carrier [323]. Abad et al.,
[324] examined various technical options to improve the CLC of
solid fuels by increasing the gassolid contact in the fuel reactor,
incorporating secondary fuel reactor to reduce the unburnt com-
pounds, recycling exhaust gases. When compared to gas and solid
fuels, the literature reported on liquid fuels in CLC is relatively less
Moldenhauer et al., [325] employed kerosene (with and without
sulfur) as a liquid fuel with various metal oxides in a 300 W
reactor. They could achieve 99% conversion of fuel carbon to CO2.
3.1.1. Oxygen carriers
Oxygen carriers are important for a CLC system. Cho et al., [326]
found Ni based metal oxide to be a better performer vis a vis other
metal oxides in terms of reduction capacity but exhibited low
1338 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
Fig. 10. The reactor systems for CLC. (a) Fluidised bed; (b) Moving bed; (c) Packed bed; (d) Rotary bed.
strength. Apart from pure metal oxides, mixed metal oxides have
been employed to derive synergistic effect from CuNi and NiCo
combinations [327]. To enhance the mechanical strength and
stability, metal oxides are used with supports like Al2O3, TiO2,
ZrO2, SiO2, coal y ash, etc. They are prepared by mechanical
mixing, co-precipitation, freeze-granulation, spray drying and
impregnation [103,328]. Ryden et al., [329] have employed per-
ovskites and mixed metal oxides of NiO, Fe2O3, Mn3O4. They found
that the perovskites are best suited for chemical loop reforming
(CLR) while mixed oxides for CLC. To reduce the cost of metal
oxides, natural minerals like ilmenite, bauxite waste, manganese
ore and few industrial wastes like iron oxide scale, FeMn slag, etc,
also have been employed in the recent past with encouraging
results [330333]. Ilmenite along with NiO was found to show
higher combustion efciency than its pure form [334]. Kallen et al.,
[335] have very recently employed combined oxides of iron,
manganese, and silica with different compositions. Ryden et al.,
[336] have found that composite materials like NiO or Fe2O3,
Al2O3-, NiAl2O4- or MgAl2O4- based supports and CaMnO3- with
perovskite structures demonstrated high attrition resistance. Cal-
cium Looping (CaL) technology is now emerging as a potential and
sustainable post-combustion CC option. Rapid drop in the CaO
conversion in just few cycles has been the major challenge for its
scale-up [337].
3.2. Reactor engineering aspects
Fixed, moving and uidized bed contactors with single/dual
circulating bubbling and spouting facilities have been used in
batch and continuous modes. The typical components are fuel and
air reactors, loop seal, cold traps, hydrogen generator and other
auxiliary facilities [338342]. Rotarybed reactors are employed for
CLC [343]. The comparative performance of xed and uid con-
tactors have been made for coal fueled CLC [345]. The superior
performance of xed bed contactor is established as far as fuel
conversion and CO2 concentration are concerned. However oxygen
carrier particles have been found to undergo undesirable struc-
tural transformations. A novel hybrid solar thermal chemical
power looping cycle is developed recently with 50% efciency
under 50% share of solar energy [346]. The commonly employed
reactor congurations are shown in Fig. 10.
3.3. Kinetic and modeling studies
With the help of modeling 1D studies, Annaland et al., [344]
established the desirability of a twin packed bed contactor con-
guration in terms of reduced oxygen carrier (OC) requirement.
Markstrom et al., [347] employed a multistaged packed bed model
for solid fuel based CLC with ilmenite as oxygen carrier. Ghoniem
et al., [348] employed CFD modeling for oxyfuel combustion of
coal. Cuadrat et al., [349] studied the nature of oxygen carrier, its
porosity and the role of gasifying agents in a uid bed contactor.
Employing semi-empirical correlations, the performance of a uid
bed contactor for CLC has been simulated with ilmenite as oxygen
carrier. The need for more accurate submodels has been noted.
Employing heterogeneous transport modeling, predictions are
made on intra-particle diffusion, temperature variations in the
reaction zone and gassolid diffusions in a packed bed contactor
[350]. The dynamics of a uid bed contactor for CLC, gas composi-
tion and ow proles, conversions encounter by the oxygen carrier
and CO2 capture efciency received attention in another study
[351]. Bollas et al., [352] compared various reaction schemes and
kinetic mechanisms associated with CLC using methane as fuel
and NiO as the oxygen carrier in a xed bed contactor. A transient
plug ow reactor model with axial dispersion has been used for
simulation studies. Interestingly, shrinking core reaction model is
employed to analyze the reduction reaction of NiO by CO, H2 and
CH4. Employing CFD analysis for a hydrogen fueled contactor. The
bubble hydrodynamics is studied for CaSO4 as oxygen carrier
[353]. Employing Reynolds averaged Navier Stokes equation,
numerical simulations of oxyfuel combustion is studied [354].
Table 5 highlights the CLC contactors, oxygen carrier systems,
kinetics and mass transfer informations and other details.
CLC, which is a post-combustion CC methodology, is a highly
signicant and upcoming technology that has huge potential in
terms of energy efciency, possible integration with power plants
and inherent carbon capture feature. For commercialization of this
technology, more focused studies need to be done on solid fuels in
terms of identifying appropriate oxygen carriers with all the
desired attributes, reactor congurations especially suitable for
solid fuels and real time process conditions and accessing all
possible energy integration options.
4. Cryogenic separation
Cryogenic separation of air and cryogenic distillation of carbon
dioxide (
73.3 1C) has got immense industrial importance in CC.
Membrane separation, adsorption and cryogenic distillation are
among the novel methodologies for CO2 separation. Cryogenic
separation of air is known from the early 19th century onwards.
Cryogenic separations suitable for high CO2/H2S gases in natural
gas were mostly employed for off-shore applications. Some of the
noted processes patented are the Ryan Holmes method (1982)
[380], the controlled freeze zone (CFZ) method (1985 at Exxon
Mobil Upstream Research Company) [381,382], the Cryocell
Table 5
Summary of chemical looping combustion based carbon capture.

Fuel Type OC , fuel type Reactive Operating Conditions CC(%), Kinetics/mass transfer Challenges Remarks Ref
Separator P,T,C,G Purity (%)

Coal CuO, CaO 3-FBR (2- Dp:50100 stage I:20 min, 85,NA C H2 O-CO H2 H 273:15 130:88 kJ=mol Temperature, preparation of Auto-thermal balance, H2 [355]
CLC's) 20 mL/min argon saturated CO H2 O-CO2 H 2 H273:15
41:20 kJ=mol CuOCaO. & CO2 production
with H2O. stage II: at 850 1C, stage I CO CuO-Cu CO2 H273:15
126:92 kJ=mol simultaneously
20 min stage III: in air for H2 CuO-Cu H 2 O H273:15
85:72 kJ=mol
10 min
CaO CO2 -CaCO3 H273:15
178:25 kJ=mol
stage II CaCO3 -CaO CO2 H273:15
178:25 kJ=mol
stage III 2Cu O2 -2CuO H273:15
311:72 kJ=mol

B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

C/CuO/CaO mole ratio of 1:1:1
coal, C2H5OH, Iso-octane, Na2SO4 , CaSO4 TGA T: 2001200; molar ratios of NA,93 (with Combustion of iso-octane (-5101.58 kj/mole) The Hr depends on the fuel Na2SO4 & CaSO4 are [356,357]
C3H8 & CH4. carbon/CaSO4 0.5 & CaSO4 at with Na2SO4 and CaSO4 produces without but not on OC used. suitable.
carbon/steam 1 850 SO2 formation between 200 1C and 344.3 1C
975 1C).
the yield depends on OC. An increase in the
steam/ CO2 ratio increases
the CO2 efciency with
reduced SO2 impact.
Liquid fuel combustion with metal oxides.
CnHm (2n m) MeOx-nCO2 (m)H2O (2n m)
MeOx
1
MeO1
x O2-MeOx
CnHm (n m)O2-nCO2 (m)H2O
MeOx2MeO1
x O2
Coal Calcitic & TGA AR: T:25, P:0.1, VO2/H2O:1; 99 (NiO at NiO to Ni converts in 3 min with CH4 at 600 1C Dp, origin and composition of 1 mole of iso-octane [358360]
dolomitic 950 1C CH4 OCs. -solids inventory combustion produces 17
as fuel),NA depends on type of fuel( moles of H2 CO
CH4 4CO 4H2)
NiO CH4-CNi 2H2 H 191 kJ/mol Porosity favors CO2
diffusion in CaCO3
decomposition.
CoO to Co converts in 1 min with CH4 at 600 1C. 0.3 kg of high-purity
H2 produces from 1 kg
CH4.
95% Ni oxidizes to NiO
with steam in 30 min.
83% of Co oxidizes
with steam in 40 min.
Coal Coal y-ash, TGA, BFB Reducing mixture of H2: 89% at rC;inst mchar
1
U dmdtchar 1
1X char U dXdtchar -Lower combustion y-ash based copper [361364]
bauxite waste, H2O:N2 5:40:55, 200 LN/h; 900 1C, NA efciency with higher OC/ oxide was favorable with
low Ni content Vgas: 0.1 at 900 1C . 95% at fuel ratio. high CO/H2 ratio as fuel.
CaO Al2O3 1000 1C, NA
Char gasication in CO2, the char conversion
from 0.59 at 900 1C 0.65 rate was four times higher
at 1000 1C. at 980 1C than at 900 1C.

Suitable for calcium

looping as a sustainable
emerging technology.
Syngas, H2 Ilmenite, CaO, 2-stage T: 3701030, HR: 9099, 100,NA The packed bed of OC reduces the need of highly efcient PP of O2 in reactors; high -Solids ux affects the [365369]
CuO on Al2O3 PBR-CLC XOC:8095 cyclone to reduce cost; Boron Nitride(BN) used as the dense solid inventories. increase in calciner and
support material due to high thermal conductivity, low carbonator supercial gas
thermal expansion and high thermal stability. velocities & operation of
loop seals

1339
 1340
Table 5 (continued )

Fuel Type OC , fuel type Reactive Operating Conditions CC(%), Kinetics/mass transfer Challenges Remarks Ref
Separator P,T,C,G Purity (%)

Impurities in recycled
ue gases; operational heat
management & switching
valves issues.
Ratio of OC (CuO)to
inert alumina is 1:6 for
better performance in
PBR.
CH4, Coal CuO/Cu, Iron CMBS or Iron Oxide:950 1C, FF:1.18, 499, 495 The reduction kinetics, the activation energy parameters Reaction heat exceeds the solid fuel conversion [370375]
Oxide, BN- RPBR CO2 EF:10, DT: 5.25 are critical to nd fuel conversion efciency, temperature convective heat-transfer rate in the condensed-size
to the gas ow.

B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

support (1 MWth) distribution and carbon separation efciency. reduces the process area
material as footprint.
dense layer in
RPBR.
Adequate residence time of gas in the channel
tfuel needed for complete conversion of fuel
RH
t f uel 0 U dz
f uel
Z t 99%;f uel
Higher costs due to
optimum performance to
char conversion with CO2
capture.
CuO/Cu: Tin :550, P:1, FI:15 ,
CPs:30, FT:1041.5, ufuel:0.09
coal, kerosene, biomass Ilmenite, IFBR Bd:4.750; Dp:128 Umf: 8399.3% at PRC increases linearly by solid ow rate. Scale-up, fuel conversion, The volumetric gas ow [376379]
Mn3O4: MgO 0.0129 : 0.64 800950 1C Agglomeration and attrition. in the AR must be 410
ZrO2 (40:60) , , NA times than that in the FR
CuO: ZrO2 Suitable for iG-CLC.
(20:80)
PRC decreases at 46  Umf. [318320]
CH4, Syngas Fe2O3:Al2O3 CC-MBR T: 700975; SITC:2030; 499%CH4 At 900 1C, the reduction of Fe2O3 to Fe with CO generates The formation of FeO and System is far from use in a [323,324]
(60:40) SFRR: 810 for CO SFRR:4 and 100% 37.7 KJ/mol Fe2O3 of heat but its reduction with H2 gas needs FeAl2O4 indicates further power plant. It is
12 for H2 Fsolids:1.72.5 syngas 61.8 KJ/mol Fe2O3 of heat. utilization of oxygen in iron- developed for CDCL.
conversion. based OC's can be achieved.
499.99%H2 4 1.14.
purity.
 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350 1341

method (developed by Cool Energy Ltd and tested in collaboration
with Shell in Australia ,Perth) [383], Twister technology (2004)
[384] and the Sprex method (developed jointly by IFP, Total, and
Prosernat, 2007) [385]. It has been noted by Yongliang Li [386]
that separation by the cryogen occurs due to decrease in its
internal energy with increase in exergy and also it can be an
efcient medium to recover heat due to their low critical tem-
perature. Oxygen is produced commercially either by cryogenic
distillation process or by adsorption based processes such as VPSA.
4.1. Recent developments
In 2002, Clodic and Younes developed the cryogenic CO2
capture process in which CO2 was desublimated into a solid onto
surfaces of heat exchangers and were cooled by evaporating a
blend of refrigerants [381,387]. Pradeep Bansal (2012) [388],
observed that CO2 as a refrigerant performs signicantly better
than the conventional single stage refrigerants. Martin J. Tuinier et
al., (2012) [389] proposed that the novel cryogenic packed-bed
technology requires a 22% lower energy duty (2.9 MJ/kgCH4 vs
3.7 MJ/kgCH4 for the VPSA process). At a low temperature of

105 1C, the product gas leaving the packed beds reduces the
cooling costs further. Cryogenic technologies operate at high
pressures and low temperatures (o120 K or a liquid boils at
below
150 1C) [390,391]. These systems are preferable to other
conventional CC methods due to their small system size, low
energy requirement, separation of acid gases in liquid form at high
pressure which could be readily pumped to a reservoir [392]. The
cryogenic capture process can reach 99% CO2 capture efciency (at
1 atmosphere) at
135 1C and 90% at
120 1C [393]. In cryogenic
separation of CO2, the moisture in feed gas should be removed in
order to avoid plugging in the system. But, the major limitation of
this methodology is their high capital and operating costs.
4.2. Engineering aspects
It has been reported by Takeshi Kuramochi (2012) [394] that
the critical factors to be considered in cryogenic separation of CC
are capacity factor (9197%), energy prices (natural gas: 82007/
GJ, coal: 2.52007/GJ, grid electricity: 55/MWh), economic plant
lifetime (20 years), CO2 compression pressure (110 bar) and grid
electricity CO2 intensity (400 g/kWh). In condensed rotational
separation (CRS), maximum compression ratio is 4 per stage with
heat exchanger effectiveness of 82% to achieve 7090% CO2
recovery. The energy penalty in CRS has been reported as 912%
for an inlet CO2 concentration of 4070% and for CRS combined
with oxygen enriched coal, combustion is 1619% (2012)
[395,396]. It is a single process of sequestration and compression.
CRS separates CO2 in liquid form with energy penalty slightly
higher than gas compression alone. The inlet conditions of feed
and exit conditions of product were maintained 1 bar and 40 1C in
CRS. It is capable of producing waste stream purity of Z95%CO2
liquid at 100 bar pressure. Cryogenic combined cycles integrated
with molten carbonate fuel cells (MCFC) reported with an electric
efciency similar to that of the original combined cycle (58.7%
LHV). In this cell, the critical parameters are current density
ic 1500 A/m2, with cell voltage at 0.708 V and Specic Primary
Energy Consumption for CO2 Avoided (SPECCA), measured in
kJLHV =kgCO2 (2011) [397]. Annaland et al., [398] have made a
techno-economic comparison between cryogenic CO2 capture

Table 6
Summary of cryogenic based carbon capture.

Reactive Operating conditions CC (%), Kinetics/mass transfer Challenges Remarks Ref

separator P,T,C,G Purity of
CO2(%)

CRS MCR:4; HEE: 82
GTC: 80 (per stage)
Finlet:1 atm, 40 1C
Pexit: 1 atm, 40 1C,
4070% of inlet CO2
Waste: 100 atm, 40 1C
CCI with O2 utilization factor UCO2:11%; 80, NA
MCFC ic:1500
STCR: 3.5 at anode inlet
Cell voltage:0.708 V
CASU-PB O2: 80 mol% (inlet purity)

192 1C, 1 atm and
172 1C,
6 atm
Dp 4.04, Bd:2.547
DOCPB T:
150, Fsolids: 312
Dp 4.04 mm, Bd: 2.547
PBR properties:
Lbed :8; Dbed : 3
Z 95 at The phase equilibrium model is based Energy penalty is 912% Compression with [395,396]
100 atm, on equi-fugacity calculations using and for CRS combined single process of [398,399]
NA PengRobinson Equation of State, Van- with oxygen enriched sequestration.
der-Waals one-uid mixing rules. coal combustion is 16% bulk separations of
19%, 70%90% CO2 CO2 possible.
recovery.

HRREF 3600:1=
1=REF higher CO2 concentration Electric efciency is same [397]
SPECCA HRREF
REF

on the cathode side of the original combined
cycle (58.7% LHV), 22%
increase in power output.
90, 95 NA Complex operating Higher energy penalty to [406]
conditions of heat achieve liquefaction of CO2
exchangers. , H2, O2 and N2 gases.
98, 4 99    2 Bed dimensions Novel CPB needs o 22% [407413]
C
ef f 1
A g s g Ag g p;g g;s1as
depends on cycle times. energy duty (2.9 MJ/kgCH4
 0:45
g;s
dg 2:978 1 0:095 Re PrdLhc High energy vs 3.7 MJ/kgCH4 for the
h
consumption and heat VPSA process)
2 d
2
Dax Def f ;i 192D
g h;c
leaks.
ef f ;i

Porosity 0.7; Bd: 7.750

 
Cryogenic MFgas:7.69; T:
20; idle 480, NA mt hm:CO2 CO2 ;g
CO2 ;s Long pre-chilling Energy penalty of [414416]
CO2 operating time of 4 h, ow time and limitation of 3.4 MJ/kg CO2.
Capture rate: 2 L/min; temperature of cooling area. -High efciency, [400405]
by FPSC SC-1 of
20 1C. convenient to operate
machine and small size.
The frost layer of The bed capacity is
captured CO2 will much higher with
adversely affect the 8 factors higher.
heat transfer. Deep H2S removal is
possible at temperatures
150 1C required.
1342 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350

using cooled packed beds, amine based absorption and membrane
separation and found that the availability and the cost of the
required utilities like LNG for the cryogenic process, steam for
absorbent process determines the preferred option and that the
initial bed temperature, feed ow rates and CO2 concentration in
the feed are critical parameters affecting the process economics.
The cryogenic capture would be best candidate for low pressure
drop and simultaneous removal of various impurities in a single
process. Surovtseva et al., [399] have demonstrated the combined
use of hydrate and cryogenic methods at pilot level for enhanced
CC for IGCC ue gases with CO2 purity of 97% achieved in liquid
form with reduced energy consumption. A novel stirling cooler
system has been employed by Kitamura et al., [400] for cryogenic
CC achieving the CO2 separation from ue gas of 85% with 3.4 MJ/
kg CO2. This was found to be advantageous as the CC could be
achieved at atmospheric pressure to avoid the regeneration of
solvent and energy penalty of pressure drop. The long idle times
and higher heat transfer resistances limiting the overall efciency
were the challenges to overcome in future research. Besides
packed beds and stirling coolers, dynamically operated low cost
ber beds (with high areavolume ratio and lower sweep gas
pressure drop) were successfully employed for the enhanced
cryogenic CC. Two types of ber materials were tested viz., hollow
cellulose acetate and monolament nilon were used in a two stage
process achieving CO2 purities between 28 mol% and 99.5 mol%.
This would be a potential method to reduce the capital costs of the
cryogenic method and to increase the CO2 loading per chilling
cycle at larger scales [401]. Kentish et al., [402] have found that by
integrating membrane separation (three stages) with cryogenic
separation, the cost of separation has been signicantly reduced to
less than $32 per ton with a feed containing 33 mol% CO2. Berstad
et al., [403] have done a critical review on the applications and the
potential for low temperature CO2 capture technologies and found
that specic power consumption and the capture ratio depends on
feed CO2 concentration and that the low temperature capture was
more suitable for syngas from coal gasication vis a vis baseline
technology. Song et al., [404] have very recently used response
surface methodology (RSM) for optimization of cryogenic CC and
found that the optimal conditions are ow rate of 2.16 L/min;
temperature of
18 1C, operating time of 3.9 h to achieve the
capture of 95.2% CO2 with 0.52 MJ/kg captured CO2 input electricity
and productivity of 44.37 kg CO2/h. Recently energy analysis has
been done for the cryogenic CO2 capture process based on stirling
coolers with three sections of pre-chilling, CO2 anti-sublimation
and storage and found that the total energy consumption was
689.2 J/L ue gas [405]. All the above studies on cryogenic CC
indicate that it has a high potential for reducing energy penalty
but needs further research in developing the cost effective reactor
congurations with cheap coolants.
The following Table 6 describes chronological research devel-
opment with various process options for cryogenic separation of
CO2 and air.
Among available process options with cryogenic separation of
CO2 and air, CRS technology is the only viable option of compar-
ably less energy penalty with better yield of CO2 separation. But,
CRS technology needs to be tested on pilot scale for commercial
viability with minimal gas leakages concerned.
5. Sustainability through CC and critical comparison of various
CCTs
5.1. Enhancing the sustainability levels of CC technologies
The CCS is a family of technologies and techniques that enable
CO2 capture for enhancing the sustainability of fuel combustion
processes. They can be viewed as a portfolio of solutions with
potential to enhance their sustainability levels further by introdu-
cing new technological solutions, renewable options and sharpen-
ing energy utilization efciencies. The current CC options can be
considered as 2030% of the overall enhancements, the world
science has to achieve. Whether any CCS technology is in transi-
tion or an end state of sustainability depends on the time frame
and technology status.
The CCS technologies have to be so designed that they deliver
consistent environmental and social benets which exceed their
cost of capital, energy and operation. The rst level of CCS
technologies have focused on the basic requirement of environ-
ment viz., GHG emission minimization for human health and
safety with inherent economic tradeoffs. The second and third
generation technologies will adopt more sustainable retrots
which can readily curtail the use of fossil fuels and capture agents
and phase out technoeconomically inefcient process options. For
example, the current option of storing CO2 into geological

Table 7
Comparison of various reactors used for CC.

Parameter Parameter signicance Fluidized-bed Moving- Packed-bed Rotary bed

bed

Gassolid contact Perfect contact is essential for fast and complete Limited Fair Good Excellent
operation.
Temperature control Uniform temperature prole for the oxygen carrier is Excellent Good Limited Excellent
designed.
Regenerability Readiness with no. of cycles. Good Good Limited Excellent
Scale-up Retention of advantages with scale-up is a challenge. Good Fair Fair Excellent
Pressure drop Lower pressure drop is preferred for minimal external Good Good Fair Excellent
power intake.
AAP Agglomeration and Attrition losses affect CC efciency. Very high medium Limited Limited
Oxygen carrier High circulation rate is required for higher capacities. Very high medium Limited Limited
circulation
Fuel conversion 100% conversion is desired. Good Fair Excellent Excellent
Gas leakage Air leakage increases the cost of CO2 separation. Fair Fair Limited Very high
CO2 separation separation from ue gases OFC-II, OFC-III, OFC-II, Membrane, adsorption, OFC-II, OFC-III
SAFB OFC-III Absorption,
TSA,PSA,ESA, Cryogenic CO2
separation
CO2 combustion Fuel combustion Post-CCC,OFC-I Post-CCC Post-CCC &pre-CCC Post-CCC,OFC-II,
OFC-III

Note: AAP: agglomeration and attrition of particles.

 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350 1343

Table 8
Critical comparison of technologies.

CCT Type Conventional Novel methods CC () Reactors Kinetic modeling and Challenges
methods (max. simulation
achieved)

Absorbent Pre-CCC, Post- Single solvents as Mixed solvents as 100 PBR, Double stirred cell, NLP model, absorber Solvent
CCC piperazine, ionic liquids, MEA K2CO3, AMP-PZ, bubble column, rotating performance, Sorbent selection and
binding organic liquids, PEI-SiO2, Alcohol/amine/ packed bed, tray towers ow characteristics and reactor type
MEA, K2CO3, DIPA, H2O, DEA-MDEA, MEA- kinetics
MDEA, etc. DEA
Adsorbent Post-CCC ViscoseRayon HCM, Flyash PEI PEG, Co- 95 SAFB, PBR (TSA,PSA and Langmuir adsorption Faster
ZX MEA, NaX, MOF-74(MS), CaO (CLP), ESA), RPB isotherm, Eulerian synthesis with
yash PEI PEG, PEI MCM-41, PEI- Lagrangian model, Toth MS and
UiO66-MOF silicagel, amine silica and dual site Langmuir enhanced
aerogel, FAC isotherms, Molecular and capacity with
Knudsen diffusion, ZLC KOH & NaOH
technique, uidized bed
contactor performance
Membrane Post-CCC Micro-porous membrane Liquid in pores of 100 Hollow ber and Flat- equations of motion, Viscosity with
membrane and dense Sheet membrane packed One-dimensional, two- ionic
membranes, DEA columns dimensional model and membrane
supported on poly vinyl convection-diffusion,
alcohol, ionic liquids Regenerator height and
supported on PVDF, multiphase CFD ow
polymers,..etc
OFC(OFC-I) OFC ASU for pure O2 mixed 35%O2, 65%CO2 and sand 100 FBR, PBR Gas composition and Inventory and
with recycle CO2 particles for enhanced load generation models, scale-up
combustion Adaption of non-linear
control gains, turbine
system
CLC(OFC-II) OFC NiO, CuO, Mn2O3, Fe2O3, MOF, CaO supported on 499 RPBR,CFBR, PBR Hydrodynamic, Heat Inventory,
etc. cement, transfer and mass attrition,
transfer models, 3-CLC agglomeration
reactors for NH3 and scale-up
synthesis, 1D & 2D
reactor models, large
eddy simulations.
CLOU(OFC-III) OFC CoO, Mn2O3, CuO, etc. CuO supported on 100 RPBR Mass transfer and heat Inventory,
MgAl2O4, iG-CLC for in- transfer models, Partial agglomeration
situ gasication of solid pressures of O2 in and scale-up
fuels with suitable OC. oxidation and reduction
reaction rates, 1D & 2D
reactor models, large
eddy simulations.
Algae systems Bio- Algae in open pond Algae in bio reactors 100 BESs, MEDC, BR-MPBR Inventory and
sequestration cultivation scale-up
Cryogenic CO2 Cryogenic CO2 Cryogenic chillers, Heat CCI with MCFC, FPSC 100 PBR, Stirling cooler Based on equi-fugacity 1619% Energy
separation capture exchangers model, frosted CO2 penalty
depends on heat transfer
between gas stream and
cooling ns

formations has to be transient solution since public opposition and
concerns about global climate change have to be met in due course
of time.
Viewed from the above context, the current and future devel-
opments in CC technologies have also to be explained from
sustainability consideration. The CO2 capture by the absorption,
adsorption or membrane separation if used in conjunction with
CO2 utilization processes like urea, precipitated CaCO3, CO and
methanol generation will signicantly nullify the energy penalties
associated with the CC process. They become more sustainable
from energy and material utilization viewpoints. Enhanced oil
recovery with captured CO2 will enable its large scale utilization at
a higher sustainability level. The use of environment friendly
absorbents like ionic liquids will further enhance the sustainability
levels of these processes. The CLC option with reusable metal
oxides derived from unutilized ores, industrial or agro wastes is
much more sustainable option than oxyfuel combustion. The uses
of hybrid renewable nonrenewable energy options provide a
relatively lower carbon energy option eminently suitable as a
transition option. Tables 7 and 8 show comparison of reactors used
in CC and critical comparison of CC technologies respectively.
Various carbon capture technologies discussed above may be
employed for pre- or post-combustion CC or both. The critical
comparison of all these technical options has been provided in
Table 7 with reference to classication of the CCT, conventional
and novel materials employed, contactor congurations used to
achieve the objective, maximum CC achieved, important models
developed and used to explain them besides giving the challenges
and future directions for research. Table 8 gives the comparison of
all reactors/contactors that could be used for various carbon
capture methods.
6. Conclusions
In this paper, various CC technologies viz., absorption, adsorp-
tion, membrane separation, oxy and chemical looping combustion
and cryogenic separation employed as pre- or post-combustion CC
1344 B. Sreenivasulu et al. / Renewable and Sustainable Energy Reviews 41 (2015) 13241350
options have been comprehensively reviewed w.r.t. material
development, process and engineering aspects including contac-
tors/reactor congurations and their design aspects along with
successful models developed to explain the process performance.
This review shows that the tremendous global knowledge base
available in this area and a portfolio of alternative technologies
exists now though at different technology readiness levels. Some
of them have passed laboratory, bench and pilot plant stages of
development they need to be demonstrated on a larger scale. At
this juncture, no technology may be a credible candidate by itself
for commercial level implementation. However, the portfolio as a
whole is large enough to throw several commercially viable
alternatives in the future.
The post-combustion capture of CO2 from industrial ue gases
through gasliquid absorption need high level R&D with focus on
evolving cost effective desorption option. At present, tt is the only
industrial carbon emission management technology that has very
high potential for wide scale deployment. The large scale storage
of CO2 is not a long term solution. The commercial success of CC
technologies to a great extent depends on CO2 utilization to
generate industrial chemicals of high commercial value. Intense
R&D is required in this area. The largest deployment of CC
technologies has to occur in developing countries in the coming
years and CO2 utilization will be an important component of their
effort to combat climate change.
Dedication
This paper has been gratefully dedicated to our beloved
teacher, Dr. K.V. Raghavan who has been our constant source
of inspiration, enthusiasm and support on the eve of 50 years of
illustrious research career completion on 1/10/2014.
Acknowledgments
The authors would like to express their gratitude to the
management of BITS-Pilani, Hyderabad campus for the infrastruc-
tural support provided towards the research work.
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