1 s2.0 S1364032117310699 Main
1 s2.0 S1364032117310699 Main
1 s2.0 S1364032117310699 Main
A R T I C L E I N F O A BS T RAC T
Keywords: Hydrogen is an attractive energy carrier due to its potentially high energy efficiency and low generation of
Hydrogen pollutants, which can be used for transportation and stationary power generation. However, hydrogen is not
Chemical-looping readily available in sufficient quantities and the production cost is still high. Steam methane reforming (SMR)
CO2 capture process is now the most widely used technology for H2 production, but this process is complex and cannot get
Oxygen carrier
thorough carbon capture. Hydrogen production using chemical looping technology has received a great deal of
attention in recent years because it can produce hydrogen with higher process efficiency and can capture carbon
dioxide. Many researchers have carried out intensive research work on the hydrogen production processes using
chemical looping technology. Based on the previous studies stated in the literature, the authors try to give an
overview on the recent advances of two categories, chemical looping reforming (CLR) and chemical looping
hydrogen production (CLH) processes. Besides, the characteristics of the processes are pointed out based on the
comparison with the conventional SMR process. The existing technical problems and the aspects of future
research of each approach are also summarized.
⁎
Corresponding author.
http://dx.doi.org/10.1016/j.rser.2017.07.007
Received 5 April 2017; Received in revised form 4 June 2017; Accepted 4 July 2017
Available online 09 July 2017
1364-0321/ © 2017 Elsevier Ltd. All rights reserved.
M. Luo et al. Renewable and Sustainable Energy Reviews 81 (2018) 3186–3214
2. Steam methane reforming process than 22% if carbon capture and storage (CCS) system is added [23].
Therefore, although it is wildly used in hydrogen generation, SMR
The SMR process consists of feed stock purification, steam reform- process is a complex process that involves many complex catalytic
ing, a high-temperature shift reactor, a low-temperature shift reactor steps. Additional energy and equipment is needed to separate CO2 from
followed by a pressure swing adsorption apparatus for purification of the exhaust gas, and this process cannot achieve a 100% CO2 capture
the produced hydrogen. The schematic diagram of the SMR process is rate. In addition, the heat transfer coefficient of the internal tube in
shown in Fig. 1. reformer is the rate-limiting parameter, which needs to be increased.
The methane needs to be firstly desulfurized since small amounts of
sulfur are enough to poison the catalyst. Desulfurized methane is then 3. Hydrogen production using chemical looping technology
catalytically reformed at the temperature range of 970–1100 K to
produce synthetic gas (syngas) with a mixture of CO and H2 [15]: Chemical looping technology has received great attention in recent
years. A typical process is chemical looping combustion (CLC). This
CH4+H2O = CO+3H2-206·3 kJ/mol (1)
process is different from conventional combustion process, which is
Syngas is cooled and then shifted in the water-gas shift (WGS) accomplished by using two reactors and a circulating metal oxide, see
reactors, where the WGS reaction happens to increase the H2 yield and Fig. 2. The oxygen carrier constantly circulates between the fuel reactor
to decrease the CO concentration [16–18]. (FR) and air reactor (AR). In the FR, the particles are reduced by the
fuels, and the fuels are oxidized to CO2 and H2O through reaction 6. In
CO+H2O = CO2+H2+41·0 kJ/mol (2) the AR, they are oxidized to its initial state with O2 through reaction 7.
As a final stage, the gases including CO2, water, methane, and CO Due to the fact that the fuel and air are separated in CLC, the
need to be removed from the flue gas, and the total reaction of SMR combustion products of CO2 and H2O are not diluted with nitrogen.
process is as follows: This means that by condensing the H2O, it is possible to obtain almost
pure CO2 without expending any extra energy needed for separation.
CH4+2H2O = CO2+4H2-165·3 kJ/mol (3) Other benefits include a large elimination of NOx emission [25–29] and
high thermal efficiency [27].
The SMR reaction (Eq. (1)) is highly endothermic and usually runs
at high temperature above 1073 K. In order to sustain this endothermic (2n + m)MxOy+CnH2 m = (2n + m)MxOy-1 + mH2O+nCO2 (6)
reaction, heat is supplied to the reforming reactor by burning part of
the natural gas or the purge gas from the pressure-swing adsorption
(PSA) in a furnace. Therefore, this process also gives off carbon MxOy-1 + 1/2O2 = MxOy (7)
monoxide and carbon dioxide. Nickel is usually used as the major Chemical looping combustion is used in heat and power generation
metallic component of the SMR reaction catalysts. However, the process. Hydrogen production using chemical looping technology
catalyst loaded into the tubes of the reformer is poorly utilized as the utilize the same general principles as CLC. The difference is that the
heat transfer coefficient of the internal tube wall being the rate-limiting wanted products are not heat but H2 or/and syngas (H2 and CO).
parameter [19]. SMR process also involves the risk of carbon formation Hydrogen production using chemical looping technology can be
with Ni particles as catalyst. Generally, the methane decomposition summarized into two categories, chemical looping reforming (CLR)
(Eq. (4)) and the Boudouard reaction (Eq. (5)) may occur during the and chemical looping hydrogen production (CLH). Other new pro-
process [20,21]. Carbon formation may lead to degradation of catalysts cesses coupled the chemical looping to produce H2, such as methane
and other severe operational trouble, which must be eliminated. cracking thermally coupled with a CLC process [31], or the methane
CH4 = C+2H2 (4) direct thermocatalytic decomposition by using an activated carbon as a
catalyst [32] have also been proposed and investigated, but they are not
2CO = C+CO2 (5) contained in this paper and can be found elsewhere.
The WGS reaction (Eq. (2)) involved a complex system. This is 3.1. Chemical looping reforming
traditionally carried out in two fixed bed adiabatic reactors, connected
in series with a cooler between them [16]. The first reactor operates at The concept of CLR was originally proposed by Mattisson and
higher temperatures and employs a Fe/Cr catalyst. The second reactor Lyngfelt et al. [33] in 2001. Based on the principle and characteristics,
with a Cu/Zn/Al catalyst operates at lower temperatures in order to
increase the possible equilibrium conversion of CO as the WGS
reaction is exothermic.
PSA and amine absorption technology can be used to capture CO2
and purify H2 produced in the SMR process. In older plants, CO2 is
subsequently removed by means of a chemical absorption unit. Modern
hydrogen plants apply PSA to separate hydrogen from the other
components, which produces higher quality hydrogen (99.999%
against 95–98% for scrubbing systems) at feedstock pressure (circa
25 bar) [22]. However, these processes increase the total investment
costs and decrease the thermal efficiency of the SMR process. It is
estimated that the cost of hydrogen generation will increase by more Fig. 2. The schematic diagram of chemical-looping combustion process [30].
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N2, O2 H2O, CO2 H2O. To achieve a pure hydrogen stream, this reformer-gas should be
converted in a WGS reactor to maximize hydrogen production and
finally CO2 and H2 could be separated with pressure swing adsorption
MyOx
or absorption with suitable amine solvent. The basic principles of
AR FR CLR(a) are illustrated in Fig. 5.
Steam If the fuel is methane and NiO is selected as an oxygen carrier, the
Fuel & Steam
Reformer
MyOx-1 main reactions in the FR are:
Direct partial oxidation with metal oxide:
Air PSA offgas Heterogeneously catalyzed steam reforming and CO shift reaction:
(H2, CH4, CO2, CO)
CH4+H2O = CO+3H2- 225·5 kJ/mol (9)
Reformer gas
(H2O, H2, CO2, CH4, CO)
CO+H2O = CO2+H2+33·6 kJ/mol (10)
Fig. 3. Schematic description of CLR(s).
Internal combustion:
it can be classified into three approaches: i) Steam reforming using
CO+NiO = CO2+Ni+47·2 kJ/mol (11)
chemical looping combustion, CLR(s), which is also called “Steam
reforming integrated with chemical looping combustion (SR-CLC)” in
H2+NiO = H2O+Ni+13·6 kJ/mol (12)
many literatures, ii) Autothermal chemical looping reforming, CLR(a),
and iii) Chemical looping reforming of methane, CLRM, which is also
CH4+4NiO = CO2+2H2O+4Ni-137·7 kJ/mol (13)
called “Chemical looping steam methane reforming (CL-SMR)” or
“Two-step steam methane reforming”. In the AR the metal oxide will be oxidized by air according to:
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(a) The reformer in the FR [31]. (b) The reformer in the AR [35].
Fig. 4. Schematic diagram of the CLR(s) system.
Depleted Air Reformer Gas Ni-ferrites [45], (Zn, Mn)-ferrites [46], Cu-ferrites [47–49], and Ce-
N2 H2, CO, H2O, CO2 based oxides [50–55] have been considered as possible oxygen carriers
for this process.
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[83] also evaluated the performance of NiO-based oxygen carriers 3.1.2.2. Ce-based oxygen carriers. The feasibility of the CeO2 on the
supported on ZrO2, TiO2, SiO2, Al2O3 and NiAl2O4 in CLRM process. It partial oxidation of methane into synthesis gas has been confirmed by
was found that the NiO/ZrO2 exhibited the best performance on CH4 Otsuka et al. [51,166] and Wei et al. [89]. Direct conversion of methane
conversion and stability in 20 redox cycles. In addition, it was observed into synthesis gas with the H2/CO ratio of 2 has been demonstrated
that the oxygen carriers prepared by a deposition-precipitation method using CeO2 as an oxidant at temperatures higher than 600 °C.
had higher tendency to increase the carbon deposition than the oxygen However, methane cracking and the decrease of reactivity was also
carriers prepared by dry impregnation [56]. observed when CeO2 was used during redox cycles [53]. Different
Despite the superior activity and the selectivity, the selectivity to materials have been added as promoters to increase the selectivity of
synthesis gas of the nickel-based oxides need to be further improved the Ce-based oxygen carriers.
[39,63]. Mattisson et al. [163] found that almost complete conversion
of CH4 into CO2 and H2O could be achieved even with a very small The mixed-metal oxides by combining another material to CeO2
amount of NiO. Therefore, the syngas yield largely depends on the could be a way to increase the reactivity, stability, and selectivity. Many
oxidation degree of the oxygen carrier. CO2 and H2O can be easily kinds of Ce-based oxides, such as Ce–Zr [94,95,101], Ce–Fe
formed by highly oxidized Ni-based oxides and CO and H2 generated by [52,86,92,96–98], Ce–Al2O3 [87,89], Ce–MgO [99], Ce–Cu, Ce–Mn
reduced particles [65,75]. Nakayama et al. [70,126] proposed the [85], Ce–Nd [93] and so on were investigated. In general, Ce–Fe mixed
reactivity of NiO–Cr2O3–MgO complex oxide as an oxidant to produce oxides exhibited good activity and stability among all the oxides. But
nitrogen-free synthesis gas or hydrogen by the partial oxidation of their selectivity for syngas generation was strongly affected by the
methane. It was found that the lattice oxygen was effectively trans- specific surface area of oxygen carriers. Moreover, the doping ratio of
ferred to CH4 to give H2 and CO in the ratio of 2–3:1 at 700 °C. The Fe to Ce should be carefully settled because the high content of Fe
oxygen carrier exhibited high and constant catalytic activities for failed to increase the CH4 conversion and inclined to decrease the CO
repeated reduction with CH4 and oxidation with air cycles without selectivity [98].
significant carbon deposition. The addition of Cr2O3 weakened the Ni– The addition of Pt [50,51,88] and Rh [88] remarkably accelerated
O bond in NiO–MgO complex oxide, and decreased the temperature of the formation rates of H2 and CO and decreased the activation energy
the reaction of CH4 with NiO [70]. of synthesis gas production. The promoters not only drastically
One of the major issues in the CLR processes of hydrocarbons using enhanced the conversion of methane, but also lowered the temperature
the nickel-based materials is the deactivation caused by carbon necessary to reduce the cerium oxide, while the promoters may also
deposition on the surface of the matierial. One possible way to serve lead to some carbon formation [88]. The reduced oxide can be fully
this problem is to add small amount of alkali metals, which could regenerated and the carbon deposited can be completely removed by
effectively reduce carbon deposition on the material surface in the high oxygen. He et al. [85] investigated the effect of additions Fe, Cu, and
temperature reforming process [164,165]. Another method is to add Mn on the reactivity of CeO2. It was revealed that the addition of
small amount of steam to the reactor to reduce or even eliminated the transition-metal oxides into cerium oxide could improve the reactivity
carbon deposition [39,75]. However, the successfully operation of of the Ce-based oxygen carrier, and the three kinds of mixed oxides
a140 kW dual circulating fluidized bed pilot plant has been implemen- showed high CO and H2 selectivity at the temperatures above 800 °C.
ted using NiO/NiAl2O4 with or without small MgO added as oxygen Among the three kinds of oxygen carriers, Ce–Fe–O presented the best
carriers and natural gas as fuel [38]. Results showed that even though performance, and methane was converted to synthesis gas at a H2/CO
no steam was added to the natural gas, no carbon formation was found molar ratio close to 2:1 at a temperature of 800–900 °C. Wei et al.[91]
for global excess air ratios larger than 0.4. Thus, the carbon deposition also explored the reactivity of Ce–Fe–O mixed oxide (Ce/Fe=7:3) in
was not a problem in a real process. Furthermore, other cheracteristics, direct partial oxidation of methane to syngas process. Approximately
such as the toxicity and the cost of nickel-based oxygen carriers may 99.4% H2 selectivity, 98.8% CO selectivity and 94.9% CH4 conversion
limit their application. were achieved at 900 °C in fixed bed experiments. The Ce–Fe–O mixed
Other than CH4, Ni-based oxygen carriers also have promising oxide as the oxygen carrier showed good methane selectivity into
properties in converting liquid and solid fuels to syngas, which will be syngas by the lattice oxygen and cycle performance in redox cycles.
reviewed in Section 3.1.3. Note that, the feasibility of the Ce-based materials is confirmed
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Table 1
Summary of the oxygen-carriers tested in different CLR units.
(i) 11 wt% NiO (i) α-Al2O3 (i)–(iii) DP n.g. TGA, bFB [56]
(ii) 16 wt% NiO (ii) θ-Al2O3 (iv)–(v) DIMP
(iii) 21 wt% NiO (iii) γ-Al2O3
(iv) 26 wt% NiO (iv) α-Al2O3
(v) 28 wt% NiO (v) γ-Al2O3
17–18.5 wt% NiO CaAl2O4 PUR CH4+H2, CH4 PB [57]
18 wt% NiO α-Al2O3 PUR Glycerol FxB [58]
18 wt% NiO α-Al2O3 PUR Waste cooking vegetable oil PB [59,60]
18 wt% NiO α-Al2O3 PUR Pyrolysis oil PB [61]
18 wt% NiO α-Al2O3 PUR Acetic acid PB [62]
(i) 18 wt% NiO (i) α-Al2O3 (i) IMP n.g. cFB [63]
(ii) 20 wt% NiO (ii) MgAl2O4 (ii) FG
(iii) 21 wt% NiO (iii) γ-Al2O3 (iii) IMP
(i) 18 wt% NiO (i) α-Al2O3 WIMP CH4 TGA, cFB [64]
(ii) 21 wt% NiO (ii) γ-Al2O3
(i) 18 wt% NiO (i) α-Al2O3 IMP CH4+H2, H2 FxB [65]
(ii) 21 wt% NiO (ii) γ-Al2O3
(i) 18 wt% NiO (i) α-Al2O3 WIMP CH4 pFB [66]
(ii) 21 wt% NiO (ii) γ-Al2O3
(i) 18 wt% NiO (i) α-Al2O3 IMP CH4, H2, CO TGA [67]
(ii) 21 wt% NiO (ii) γ-Al2O3
(i) 18 wt% NiO (i) α-Al2O3 (i) WIMP Bioethanol cFB [68]
(ii) 21 wt% NiO (ii) γ-Al2O3 (ii) HWIMP
(i) 18 wt% NiO (i)α-Al2O3 PUR Ethanol/bio-oil aqueous fraction PB [69]
(ii) 25 wt% NiO (ii)γ-Al2O3 mixture
(i)–(vii) 20 mol% NiO (i) MgO (i)–(vii) IMP CH4 FxB [70]
(viii) NiO–Cr2O3 (ii) Al2O3 (viii)–(x) EM
(ix) NiO–MgO (iii) SiO2
(x) NiO–M–MgO(M=Al2O3, CaO, Cr2O3, (iv) TiO2
Fe2O3, Co3O4), Ni/additive/Mg = (v) Y2O3
16:4:25 as a molar ratio (vi) La2O3
(vii) CeO2
(viii) MgO
(ix)–(x) None
20 wt% NiO CaAl2O4 PUR H2, CO, CH4 TG, FxB [71]
25 wt% NiO Al2O3 COP Glycerol FxB [72]
(i) 35 wt% NiO (i)–(iv) SiO2 DIMP CH4 bFB [73]
(ii) 39 wt% Fe2O3
(iii) 41 wt% CuO
(iv) 47 wt% Mn2O3
40 wt% NiO (i) α-Al2O3 SD n.g. cFB [74]
(ii) α-Al2O3–MgO
40 wt% NiO Mg–stabilized ZrO2 FG n.g. cFB [75]
40 wt%NiO (i) Al2O3 WIMP CH4 TGA, FxB [76]
(ii) ZrO2
40 wt% NiO α-Al2O3 SD Raw gas from biomass gasifier cFB [77]
40 wt% NiO (i) NiAl2O4 SD n.g. cFB [38]
(ii) 42 wt% NiAl2O4+18 wt%
MgAl2O4
40 wt% NiO (i) α-Al2O3 SD n.g. cFB [74]
(ii) α-Al2O3+MgO
40 wt% NiO MgO–ZrO2 FG Kerosene cFB [78]
(i) 40 wt% NiO (i) NiAl2O4 (i)–(iii)FG Toluene TGA, FxB [79]
(ii) 40 wt% Mn3O4 (ii) Mg–ZrO2 (iv)–
(iii) 60 wt% NiO (i) MgAl2O4
(iv) ilmenite ores (iv) None
(i) 40 wt% NiO (i) NiAl2O4 (i)–(iii)FG CH4, CO, CH4+H2O, TGA, FxB [80]
(ii) 40 wt% Mn3O4 (ii) Mg–ZrO2 (iv)– CH4+C7H8+H2O, CO+H2,
(iii) 60 wt% NiO (i) MgAl2O4(iv) None CH4+C7H8+H2O+CO+H2,
(iv) ilmenite ore CH4+C7H8+H2O+CO+H2+CO2
(i) 40 wt% NiO (i) NiAl2O4 FG CH4 bFB [81]
(ii) 60 wt% NiO (ii) MgAl2O4
42.1 wt% NiO NiAl2O4 COP Glycerol MB [82]
42.1 wt% NiO NiAl2O4 COP Glycerol FxB [72]
60 wt% NiO MgAl2O4 FG n.g. cFB [39]
(i) 100 wt% NiO (ii) ZrO2 WIMP CH4 FxB [83]
(ii)–(vi) 40 wt% NiO (iii)TiO2
(iv)SiO2
(v)Al2O3
(vi)NiAl2O4
(i) 100 wt% NiO (i)– Ultrasound assisted Ethanol TGA, FxB [84]
(ii) xNi (x = 10 , 20, 30 wt%) (ii)Montmorillonite cation exchange
(continued on next page)
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Table 1 (continued)
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Table 1 (continued)
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Table 1 (continued)
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the liquid fuel can have the similar performance with that of gaseous
fuels in a continuous CLR(a) process. Ortiz et al. [168] investigated the
reaction conditions at for a high Syngas-H2 production in the CLR(a)
system with ethanol as fuel based on the thermodynamic equilibrium
state. The feasibility of CLR(a) using bioethanol was demonstrated in a
1 kWth circulated fluidized bed reactor during more than 50 h [68]. A
syngas composed of ≈ 61 vol% H2, ≈ 32 vol% CO, ≈ 5 vol% CO2 and ≈
2 vol% CH4 was obtained.
Mendiara et al. [79,80] selected toluene (C7H8) as model compound
of biomass tar and evaluated the feasibility of CLR(a) process as a
technology for biomass tar cleaning. The performance of four oxygen
carriers (60% NiO/MgAl2O4 (Ni60), 40% NiO/NiAl2O4 (Ni40), 40%
Mn3O4/Mg–ZrO2 (Mn40) and FeTiO3 (Fe)) were tested under alter-
nating redox cycles and the conditions to minimize the carbon
deposition have also been investigated. It was found that Ni40 and
Mn40 showed stable reactivity to C7H8 after a few cycles. Ni40 showed
a high tendency to carbon deposition, but this could be completely
avoided by adding water with a H2O/C7H8 molar ratio of 26.4. Fig. 9. Ethanol adsorption and transformation over CoFe2O4 (A), NiFe2O4 (B), and
However, the deposition could not be completely avoided in spite of Fe3O4 (C) [117].
the high H2O/CxHy molar when CH4 and C7H8 were mixed when using
Ni40 as oxygen carrier [80]. Lea-Langton et al. [61] studied the common to all spinels and corresponds to a dehydrogenation to
feasibility of pine oil and palm empty fruit bunches (EFB) oil with acetaldehyde. However, the following pathways depended on the
Ni/Al2O3 as a catalyst and an oxygen transfer in a packed bed at spinel. Acetaldehyde could be either oxidized to acetates (NiFe2O4),
600 °C. The results were remarkable with the maximum averaged fuel mainly decomposed to CO and methane (CoFe2O4), or completely
conversions of pine oil and EFB oil ~ 97% and 89% when the steam/ oxidized (Fe3O4) (see Fig. 9).
carbon ratios of 2.3 and 2.6 respectively during the reduction process. Jiang and the co-operators [84] in Dalian University of Technology
The yield efficiency of H2 produced were approximately 60% and 80% investigated the reactivity of synthesized NiO supported on montmor-
with little CH4 as by-product. However, the H2 yield and the rate of illonite using ethanol as fuel in a fixed-bed reactor. It was found that
reduction decreased during redox cycles. 20Ni–MMT exhibited high H2 selectivity (above 70%) and ethanol
The researchers in university of Leeds have investigated the CLR(a) conversion. The ethanol conversion maintained almost 80% even after
processes using different liquid materials, such as acetic acid [62], 20 cycles. They also investigated the CLR(a) process of glycerol using
sunflower oil [169], glycerol [58] and waste vegetable cooking oil Ni-based oxygen carriers supported on NiAl2O4 [72,82] and Al2O3-
[59,60] to determine the suitability of liquid fuels to maintain steam Montmorillonite with or without Ce promoter [170] as oxygen carriers.
reforming activity under chemical looping reforming conditions. It is The authors found that the CeNi/Al–M–41 displayed the superior
worth noting that when waste cooking oil was used, high purity reactivity and excellent stability due to the strengthened anti-sintering
hydrogen ( > 95%) was produced at 600 °C and 1 atm with the molar and coke capability [170]. The H2 concentration of 90% of the
steam to carbon ratio of 4. The fuel and steam conversion were higher equilibrium value was achieved at 600 °C, and glycerol conversion
when the sorbent material was added. was up to 99% [72]. When CaO was added as a sorbent to remove the
In CLRM process, the modified ferrospinels MFe2O4 (M = Fe, Co or CO2, high-purity H2 of 94.6% is obtained when steam to carbon (S/C)
Ni) were employed as oxygen carrier materials, and they showed was 3 at the initial temperature of 600 °C [82].
promising features for hydrogen production using ethanol or methanol CLR technology can also be used for tar elimination (cleaning) in
as the reducing agent [117–121]. The chemical looping process for biomass-derived gasification gas [143]. In the FR, the oxygen carriers
ethanol reforming over the modified ferrospinels is shown in Fig. 8. not only acts as an oxygen carrier, but also acts as a catalyst for tar
The sintering of magnetite and carbon deposition during redox cycles reforming. The reforming of tars has been tested with the natural ore
[121], the reaction routes and the related reaction mechanism [117] ilmenite [115,143,157,158], synthetic Mn3O4 supported on ZrO2 [157]
together with the reactivity of the mixed ferrospinels [118] during the and NiO supported on α-Al2O3 [77,144] as oxygen carriers. Ni-based
processes of ethanol anaerobic decomposition and oxidation were also materials showed the best catalytic performance with the overall tar
studied. According to the obtained results it can be concluded that, conversion more than 95% at 880 oC [77,144], while the corresponding
compared with magnetite, the Ni ferrite showed a higher activity in value for ilmenite catalyst was 60% at 850 °C [144]. Even though the
ethanol anaerobic oxidation and decomposition [118]. For Co-ferrite, a superior reactivity to convert hydrocarbons, Ni-based materials suffer
complete re-oxidation of CoFe2O4 to its original oxidation state was not from the characteristics of toxic and high price. The alternative
possible using only water as the oxidant; therefore, an extra oxidation materials such as supported Cu-based materials and perovskite
of the material with air was needed [119]. The reaction routes of the La0.8Sr0.2FeO3 were identified as promising bed materials for CLR
anaerobic oxidation of ethanol followed over each material were with C2H4 as a tar surrogate [158]. However, it was found that Cu-
investigated by using in situ DRIFTS-MS method [117]. Results based materials unable to convert aromatics and C2H4 with the
showed that the first step in ethanol transformation appeared to be presence of monoaromatic compounds, while La0.8Sr0.2FeO3 perovskite
supported on γ-Al2O3 achieved high conversion of all tar surrogates
investigated [156].
Different from CLC, the target products in FR of CLR processes are
syngas, therefore, it would be recommended if the oxygen carrier can
react with the solid fuels but not further with the synthesis gas
produced to produce CO2 and water, therefore, it is hard to control
the reaction selectivity to produce syngas. Only few investigations
reported in the literature about the CLR processes using coal as fuel to
produce syngas [122,153,159,160]. Liu et al. [159] investigated coal
Fig. 8. The CLRM of ethanol over modified ferrospinels. A= Fe, Co, Ni or Cu [118].
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gasification using calcium sulfate (CaSO4) in a fixed-bed reactor. It was the H2 to CO equaled to about 2:1. The carbon formation was reduced
found that the CaSO4/C molar ratio should be higher than 0.2 to reach or eliminated by adding 25–30 vol% steam to the natural gas. Except
auto-thermal balance and the corresponding syngas yield is about 1.2 the common gaseous fuels, a liquid fuel, sulfur-free kerosene, has been
moles per mole carbon, respectively. They also observed that the total used for H2 production in this continuous unit with NiO/(MgO–ZrO2)
syngas yield decreased with the present of oxygen carrier due to the as an oxygen carrier [78]. During the experiments lasted for 20 h,
reaction of syngas generated with CaSO4. They also found that CO2 can nearly all hydrocarbon could be reformed into a synthesis gas. In the
promote the reaction between coal and CaSO4 [160]. Guo et al. [122] best case, only 0.01% of the fuel carbon remained as hydrocarbon.
assessed the reactivity of Ca-decorated iron based oxygen carriers with de Diego et al. and the co-operators in Institute of Carboquímica
coal in a batch fluidized-bed reactor for synthesis gas generation. They presented the experimental results obtained in a circulating fluidized
found that when Fe2O3 was used as the oxygen carrier, the volume bed reactor using methane [64] and bioethanol [68] as fuel. The
concentration of the synthesis gas was lower than that without the schematic diagram of the facility is shown in Fig. 10(b). NiO21–γ-
oxygen carrier since iron oxide reacts with the synthesis gas produced Al2O3 and NiO18–α-Al2O3 were used during more than 50 h of
by coal-steam gasification. However, the H2 volume concentration and operation respectively. It was found that in all operating conditions
carbon conversion increased when CaO was added due to the catalytic almost full conversion of CH4 or the bioethanol was achieved, and
effects of CaO. Recently, Siriwardane et al. [135] confirmed that carbon formation was easily avoided. The auto-thermal conditions
BaFe2O4 and CaFe2O4 were excellent for CLR(a) of coal as those two could be obtained by adjust in the NiO to fuel molar ratio. When using
materials had high reactivity with coal but low reactivity with synthesis bioethanol as fuel, a syngas composed of ≈ 61 vol% H2, ≈ 32 vol% CO,
gas. The synergetic effect between steam and the oxygen carriers was ≈ 5 vol% CO2 and ≈ 2 vol% CH4 was reached at auto-thermal
observed. The investigations of hydrogen-enriched gas production from conditions for both materials [68]. A pilot plant up to 140 kW (see
steam gasification using CaO-based materials as a catalyst and oxygen Fig. 10(c)) has been successfully constructed and operated in Vienna
carrier transfer in the chemical looping gasification process has been University of Technology for the CLR(a) of natural gas [38]. Two
reviewed by Udomsirichakorn et al [171]. nickel-based oxygen carriers, NiO/NiAl2O4 with or without small MgO
Considering the biomass, Wang et al. [172] conducted the thermo- added were used as bed materials. Results showed that the FR exhaust
dynamic analysis of syngas generation from biomass based on the gas approached thermodynamic equilibrium. Even though no steam
method of Gibbs free energy minimization with Mn2O3 as an oxygen was added to the natural gas feed no carbon formation was found for
carrier, and the results showed that the total dry concentration of CO global excess air ratios larger than 0.4.
and H2 could reach to 98.8%. García-Díez et al. [173] also conducted As mentioned in Section 3.1.3, CLR technology has also been
the mass and heat balances to determine the auto-thermal conditions proposed for tar elimination (cleaning) in biomass-derived gasification
that maximize H2 production using three different types of bioethanol gas. The researchers in Chalmers University of Technology tested the
as fuel. Results showed that when diluted ethanol (~52 vol%) was used, reforming of tars in a circulated continuous unit (see Fig. 10(d)) with
4.62 mol of H2 per mol of ethanol was obtained and the system could the natural ore ilmenite [143], synthetic Mn3O4 supported on ZrO2
reach the auto thermal state. The CLR(a) process of biomass has been [157] and NiO supported on α-Al2O3 [77,144] as bed materials. It was
demonstrated in TGA [149,152], small batch fixed-bed reactor [152], found that the tar removal efficiency is high than 95% when using Ni-
tube reactor [159], or fluidized-bed reactor [145–147]. It was found based materials, and the matierials maintained the oxygen transfer and
that the iron oxide not only act as a catalyst for biomass tar cracking catalystic properties during the test [77,157].
[149] but also as an oxygen carrier to transfer oxygen. Nevertheless, the Solid fuels such as biomass has been investigated in different
reactivity of lattice oxygen in hematite particles is slightly lower than circulated units. Ge et al. [142,148] investigated the performance of
that of steam [145]. Steam introduction can promote the reforming syngas production process using natural hematite as an oxygen carrier
reactions [147]. A 25 kWth prototype in Southeast University was and biomass as fuel in a 25 kWth interconnected fluidized bed reactor
constructed to investigate the performance of biomass direct CLR(a) (Fig. 10(e)). It was found that when the hematite mass percentages
using hematite as an oxygen carrier [142]. The maximum syngas yield was higher than 40 wt%, the system could reach auto thermal station.
reached to 0.74 Nm3 kg−1 when the gasification temperature was set to The experimental results also showed that 860 °C was the optimal
be 860 °C. Ge et al. [148] carried out the CLR(a) of biomass in a gasification temperature corresponding to higher carbon conversion
25 kWth continuous reactor using natural hematite as an oxygen efficiency and maximal syngas yield (0.74 Nm3 kg−1). The CLR(a) of
carrier. The syngas yield in the continuous reactor reached the biomass was also performed in a 10 kWth interconnected fluidized bed
maximum value of 0.64 Nm3 kg−1 at 850 °C. rector (see Fig. 10(f)) with Fe–Ni bimetallic oxygen carrier in
Guangzhou Institute of Energy Conversion [137]. The composition of
3.1.4. Continuous operation experience of the circulating reactors CO and H2 as well as the gasification efficiency of biomass increased
To investigate the industrial operation of CLR, the different when using Fe–Ni bimetallic oxygen carrier than that using the Fe2O3/
research groups of Sweden, Spain Australia, and China have investi- Al2O3 oxygen carrier. The optimal value of the gasification efficiency
gated the process in different continuous reactors. Chemical-looping reached to 70.48% when the biomass feeding rate was 1.6 kg/h.
processes could be designed in several ways but circulating fluidized Recently, Zeng et al. [151] proposed and investigated a novel chemical
beds are likely to have an advantage over other alternatives since this looping gasification process to generate syngas with high H2/CO ratio.
design provides good contact between gas and solids and allows a As shown in Fig. 10(g), H2 is generated by steam-iron process in the
smooth flow of oxygen-carrier particles between the reactors. The CLR SR, and CO is produced by biomass gasification process in the FR,
processes have been demonstrated at atmospheric pressure not only at therefore, the ratio of can be adjusted. When sawdust was used as fuel
a laboratory scale, but also in continuous units up to 140 kWth pilot and iron ore as an oxygen carrier, the cold gas efficiency of 77.21% and
plant. The summary of CLR circulating reactors are listed in Table 2, the H2 yield of 0.279 Nm3 kg-1 were obtained at the optimized
and the corresponding CLR facilities are shown in Fig. 10. conditions.
Rydén et al. [39] described the continuous chemical-looping
reforming of natural gas in a laboratory reactor. The reactor consisted 3.1.5. System integration and economic analysis
of two interconnected fluidized beds, which is shown in Fig. 10(a). The economic analysis of CLR(a) process has been conducted at
NiO-based oxygen carriers supported on NiO/MgAl2O4 [39], Al2O3(α- atmospheric and pressurized conditions [174–176]. The calculation
Al2O3 or γ-Al2O3) [63] NiO/Mg–ZrO2 [75] were used as oxygen results showed that pressurized CLR(a) potentially has very high
carriers. Complete conversion of natural gas was achieved in the FR efficiency. The efficiency could be at least 4% higher than that for the
and the selectivity towards H2 and CO was high and the mole ratio of conventional steam reforming with CO2 capture by amine scrubbing.
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Table 2
Summary of CLR circulating reactors.
Location Unite size Configuration Fuel Oxygen careers Operation time References
(kW) (h)
Chalmers University of Technology, Chalmers, 0.1–0.3 AR-fluidized bed n.g. NiO/MgAl2O4 41 [39]
Sweden FR-fluidized bed NiO/Mg–ZrO2 24 [75]
NiO/MgAl2O4, NiO/α-Al2O3, 160 [63]
NiO/γ-Al2O3
kerosene NiO/(MgO–ZrO2) 20 [78]
Institute of Carboquímica, ICB–CSIC, Spain 0.9–1 AR-bubbling CH4 NiO/γ-Al2O3, > 50 [64]
fluidized bed Bioethanol NiO/α-Al2O3 > 50 [68]
FR-bubbling
fluidized bed
Vienna University of Technology, Vienna, 120–140 AR-fast fluidized bed n.g. NiO/α-Al2O3, NiO/(α-Al2O3– > 90 [38,74]
Austria FR-turbulent MgO)
fluidized bed
Chalmers University of Technology, Chalmers, n.a. AR-circulating Raw gas from Ilmenite ore n.a. [143]
Sweden fluidized bed biomass gasifier Mn3O4/MgZrO3 n.a. [157]
FR-bubbling NiO/α-Al2O3 7 [77]
fluidized bed Ilmenite, NiO/α-Al2O3 8 [144]
Southeast University, Nanjing, China 25 AR-high velocity Rice husk Natural hematite n.a. [142,148]
fluidized bed
FR-bubbling
fluidized bed
Guangzhou Institute of Energy Conversion, 10 AR-fast fluidized bed Sawdust of pine Fe–Ni bimetallic (Fe2O3/ n.a. [137]
Chinese Academy of Sciences(CAS), FR- bubbling Al2O3/NiO = 7/3/0.53 as mass
Guangzhou, China fluidized bed raion)
Southeast University, Nanjing, China n.a. FR-fast fluidized bed Pine sawdust Iron ore n.a. [151]
SR- bubbling
fluidized bed
The reformer efficiency above 81% is possible if the oxygen carrier the conventional fired tubular reforming (FTR) with CO2 capture
particles have high stability at the temperature as high as 1200 °C. The technology (MDEA absorption method). The cost of H2 production
reactivity of two Ni-based oxygen carriers under pressurized conditions also reduced from 0.28 €/Nm3H2 to 0.19 €/Nm3H2.
during the CLR(a) process was confirmed by Ortiz et al [66]. It was He et al. [128,179] proposed a hybrid solar-redox scheme (Fig. 11).
found that at all operating pressures the CH4 conversion was very high Both the liquid fuel and hydrogen are produced from methane and
( > 98%) and no carbon formation was detected. integrated solar energy in two redox steps based on CLRM process. In
Note that the CLR(a) under pressure conditions also face some the Reducer, methane is partial oxidized by the material (Fe3O4–LSF)
problems before this can be realized. Firstly, the fuel conversion is into CO and H2, which is then converted into naphtha and diesel in the
thermodynamically hampered by pressure so the FR temperatures of Fischer–Tropsch (F–T) reactors. In the Oxidizer, steam oxidizes the
1000 °C or higher will be required to obtain sufficient conversion of the reduced material from the previous step, producing concentrated H2.
fuel [174]. Integration with a gas turbine is indispensable in order to The overall process efficiency is estimated to be 67.5% (HHV), which is
obtain high efficiency. Otherwise there would be a large efficiency 7.7% (HHV) more efficient than SMR based co-production processes.
penalty for air compression. Secondly, the pressurized circulating The methane to fuel efficiency from the hybrid solar-redox process is
fluidized beds are not conventional technology. Hence the pressurized estimated to be 99.4% on an HHV basis [179].
CLR(a) technology needs further development to be used in industrial There are few investigations about the CLR(s) process. Pans et al.
process. [36] conducted the evaluation of the two configurations using iron-
da Silva et al. [177] analyzed the performance of a PEMFC (proton based oxygen carriers based on the mass and enthalpy balances. The
exchange membrane fuel cell) system integrated with a biogas CLR(a) results showed that a H2 yield value of 2.45 mol H2 per mol of CH4 can
processor. Compared with conventional process, the results showed be obtained with the reformer tubes located inside the AR. This
that CLR(a) process can achieve high advantages when integrated with corresponds to a CH4 to H2 conversion of 74.2%, which is similar to
a PEMFC system. CLR(a) can be seen as an advantageous reforming state-of-the-art H2 production technologies, but with inherent CO2
technology, not only because it allows that the global process can be capture in this process. Rydén et al. [175,176] evaluated the economy
operated under auto-thermal conditions but also due to that it allows of CLR(s) process. It was found that CLR(s) process also seems well
the PEMFC stack to achieve values of voltage and power closer to those suited for large scale production of high purity H2 with CO2 capture.
obtained when SR fuel processors are used. The global efficiency This concept utilizes conventional technology and moderate tempera-
obtained for fuel processors based on CLR(a) technology is close to ture and pressure, and may be easier to put into practice than CLR(a).
those achieved by conventional fuel processors. At low loads, efficiency An overall efficiency in the order of 80% seems possible.
is around 45%, whereas, at higher power demands, efficiencies around
25% are calculated for all the fuel processors.
Spallina et al. [178] proposed a membrane assisted chemical 3.2. Chemical looping hydrogen production
looping reforming (MA-CLR) system for pure H2 production. In this
system, the natural gas is converted in the FR by reaction with steam Fuel cell technology can convert chemical energy into electrical
and an oxygen carrier, and the produced H2 permeates through the energy with high efficient without emissions of environmental pollu-
membranes for separation. Techno-economic assessment of the con- tants, which makes fuel cells one of the most promising sources for
cept showed promising results. The H2 production efficiency of the future power generation. The carbon monoxide level in the gas has to
MA–CLR system was above 90%, which was 30% higher than that of be reduced to a level below 20 ppm in order to avoid poisoning of the
catalyst at the fuel cell electrodes [180–182]. Therefore, high-purity
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(a) 100W CLR for natural gas, (b) 900W CLR for CH4,
Chalmers University of Technology, Sweden [39]. Institute of Carboquímica, Spain [64].
(c) 140kW CLR for natural gas, (d) CLR for raw gas from biomass gasifier,
Vienna University of Technology, Austria [38]. Chalmers University of Technology, Sweden
[157].
(e) 25kW CLR for biomass, (f) 10kWth CLR for biomass,
Southeast University, China [142]. Southeast University, China [137].
hydrogen is required in the fuel cells, such as polymer electrolyte fuel Iron has long been known to produce H2 when reacted with steam.
cells (PEFCs). At present, more attention is paid to the steam-iron In 1910, Messerschmitt [187] patented the steam-iron process for
process because it can produce hydrogen with high purity [183–186]. producing hydrogen using the Fe3O4 to Fe0.947O transition. In recent
The high purity hydrogen with the concentration of CO lower than years, the steam-iron process again gets attention because of the
5 ppm can be produced using CLH process [186]. potential to produce H2 with inherent CO2 separation.
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Fig. 12. The schematic diagram of the chemical looping hydrogen production.
The schematic of CLH process is shown in Fig. 12. In the FR, the low conversions for both reducing gas and steam are limited by the
reducing gases reduce the metal oxide (MO) to the metal form (M) thermodynamic property of the FeO and Fe3O4 phases. The two-reactor
according to reaction 19, releasing water vapor and carbon dioxide: steam-iron arrangement can be modified by adding an AR [188,190].
The schematic diagram of the three-reactor CLH system is shown in
MO + CO/H2 = M + CO2/H2O (19)
Fig. 12(b). In the third reactor AR, Fe3O4 is subsequently regenerated
The reduced metal particles are transported to the steam oxidation to Fe2O3 by oxidizing oxygen in air. Final oxidation in air has the
reactor and react with steam according to reaction 20, producing potential to oxidize any contaminants, e.g. carbon or sulfur, deposited
hydrogen and metal oxide particles. The regenerated metal oxide can on the particles, and the produced Fe2O3 can increase the conversion of
be used in another redox cycle. reducing fuels.
The possible reactions in the three reactors when coupling the
M + H2O = MO + H2 (20) gasification process are listed as follows [186]:
If the fuel can be fully converted, the flue gas from the FR will be Under the CO2 conditions, the coal gasification occurs as
CO2 and H2O. The exhaust gas form the steam oxidation reactor is only C+CO2 = 2CO-172·4 kJ/mol (21)
the mixture of H2 and water vapor. Almost pure CO2 and H2 can be
obtained from the outlet of the FR and the SR only with water The reductions of Fe2O3 with CO, a major component in syngas,
condensed. In general, the advantages of the CLH process can be occur by
classified as follows:
3Fe2O3+CO = 2Fe3O4+CO2+43·2 kJ/mol (22)
1) No water gas shift reactor and CO2 separation process are needed;
0·947Fe3O4+0·788CO = 3Fe0·947O+0·788CO2-37·3 kJ/mol (23)
2) Only one kind of oxygen carrier is required compared to the
complex solid catalysts in SMR process; Fe0·947O+CO = 0·947Fe+CO2+16·7 kJ/mol (24)
3) No further hydrogen purification process is needed due to the
highly concentrated of hydrogen. The produced Fe or Fe0.947O can be oxidized by steam to generate
hydrogen
CLH process is also called “Chemical Looping Steam Reforming
0·947Fe+H2O = Fe0·947O+H2+23·8 kJ/mol (25)
(CLSR)”, “Chemical looping water splitting (CLWS) process” or
“Chemical storage of hydrogen process” in some literature.
3Fe0·947O+0·788H2O=0·947Fe3O4+0·788H2+69·2 kJ/mol (26)
The traditional steam-iron process mainly focused on hydrogen
production and could only partially convert the reducing gas [189]. The In the air reactor, Fe3O4 can be reoxidized to Fe2O3
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Table 4
Summary of the oxygen-carriers tested in different CLH processes.
Fe2O3 – MM CO PB [186]
Fe2O3 – MM Syngas produced form PB [197]
in situ coal/coal char
gasification
Fe2O3 – WG H2, CO bFB [198]
Fe2O3 – MM Char, K–char, Ca–char bFB [199]
Fe2O3 – MM H2, CO PB [200]
Fe2O3 – MM CO TGA [201]
(i) Fe2O3 – CAM H2, CH4 ETB [202]
(ii) NiFe2O4
(iii) CuFe2O4
(i) Fe2O3 – (i)–(ii) UH H2+CO CT [203]
(ii) Fe2O3–M(M= CeO2, La2O3, Ce0.5Zr0.5O2) (iii) UH+IMP
(iii) M–( Fe2O3–Ce0.5Zr0.5O2), M=Cu, Mg, Cr, Mo, M/(
Fe2O3–Ce0.5Zr0.5O2+M)=0.02, 0.05 as the weight ratio
(i) Fe2O3 (i) None (i) MM CO PB [204]
(ii) Fe2O3(x = 60, 80, 90 wt%) (ii) Al2O3 (ii) SG
(i) Fe2O3 – (i) PUR H2,H2+CH4 TGA, FxB [205]
(ii) 98 wt% Fe2O3–1.90 wt% Al2O3–0.10 wt% MoO3 (ii)–(v) SG
(iii) 98 wt% Fe2O3–1.75 wt% Al2O3–0.25 wt% MoO3 (vi) WIMP
(iv) 98 wt% Fe2O3–1.50 wt% Al2O3–0.50 wt% MoO3
(v) 98 wt% Fe2O3–1.75 wt% Al2O3–0.25 wt% CeO2
(vi)97.79 wt% Fe2O3–1.75 wt% Al2O3–0.20 wt% MoO3–
0.25 wt% CeO2
(i) Fe2O3 (i)None SG CO+H2 TGA, FxB [206]
(ii) 60 wt% Fe2O3 (ii)–(iii)Al2O3
(iii) xFe2O3–5 wt% CeO2(x = 45, 55, 65 wt%)
(i) Fe2O3 – (i)–(ii) MM CO TGA, MR [207]
(ii) La0.7Sr0.3FeO3–δ(LSF731) (iii)–(iv) MM
(iii) LSF731–xFe2O3 (x = 11, 30 wt%) +PEC
(i) Fe2O3, – (i) WG H2, CO TGA, bFB [208]
(ii) xCaO–Fe2O3, nFe2O3/nCaO=50, 57.3% and 66.7% (ii) WG+MM
(Fe2O3)1–x–(Ce0.5Zr0.5O2)x (x = 0, 0.5, 0.7, 1.0) – COP Syngas produced form two-layer [209]
in situ methane partial reactor
oxidation
(i) 15 wt% Fe2O3 LaNiO3 CAM, IMP CH4 FxB [210]
(ii) 15 wt% Fe2O3–5 wt% CeO2
20 wt%Fe2O3 ZrO2 COP CH4 MB [211]
20 wt% Fe2O3 ZrO2 COP CH4 cFB [212]
30 wt% Fe2O3 Al1.42Mg0.58O2.7 MM CH4 TGA [213]
(i) 40 wt% Fe2O3 (i) ZrO2 PEC CO PB [214]
(ii) Ca2Fe2O5 (ii) None
xFe2O3 (x = 50, 60, 75, 80, 90, 100 wt%) α-Al2O3 COP H2, CO TGA [215]
50 wt% Fe2O3 MgAl2O4 SG CH4, CO FxB [216]
xFe2O3 (x = 60, 70, 80, 90 wt%) α-Al2O3 COP H2 TGA [217]
60 wt% Fe2O3 Al2O3 MM CO PB [218]
60 wt% Fe2O3 Al2O3 MM CO TGA [219]
60 wt% Fe2O3 (i)TiO2 (i)–(ii) SSM H2, CH4, CO TGA [220]
(ii)La0.8Sr0.2FeO3
60 wt% Fe2O3 (i)Al2O3 SSM char TGA [221]
(ii)13 wt% CuO–Al2O3
(i) 60 wt% Fe2O3 Bentonite MM H2, CO bFB [222]
(ii) 60 wt% NiO
(iii) 30 wt% NiO–30 wt% Fe2O3
(i) xFe2O3 (x = 60, 90 wt%) (i) Al2O3 MM CO TGA, bFB [223]
(ii) 60 wt% Fe2O3 (ii) TiO2
70 wt% Fe2O3 Al2O3 SG H2, Syngas, CH4 TGA, FxB, [193,224,225]
cFB
85 wt% Fe2O3 xSiO2+ yCaO +5 wt% Al2O3 (x+y = MM H2 CT [226]
10 wt%, x=0, 2.5, 5, 6.5, 7.5, 8.5,
10 wt%)
90 wt% Fe2O3 Al2O3 MM H2, syngas TGA, pFxB [227]
90 wt% Fe2O3 Al2O3 MM H2 pFxB [228]
90 wt% Fe2O3 Al2O3 PUR CO bFB [229]
90 wt% Fe2O3–5 wt% Al2O3–5 wt% CeO2 – COP H2+CO pFxB [230]
98 wt% Fe2O3–1.75 wt% Al2O3–0.25 wt% CeO2 – SG Bio-fuels FxB [231]
Mo–(80 wt% Fe2O3–20 wt% Ce0.5Zr0.5O2), x = 1–5 wt% – UH+IMP H2 TGA, MR [232]
Mo–(80 wt% Fe2O3–20 wt% Ce0.5Zr0.5O2), x = 1–5 wt% – UH+IMP H2 MR [233]
98 wt%Fe2O3+1.75 wt%Al2O3+0.25 wt% CeO2 – SG Methanol FxB [234]
N–M, N= Fe2O3, Fe, M = Al, Cr, Ni, Co, Zr, Mo, M/(Fe+ M) – IMP H2 FxB [235]
= 0.05 as mole ratio
(continued on next page)
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Table 4 (continued)
Fe2O3–Mo, Mo/(Mo + Fe) = 0.00, 0.05, 0.08, 0.10 as mole – HS H2 FxB [236]
ratio
Fe3O4b M=Al2O3, Cr2O3, MgO, SiO2, nM/( WIMP CO PB [237]
nM+nFe)=0.01, 0.1, 0.3
Fe3O4b
(i) – (i) P H2 FxB [184]
(ii)M– Fe3O4b(M= Al, Cr, Zn, Ga, V, Ti, Zr, Mg, Ca, Mn, Co, (ii) COP
Ni, Cu, Y, Nb, Mo, Ce), molar ratio: M/( M+Fe) =0.03
(i) Fe3O4b – (i) P H2 FxB [183]
(ii)M– Fe3O4b(M= Al, Sc, Ti, V, Cr, Y, Zr, Mo, Ce, Mn, Co, (ii) COP
Ni, Cu、Zn, Ru, Rh, Pd, Ag, Ir, Re, Ta, W, Pt, Ga, Nb),
molar ratio: M/( M+Fe) =0.03
(i) Fe3O4 (i)None COP H2 FxB [238]
(ii) 60 wt% Fe3O4 −10 wt% CeO2 (ii)–(ix)ZrO2
(iii) 1 wt% Rh – 59 wt% Fe3O4 −10 wt%CeO2
(iv) 1 wt% Cu – 59 wt% Fe3O4 −10 wt%CeO2
(v) 3 wt% Cu – 57 wt% Fe3O4 −10 wt%CeO2
(vi) 5 wt% Cu – 55 wt% Fe3O4 −10 wt%CeO2
(vii) 3 wt% Cu – 57 wt% Fe3O4 −20 wt%CeO2
(viii) 3 wt% Cu – 57 wt% Fe3O4 −30 wt%CeO2
(ix) 10 wt% Cu – 50 wt% Fe3O4 −10 wt%CeO2
(i) 37 wt% Fe3O4b ZrO2 ALD Synthesis gas SFR [239]
(ii) 37 wt% CoxFe3−xO4
40 wt% Fe3O4b (40 wt% Fe–BHA) Barium hexaaluminate(BHA) SG Synthesis Gas FxB [240]
60 wt% Fe3O4b MgAl2O4 FG CO, Synthesis gas cFB [241]
(i) (0.045–0.45 mol%)Pd– Fe3O4b – IMP H2 TEOM [242]
(ii) (0.0065–0.38 mol%)Zr– Fe3O4b
(ii) Pd–Zr –Fe3O4b ( content of (Pd+Zr) is 0.23 mol%).)
(i) FeOx – (i) P CH4 FxB [185]
(ii) 5 mol% M–FeOx(M= Cr, Ni) (ii)–(iv) COP
(iii)5 mol%M–5 mol% Cr–FeOx(M=Co, Ni, Cu, Rh, Pd, Ir,
Pt)
(iv) 5 mol% Ni–5 mol% M–FeOx(M=Al, Ti, V, Cr, Zr)
(i) M–FeOx (M= Rh, Mo), M/(M+Fe) =0.05 as mole ratio – COP H2 FxB [243]
(ii) Rh–Mo–FeOx, Rh/(Rh+Mo+Fe)=Mo/(Rh+Mo+Fe)
=0.05 as mole ratio
(i) M–FeOx(M=Cr, Cu), (M/(M+Fe) =0.05 as mole ratio) – COP H2, synthesis gas, PB [244]
(ii) M–Cr–FeOx(M=Co, Ni, Rh, Cu), M/(M+Cr+Fe) =0.05 methane
as mole ratio
(iii) Ni–M–FeOx(M=Al, Cr, Zr, Mo) M/(M+Ni+Fe) =0.05
as mole ratio
NiFeAlO4 – SSM CO, H2 TGA, FxB [245]
NiFe2O4 – (i) SC CO, H2+CO TGA, FxB [246]
(ii) COP
(iii) HS
(iv) SG
Laboratory iron ore – MM H2, CO TGA [247]
Ilmenite and three iron ores – – Heavy fraction of bio-oil TGA, FxB [248]
Austrian MAC iron ore – – Bio-oil cFB [249]
xKNO3–iron ore(x = 0, 3, 6, and 10 wt%) – IMP CO bFB [250]
a
Key for preparation method: ALD: atomic layer deposition; CAM: citric acid method, COP: coprecipitation, DP: deposition-precipitation, DIS: dissolution, FG: freeze granulation,
HIMP: hot impregnation, HS: hydrothermal synthesis, IMP: impregnation, MM: mechanical mixing, P: precipitation, PE: pelletizing by extrusion, PEC: Pechini, SC: solution
combustion, SD: spray drying, SF: spin flash, SG: sol-gel, SP: spray pyrolysis, SSM: solid state method; WG: wet granulation, WIMP: wet impregnation, UH: urea hydeolysis.
c
The initial state was Fe2O3 in the fresh iron oxide samples, but the second and subsequent redox reactions were performed between Fe3O4 and iron metal.
b
Key for reactor type: FxB: fixed bed, pFxB: pressurized fixed bed, TGA: thermogravimetric analyzer, bFB: batch fluidized bed, cFB: continuous fluidized bed, TEOM: Tapered
element oscillating microbalance, ETB: Electronics thermobalance, PB: packed bed, MR: microreactor, CT: ceramic-tube, MB: moving bed reactor. SFR: stagnation flow reactor.
reduction performance of the iron oxide with H2 and also the could suppress the sintering, and increase the reactivity of the
reoxidation performance of the reduced iron oxide with water at low materials during the redox reactions, and the property of inhibiting
temperatures ( < 400 °C). The additives moderated the sintering of iron the carbon deposition has also been confirmed [206]. Liang et al.[210]
oxide markedly with repeated redox cycles. After that, they [183] found that the addition of CeO2 in Fe2O3/LaNiO3 promoted the
examined the effects of 26 metal additives in the iron-steam process at stability of the oxygen carrier for H2 production during the 100
a temperature range of 373–873 K. Among the 26 metal elements successive cycles.
examined as additives, Al, Mo and Ce could effectively enhance the
stability and reactivity of Fe/Fe3O4 material during the repeated cycles. The inclusion of 7.5 wt% SiO2, 5 wt% Al2O3 and less than 2.5 wt%
Co-addition of Mn, Co, Ni, Cu, and Zn worsen the reoxidation CaO was found to hinder the sintering to a large extent [226]. Rihko-
performance from the first cycle, while the addition of Ru, Rh, Pd, Struckmann et al. [203,232,233] found the Mo species improved the
Ag, Ir, and Rt could enhanced the rate of reoxidation at the first cycle stability of Fe2O3–Ce0.5Zr0.5O2 during the redox cycles. The materials
but unable to prevent the deactivation after that. Galvita et al. showed superior stability compared to those doped with Cu or Mg
[209,252] also found that when Ce was added to the iron oxide, it
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additives [203]. The positive effect of Mo has been confirmed by Wang adding small amount of promoters. As mentioned above, it is advanta-
et al. [235,236]. They found the addition of Mo not only decreased the geous to improve the hydrogen production capacity if the iron-based
temperature of water decomposition significantly, but also improved oxygen carrier is reduced to Fe0.947O or Fe, therefore, achieving deep
the stability of the samples during repeated redox cycles. A clear reduction of the oxygen carrier is a challenge for the CLH process. Liu
decrease in the activation energy was also concluded for the steam et al. [250] modified the iron ore using KNO3 and found that the K-
oxidation process when using iron oxide samples containing Mo. decorated iron ore not only could promote the reduction rate and
Romero et al. [205] also found out, that for a mixed oxide with the hydrogen production, but could weak the carbon deposition when
composition of 98 wt% Fe2O3–1.75 wt% Al2O3–0.25 wt% MoO3 main- using CO as fuel. Mixed oxides can also be used to increase the fraction
tained a slightly better hydrogen production rates than that of the of steam to hydrogen and promote the corresponding hydrogen yield,
cerium sample. such as Ca–Fe–O system [214,255] and the perovskite La0.8Sr0.2FeO3-δ
The temperature of the reaction needs to be higher than 1023 K (LSF) [127]. It was found that the equilibrium conversion of steam to
when methane is used as reducing agent. To increase the reactivity of hydrogen reached to 75% when using Ca2Fe2O5 at 1123 K, which is
the oxygen carrier with methane at relatively lower temperatures and higher than the theoretically achievable value of 62% when using iron
increase the stability of the material during the cyclic processes, oxide [214]. LSF–promoted iron oxide is shown to be capable of
Takenaka et al. [185] modified iron oxide with both Ni and Cr species. converting over 77.2% steam into H2 during redox processes [127].
Addition of Ni to iron oxides enhanced the reduction with methane and
the subsequent oxidation with water vapor at low temperatures, but Ni 3.2.1.3. Iron ore with iron oxide contained. Most of the work in the
species promoted the sintering of iron species. Addition of Cr cations to literature on oxygen carrier development of CLH process has focused
iron oxides prevented the sintering of iron species. In contrast, the iron on finding synthetically produced particles. Compared to synthetic
oxides containing both Ni and Cr species (denoted as Ni–Cr–FeOx) oxygen carrier particles, the use of natural minerals can decrease the
with the amount of each metal adjusted to 5 mol%, they found that cost of the operation. Kindermann et al. [247] investigated the
pure hydrogen could be generated repeatedly and the modified feasibility of the industrial iron ore in the reformer sponge iron cycle
material maintained the reactivity during the redox cycles at tempera- (RESC) process. They found that the porosity of the particles decreased
tures < 923 K. Urasaki et al. [242] tested the performance of the iron with the operation of the process, but the porosity would keep stable
oxide modified with very small amounts of Pd and/or Zr in the steam- during 5 redox cycles when the amount of SiO2 was high. Xiao et al.
iron reaction at the temperature of 723 K. Results showed that the [248] compared the reactivity and the ability to inhibit or minimize
addition of Pd or Zr with only 0.23 mol% in the iron oxide suppressed carbon deposition of four iron-based oxygen carriers including an
the sintering of iron oxide during the cyclic process. Palladium ilmenite and three iron ores in TGA and fixed bed reactor. Results
accelerated both the reduction and oxidation rates of partially reduced showed that the ilmenite had superior reactivity to minimize the
iron oxide, while zirconia increased only the oxidation rate. Addition of carbon deposition or Fe3C formation in the reduction process.
both palladium and zirconia together to the iron oxide resulted in However, the reactivity and H2 production capacity of ilmenite also
marked enhancement of both reduction and oxidation. decreased during 15 cycles. Recently, the Australian MAC iron ore was
Takenaka et al. [243] modified the iron oxide using Mo and/or Rh used as an oxygen carrier for hydrogen generation from nonaqueous
species. It was found that the addition of Rh species to iron oxides bio-oil in a dual circulated fluidized bed [249]. It was found that the
decreased the apparent activation energy of the hydrogen production hydrogen yield and purity declined with the cycling time, but adding
process and enhanced the formation of hydrogen at low temperatures some steam in FR was a promising approach to mitigate the oxygen
through the oxidation of iron metal with water vapor. However, Rh carrier deactivation.
species in iron oxides promoted sintering of iron species during the
redox. The addition of Mo cations to Rh–FeOx prevented the sintering
of iron species during the redox. The Rh–Mo–FeOx achieved high
stability and could produce hydrogen repeatedly through the redox. 3.2.2. Chemical looping hydrogen production using solid and liquid
They [244] also modified the iron oxides containing Cr cations. fuels
Addition of Cu, Ni or Rh to iron oxides containing Cr cations enhanced As shown in Table 3, CO, H2, syngas or natural gas (mainly CH4) is
the formation rate of hydrogen through the oxidation with water vapor commonly used as a reducing agent in CLH process, and only few
at 573 K. Ni–Cr–FeOx and Cu–Cr–FeOx as well as Rh–Cr–FeOx are investigations use solid fuels. Because the gas fuel supply cannot fully
promising oxygen carriers for pure hydrogen repeatedly through the support the energy needs of the electricity demand of the country for
redox. the long-term, it would be highly advantageous if the CLH process
Peña et al. [202] conducted the kinetic study of different metallic could be adapted for solid fuels. There are basically two approaches to
oxides, either alone (Fe2O3) or as mixed oxides (NiFe2O4, CuFe2O4) in the application of the CLH technology with solid fuel. The first one is to
a TGA system. The experimental results showed that the addition of a gasify the solid fuel firstly in a gasifier unit with pure O2 to produce
second metal to form double oxides exhibit greater reaction rates. Liu syngas, and then it can be used in a CLH process with gaseous fuel. The
et al. [246] and Kuo et al. [245] also found the self-supported NiFe2O4 second one is to add the solid fuel directly to the FR with the
oxygen carrier showed a good hydrogen production capacity and a high gasification agents, where the gasification and the combustion pro-
recovery degree of lattice oxygen. Jin et al. [222] found that when NiO cesses occur simultaneously.
was added into the Fe2O3/Bentonite particles, the (NiO: Fe2O3)/ Müller et al. [197] conducted the experiments to produce hydrogen
bentonite particle represented better reduction reactivity and stable from three representative coals - a Russian bituminous, a German
water splitting reactivity up to 7th cycle. He et al. [221] also found that lignite and a UK sub-bituminous coal. When German lignite was used,
adding a small amount of CuO to an iron-based oxygen carrier pure H2 with CO < 50 ppm could be obtained from the proposed
improved the reactivity of the oxygen carrier for solid fuel conversion. process. Stable quantities of H2 were produced over five cycles for all
Other bi-metallic systems have also been studied where cobalt, three coals investigated. Independent of the fuel, the produced H2 was
manganese or zinc were mixed together with iron [253,254]. These not contaminated with SO2. It was demonstrated that the CLH process
systems were found to be active at high temperature ( > 2000 °C) and may be an attractive approach to upgrade crude syngas produced by
consequently, but they present little interest when dealing with classic the gasification of low-rank coals to pure H2 while simultaneous
process conditions. capturing CO2.
Besides the stability and the reactivity of the CLH process, the Yang et al. [199] confirmed the feasibility of the hydrogen produc-
hydrogen generation capacity of the material can also be improved by tion using direct CLH process with coal char as fuel in a fluidized-bed
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reactor. The reduction of Fe2O3 by K–10–char at 1073 K was desirable low attrition and absence of defluidization were achieved during the
from the perspective of the carbon conversion rate and high concen- operation process, and it is estimated that the process can be success-
tration of CO2. The carbon in char was completely converted to CO2 fully obtained in a continuous three-reactor system.
when the mass ratio of Fe2O3/K–10–char was increased to 10/0.3. The A 25 kWth subpilot CLH unit (see Fig. 14) using syngas as fuel has
oxidation rate of K–10–char by Fe2O3 without a gasifying agent was been constructed and operated in the OSU using synthetic iron-based
comparable to the K–10–char steam gasification rate. The H2 yield oxygen carriers [224,225]. The H2 purity higher than 99.99% with
equaled to 1000 mL/g K–10–char could be obtained when 3 g of Fe2O3 100% syngas conversion has been achieved in this sub-pilot unit.
and 0.5 g of K–10–char was added. A 300 Wth three reactor CLH unit with CH4 as fuel was constructed
The development of solid fuel direct CLH process may be limited. and successfully operated for 13 h using 20 wt% Fe2O3/ZrO2 as an
This is because the lower reactivity between the oxygen carrier and the oxygen carrier [212]. Both of the FR and SR operated at the moving
solid fuel due to the low solid-solid contact efficiency. In the FR of CLC, bed state with the riser operated as an entrained flow reactor. In the
steam or CO2 cannot added as the gasifying agent to promote the FR, the average conversion of CH4 was 94.15% and the almost pure
reaction rate and inhibit the carbon deposition. However, in the CLH hydrogen (99.95%) was obtained in the SR.
process, this is not recommended. The reduced oxygen carrier may be Recently, hydrogen was also successfully produced from nonaqu-
partially oxidized by the gasifying agent, therefore the capacity of eous bio-oil in a dual circulated fluidized bed (see Fig. 15) using iron
producing H2 will be diminished. The conversion of the reducing ore as an oxygen carrier in Southeast University [249]. The operation
agents will also be affected, which has been verified by Yang et al. [199] results showed that the hydrogen purity remained not desirable due to
and Zeng et al.[249]. the low carbon conversion of the oil. Adding steam in FR could enhance
Up to now, there is few report on CLH process using liquid fuel. The the hydrogen purity by eliminating the solid carbon, but it also
biofuels with the advantage of being renewable feedstock are evaluated suppressed the hydrogen yield simultaneously. When the steam to oil
as possible candidates. The light [231] or heavy [248] fraction of bio-oil ratio was set to be 1.5 and the temperature of FR was 950 °C, the
has been used as fuels for hydrogen production in CLH process. hydrogen purity reached to 96% with the yield of 635 mL/mL oil.
Hydrogen was also successfully produced from nonaqueous bio-oil in
a dual circulated fluidized bed using Australian MAC iron ore as an 3.2.4. System integration and economic analysis
oxygen carrier [249]. When the steam to oil ratio was set to be 1.5, the The system integration and economic analysis are also the focus of
hydrogen purity reached to 96% with the yield of 635 mL/mL oil. Other the CLH process. Different systems for hydrogen production or/and
liquid fuels as mentioned in CLR(a) can also be used as reducing power generation has been proposed using the gaseous fuels, such as
agents, which needs to be further investigated. CH4 [213], nature gas [272,273], and even the ventilation air methane
[270]. Simulation results showed that the cold gas efficiency, the
effective thermal efficiency, and the carbon capture efficiency was
3.2.3. Continuous operation experience of the circulating reactors much higher than that of the conventional SMR process [272].
Up to now, only limited amount of studies on the continuous Considering the three streams of N2, H2 and CO2 produces in chemical
operation of CLH process have been reported. Reed [256] developed a looping process, Edrisi et al. [273] recently proposed a novel and green
process with interconnected fluidized beds for circulating iron oxides. plant configuration for urea production using the CLH process to
This enabled continuous production of H2. Rydén et al. [241] examined provide the feedstock of urea synthesis loop. The schematic figure of
the steam-iron reaction in a continuously circulated two-reactor the proposed plant and conventional process is shown in Fig. 16. In
fluidized-bed reactor. The schematic description of the reactor is this process, CLH process is used to produce the pure steams of H2 and
similar to that shown in Fig. 10(a). Fe3O4/MgAl2O4 was used as the N2 for ammonia production and CO2 for urea synthesis. The system is
oxygen carrier with carbon monoxide or synthesis gas as fuels. The simplified and therefore the economic has promising advantage than
process operated for 12 h with 9 h involved H2 generation. They that of the conventional process. Economic evaluation of the proposed
demonstrated that the conversion of gaseous fuel was at the range of plant showed a considerable rate of return (IRR) and financial interest.
60–80% with the H2 production rate of 0.33–0.58 L/min depending on The proposed plant had an IRR above 28%, whereas the corresponding
the fuel added and the reaction temperature. H2 was produced value of conventional plants was about 20%.
continuously as is shown in Fig. 13 when syngas was used as reducing There are also two ways of system integration with CLH process
fuel. It should be noted that despite reduction of the oxygen carrier to using solid fuels. One is to couple with fuel gasification process,
FeO, de-fluidization or stops in the solid circulation were not experi- another way is to direct use solid fuels.
enced, which is not as the case in CLC process [257]. Stable operation, Coal gasification process is a promising technology for clean coal
power generation process. The integrated hydrogen and power tech-
nology by firstly gasify the coal to syngas not only can increase the
power generation efficiency, but also can solve the problem of NOx and
SOx emission. This technology can also separate the carbon dioxide
when combined with CLH process. The basic schematic figure of the
CLH process combine the solid fuel gasification is shown in Fig. 17
[259]. The CLH processes in conjunction with solid fuel gasification
process using different gasification agents, such as steam [258], O2
[191], O2 and CO2 mixture [262], O2 and steam mixture [260,261,265],
and even the hydrogen produced [266,267] has been proposed and
simulated. As shown in Table 5, the system performance including the
energy efficiency, the total exergy efficiency, and the carbon capture
efficiency compare favorably with to those achieved by hydrogen
production via steam reformation of methane.
CLH process also has been integrated with other new technologies
for power generation and/or hydrogen generation. Chen et al. [265]
proposed a system which integrated the coal gasification, CLH process,
Fig. 13. Dry-gas concentration from the steam reactor with synthesis gas as fuel at and solid oxide fuel cell/gas turbine (SOFC/GT) cycle. The produced
900 °C [241]. hydrogen from the CLH process is fueled to SOFC for power genera-
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Fig. 14. Schematic diagram of the SCL process in mechanical (a) and non-mechanical (b) valve configuration [225].
Fig. 17. Simplified schematic of the syngas chemical looping process for hydrogen
production from coal [259].
Fig. 15. The schematic of the experimental set-up [249].
Fig. 16. Scheme of the proposed plant and conventional process for urea production from natural gas [273].
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Table 5
Summary of systems integration with CLH process.
M. Luo et al.
Chemical-looping and gasification system Coal Fe2O3 CLH in conjunction with a steam-coal gasification process. The peak exergetic efficiencies of the fully heat-integrated [258]
systems reached to 48.4% and 58.3% at 1 atmosphere and
10 atmospheres respectively, and the values could reach to
53.7% and 59.7% respectively when a bottoming steam
turbine cycle was set for waste heat utilization.
Syngas chemical looping process for hydrogen Coal Fe2O3 Integration of the syngas redox (SGR) process into the coal The overall efficiency of the process was 64% (HHV) with [191,259]
production from coal gasification train to produce high purity hydrogen. 100% carbon capture as compared to 57% (HHV) for state-
of-the-art coal-to-hydrogen process.
Syngas chemical looping process for hydrogen Coal Fe2O3 The SCL process is used for hydrogen production and When the hydrogen capacity was 100%, the process [260]
and electricity coproduction electricity generation at various ratios through the utilization efficiency was 67.6% (1.5% in electricity and 66.1% in
of CLG and CLC concepts. hydrogen). When electricity was the only product, the
process efficiency was 34.9%.
IGCC scheme for co-generation of hydrogen Coal Fe3O4 Hydrogen and electricity co-production process based on When the hydrogen output increased from 0 to 150 MW, [261]
and electricity with carbon capture and gasification process with iron oxides chemical looping system the net electrical efficiency decreased from 38.82% to
storage using an iron based chemical used for carbon capture. 31.38%, but the cumulative efficiency increased from
looping system 38.82% to 44.44%. The carbon capture rate was 99.51%.
Chemical looping-based hydrogen and Coal NiO/NiAl2O4, CLC process (Ni-based oxygen carriers) with the steam-iron The process simulation results showed that at the [262]
electricity plant Fe2O3 process. conditions of Fe-SR 815 °C, Fe-FR 815 °C, Ni-FR 900 °C,
Ni-AR 1050 °C, and the supplementary firing temperature
of 1350 °C, the net power efficiency, hydrogen efficiency
and the equivalent efficiency were 27.47%, 23.39% and
70.75%, respectively; the CO2 emission was 365.36 g/
kWh.
Syngas-fueled chemical looping systems for Coal Fe2O3 Two SCL systems with different reactor configurations The H2 production efficiency of the SCL-MB system [263]
H2 and electricity production (moving bed reactor and fluidized bed reactor mode) for H2 (55.1%) was higher than that of the SCL-FB system
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and electricity production. (44.0%). Both the two systems has a carbon capture
efficiency higher than 99.0%.
O2/CO2 blown UCG integrated CLH based Coal Fe2O3 Pure hydrogen is produced by using the CLH process with The net efficiency of O2/CO2 based UCG integrated with [264]
PEMFC cycle power plant the underground coal gasification (UCG) gas. Then the pure CLH-PEMFC system reaches to 43.6% with carbon capture
hydrogen is used to generate electric power in a proton and storage (CCS), while the corresponding value of the
exchange membrane fuel cell (PEMFC) system. conventional reforming based system is 37.95%.
CLHG-SOFC/GT hybrid plant Coal Fe2O3 CLH integrates the SOFC/GT (solid oxide fuel cell/gas The simulation showed that when the system pressure was [265]
turbine) cycle and coal gasification. set to be 20 bar and the cell temperature was 900 °C, the
net power efficiency of the CLHG-SOFC/GT plant reached
to 43.53% and zero carbon emission achieved.
Chemical looping zero emission coal (CL-ZEC) Coal and biomass Fe2O3 The system is based on the coal/biomass co- The energy and exergy of the system operation results were [266]
system (wheat straw) hydrogasification and the CLH technologies. analyzed. The total energy efficiency (ηte), the total exergy
efficiency (ηtex), and the carbon capture efficiency (ηcc) of
the system were found to be 43.6%, 41.2% and 99.1%,
respectively.
Integrated gasification chemical looping Coal Fe2O3 This process uses a three-step chemical loop for the The proposed system achieved an electricity efficiency of [267]
combustion (IGCLC) process production of hydrogen, combustion of gaseous fuels, and 49.5% at steam/hydrogen to carbon ratio of 2 and feed
regeneration of metal oxides. temperature of 1100 K, which was 80% higher than a
conventional coal-fired power station with CCS measures.
The carbon capture efficiency was 100%.
CDCL process Coal Fe2O3 Coal direct chemical looping hydrogen process. Simulation showed that the energy conversion efficiency of [189,259]
the CDCL process was higher 80% (HHV) for hydrogen
production and over 50% for electricity generation with
zero carbon emissions.
Integrated system for energy efficient co- Coal Fe2O3 The system integrates coal drying, coal direct chemical The H2 production efficiency and the power generation [268]
production of H2 and power looping, combined cycle and hydrogenation for H2 efficiency could reach to 71.4% and 19.9%, respectively at
production and power generation. the given conditions.
BDCL process Biomass(hybrid Fe2O3 Biomass direct chemical looping process. The BDCL process could coproduce hydrogen and [269]
poplar) electricity with a combined efficiency (ηH2 + ηE) as high as
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Renewable and Sustainable Energy Reviews 81 (2018) 3186–3214
Table 5 (continued)
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the conventional SMR case. For the same amount of H2
production the effective thermal efficiency was about 75%,
which was 6% higher than the baseline case. Moreover, the
carbon capture efficiency of the system was greater than
90%.
Urea production plant Nature gas Fe2O3 CLH process is used to produce the pure steams of H2 and N2 Economic evaluation of the proposed plant showed a [273]
for ammonia production and CO2 for urea synthesis. considerable rate of return and financial interest. In the
different production rate, the proposed plant had a rate of
return (IRR) above 28%, while the IRR of conventional
plants was almost near 20%.
Three reactor chemical looping hydrogen Nature gas Fe2O3/MgAl2O4 (30/70 wt%) A chemical looping hydrogen plant for hydrogen and power When CO2 is captured, the cost of H2 production is 1.679 [274]
production (TRCLH) plant co-generation. $/kg, which is much lower than the conventional SMR
method (~ 2.39 $/kg), while if CO2 is not captured, the
cost of H2 production is 1.404 $/kg, which is comparable
with the SMR technology.
Renewable and Sustainable Energy Reviews 81 (2018) 3186–3214
M. Luo et al. Renewable and Sustainable Energy Reviews 81 (2018) 3186–3214
4. Conclusions
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