Techno-Economic Analysis of Processes With Integration of Fluidized Bed Heat Exchangers For H2 Production e Part 2 - Chemical-Looping Combustion
Techno-Economic Analysis of Processes With Integration of Fluidized Bed Heat Exchangers For H2 Production e Part 2 - Chemical-Looping Combustion
Techno-Economic Analysis of Processes With Integration of Fluidized Bed Heat Exchangers For H2 Production e Part 2 - Chemical-Looping Combustion
ScienceDirect
highlights
Article history: This work covers a techno-economic assessment for processes with inherent CO2 separation,
Received 27 October 2020 where a fluidized bed heat exchanger (FBHE) is used as heat source for steam reforming in a
Received in revised form hydrogen production plant. This article builds upon the work presented in Part 1 of this study by
6 April 2021 Stenberg et al. [1], where a process excluding CO2 capture was examined. Part 2 suggests two
Accepted 26 April 2021 process configurations integrating steam reforming with a chemical-looping combustion (CLC)
Available online 8 June 2021 system, thus providing inherent CO2 capture. The first system (case CM) uses natural gas as
supplementary fuel whereas the second system (case CB) uses solid biomass, which enables net
Keywords: negative CO2 emissions. In both systems, the reformer tubes are immersed in a bubbling fluidized
Chemical-looping combustion bed where heat for steam reforming is efficiently transferred to the tubes. The processes include
Hydrogen CO2 compression for pipeline transportation, but excludes transport and storage. The CLC system
Steam reforming is designed based on key parameters, such as the oxygen carrier circulation rate and oxygen
Fluidized bed heat exchanger transport capacity. The first system displays a process with net zero emissions and a hydrogen
Carbon capture production efficiency which is estimated to 76.2%, which is almost 8% higher than the conven-
Negative emissions tional process. The levelized production cost is 1.6% lower at below 2.6 V/kg H2. The second
system shows the possibility to reduce the emissions to 34.1 g CO2/MJH2 compared to the con-
ventional plant which emits 80.7 g CO2/MJH2. The hydrogen production efficiency is above 72% and
around 2% higher than the conventional process. The capital investments are higher in this plant
and the levelized hydrogen production cost is estimated to around 2.67 V/kg. The cost of CO2
avoidance, based on a reference SMR plant with CO2 capture, is low for both cases (4.3 V/tonCO2
for case CM and 2.7 V/tonCO2 for case CB).
© 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
* Corresponding author.
E-mail addresses: [email protected] (V. Stenberg), [email protected] (V. Spallina), [email protected]
(T. Mattisson), [email protected] (M. Ryden).
https://doi.org/10.1016/j.ijhydene.2021.04.170
0360-3199/© 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
25356 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 2 5 3 5 5 e2 5 3 7 5
not possible because of packed catalyst would tend to accu- using biomass or NG as supplementary fuel integrated with
mulate at the bottom of the tubes due to gravity, with CLC for inherent CO2 capture.
increased risk of gas bypassing the catalyst. The reformer
tubes traditionally hang in vertical tube rows to allow for good
control of the thermal expansion which can be seen as an Plant description
additional reason for the vertical orientation. This study also
includes environmentally benign oxygen carriers for chemical- The size of the two plants is identical to the previously modelled
looping combustion suitable for large-scale operation and SMR plants in Part 1 of this study [1], producing 100 000 m3n; H2 /h,
evaluates the possibility to place the reformer tubes in the air but which did not include carbon capture. The system boundary
reactor instead of the fuel reactor. A key difference compared includes the hydrogen production plant and the CO2 compres-
to previous techno-economic studies presented by Spallina sion which is assumed to take place at the plant but excludes
et al. [29] is that an estimation of the heat transfer to the CO2 transport and storage. The overall cost is however consid-
reformer tubes is included to calculate the required bed tem- ered to be dominated by the cost of CO2 capture. Greenhouse
perature in the CLC system. This should provide a better gas emissions from process prior to the plant such as extrac-
comparison with the reference SMR plant where the heat tion, refining and transport of the fuel are not included in this
transfer to the tube surface is also included (see Stenberg et al. study. Table 2 includes some of the most important character-
- Part 1 [1]). istics of the two main process configurations.
All the mentioned processes so far rely on CO2 capture
from use of fossil fuels as fuel source (CCS) which enables SMR with chemical-looping combustion (CLC-SMR) - case
processes with close to zero if not net zero CO2 emissions. In CM
addition to CCS, carbon dioxide removal technologies (CDR)
can be used to enable net negative CO2 emissions [33]. The In Part 1 of this work [1] it was found that it is possible to
importance of CDR technologies can be motivated based on integrate SMR with fluidized bed technology where a single
the findings in a recent report from the IPCC where it is fluidized bed heat exchanger was used as heat source for
concluded that all modelled pathways to limit global warming steam reforming. The results from this study clearly showed
to 1.5 C use CDR to remove 100e1000 Gton CO2 over the 21st the benefits of increased heat transfer in increasing efficiency,
century [33]. One of the most commonly suggested measures but carbon capture was not investigated. SMR could also be
for CDR which has significant CO2 abatement potential is Bio integrated CLC technology (see Fig. 1).
Energy Carbon Capture and Storage or BECCS which relies on The CLC system consists commonly of two interconnected
CCS technology using biomass as source of carbon, thus fluidized beds and solid oxygen carriers are circulating be-
enabling net negative emissions. tween the two reactors, respectively air reactor (AR) and fuel
BECCS could be implemented also in the hydrogen pro- reactor (FR). The general reactions for a generic oxygen carrier
duction process, if the process could be partially/completely (Me) in the CLC system are presented in Eqs. (1) and (2).
based on biomass. Various alternatives to use biomass as a
feedstock for hydrogen production has been reviewed by for Fuel reactor: ð2j þkÞMex Oy þCj H2k /ð2j þkÞMex Oy1 þkH2 O
example Arregi et al. [34], Salkuyeh et al. [35], Pandey et al. þ j CO2 (1)
[36] and Shahabuddin et al. [37]. One solution which is
closely related to the suggested process here is by biomass Air reactor: ð2j þ kÞMex Oy1 þ ðj þ 0:5ÞO2 /ð2j þ kÞMex Oy (2)
gasification which could be used as a feed stream to the
Several authors have reviewed hydrogen production pro-
catalytic process in the reformer tubes. However, the need
cesses which are based on chemical-looping such as Ada nez
for gas polishing from sulphur, tar and alkali species [38,39]
et al. [19], Abad [44] and Luo et al. [45].
is still a problematic issue. In this study, we aim to consider
Among the suggested processes is the idea to integrate CLC
biomass as feedstock for the combustion process required
with SMR where the process conditions on the inside of the
to supply the heat to the natural gas reforming reactions,
reformer tubes are not altered. Case A presented in Part 1 [1]
rather than also replacing the natural gas fed to the
which is defined as a fired tubular SMR plant was used as
reformer tubes. As a result significant changes on the
reference plant to compare the new plant layouts based on
reformer tube side are avoided. This process outline leads to
CLC under the same assumptions and methodology. Just as
that the plant overall can deliver significant net negative
for case A, excess heat is used to preheat feed streams and for
emissions, since all the generated CO2 can be captured from
steam production. The first consideration for this integration
the CLC process.
is the position of the reformer tubes. The tubes could be
With biomass as fuel, the CLC process is similar to bio-CLC,
placed in the air reactor, in the fuel reactor or in a separate
which has been explored previously, e.g. Refs. [40e43]. One of
external fluidized bed heat exchanger. The vertical tubes are
the biggest challenges identified so far with this process is to
placed in the fuel reactor although previous works have sug-
achieve complete/close to complete conversion of the
gested to use both fuel reactor [28e30] and air reactor [31,32].
biomass volatiles. Flue gas cleaning is well developed for CFB
The fuel will be oxidized in the dense bed of the fuel reactor by
for biomass and it is foreseen that similar steps could be used
the oxygen carrier particles. It is therefore important to
in the bio-CLC plant despite that the gas composition is
choose a suitable oxygen carrier for the system. While the
notably different.
oxygen carrier reactivity should not limit the performance of
The aim of this work is to perform an evaluation of the
the technology as discussed in Abad et al. [44], a high chemical
techno-economic and environmental performance of SMR
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Table 2 e List of the most important differences in the modelling of case CM and CB compared to the reference case
presented in Part 1.
Item Plant configuration
Reference plant NG-CLC-SMR Bio-CLC-SMR
Case A Case CM Case CB
Feed Natural gas Natural gas Natural gas
Supplementary fuel Natural gas Natural gas Biomass
CO2 capture No Yes Yes
Oxygen carrier No C28 (CaMn0.775Mg0.1Ti0.125O3-d) Manganese ore
Oxygen transport (%) e 1.25 1.25
Heat of reaction for oxidation of OC (kJ/mol O2) 325 314
Steam-to-carbon ratio 2.7 2.7 4.5
Air-to-Fuel ratio in furnace/air reactor 1.09 1.1 [66] 1.1 [66]
Oxygen demand based on present volatiles (%) e e 10%
Air-to-Fuel ratio in oxygen polishing unit e e 1.05
HT WGS inlet temperature (C) 330 330 330
LT WGS inlet temperature (C) - e 205
Air blowers
Isentropic efficiency (%) [67] e 85 85
Mechanical efficiency [67] e 95 95
CO2 compression and purification
CO2 compressor stages e 3 3
Polytropic efficiency for stage 1/2/3 (%) [67] e 80/80/75 80/80/75
Mechanical efficiency (%) [67] e 95 95
Inter-cooler outlet temperature (C) [67] e 30 30
Compressor stage discharge pressures (bar) [67] e 4.4/18.7/80 4.4/18.7/80
CO2 pump efficiency (%) [67] e 75 75
CO2 pump driver efficiency (%) [67] e 95 95
Properties of delivered CO2 e 110 bar, 30 C 110 bar, 30 C
Air separation unit (ASU)
Oxygen purity (mol-%) [67,68] e e 95
ASU electricity consumption (kWh/ton O2) [69,70] e e 200
Fig. 1 e Simplified illustration of case CM where PSA off-gas and NG are used as fuel in the fuel reactor (FR).
and mechanical stability since is required since the solid is Part 1 as C28 (CaMn0.775Mg0.1Ti0.125O3-d) was chosen as a suit-
continuously circulated between fuel and air reactors. For this able bed material due to high reactivity with both methane/
purpose a manganese-based perovskite material, presented in natural gas [46,47] and biomass [48]. C28 has been amply
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studied in Refs. [47,49e51] where the development process of is used as the FBHE, the fuel reactor will be operated as a fast
this material is summarized by Moldenhauer et al. [47]. The fluidized bed reactor and provide circulation of the bed material.
process flowsheet for case CM can be observed in Fig. 2. The One potential obstacle with this approach is that the required
SMR process can be observed by following the black arrows particle flux could potentially be higher than what could easily
where NG used as feed leads to syngas production (see green be achieved with the FR, which is dimensioned based on the gas
arrows) and in the end produced hydrogen. The feed streams flow of fuel gas (PSA off-gas and supplementary fuel).
to the CLC system are indicated in black whereas the hot Secondly, the choice of oxygen carrier needs to be
stream with oxygen depleted air from the AR is in purple. The considered. Low cost naturally occurring ores or industrial
flue gas stream from the FR is indicated in red from which the waste materials could be a better choice than synthetic ma-
CO2 is captured. The scheme also includes thermal integration terials [23,53,54], to compensate lower lifetime due to ash and
with the steam cycle (indicated with blue arrows). The scheme solid fuel impurities. Several natural ores were investigated by
does not include cyclones for gas-solid separation. Fossdal et al. [55] where a manganese ore was picked as the
best option for CLC application. Manganese ores contain
SMR with chemical-looping combustion with biomass (CLC-
SMR) - case CB
Fig. 2 e Schematic illustration of case CM where the reformer is integrated with a FBHE unit in the FR of a CLC system.
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typically 30e60% manganese in oxide form [54]. The material be operated as a circulating fluidized bed (CFB). An oxygen
is cheap, environmentally friendly, abundant and manganese polishing unit fed with pure oxygen is used to ensure com-
oxide, which can be expected to make up a significant part of plete fuel conversion downstream of the FR.
the Mn ore, has a high oxygen carrier capacity (7e10 wt-% Many kinds of biomass should be able to use in this pro-
depending on temperature) in relation to iron for example cess. A basic feature should however be that the fuel is
(3.3 wt-%) [56,57]. Manganese ore has shown to have high gas affordable and available in large quantities. Examples of
conversion rates for syngas in CLC systems (95e100%) possible fuels are for example wood chips, GROT (tops,
[53,58,59] and up to 80% with methane [58]. In operation with branches and stumps) or other harvested forest residues
biomass in CFB units today where silica sand is used as bed which cannot be used by the pulp & paper industry and
material the temperature is limited to below 900 C, mainly sawdust, a by-product of sawmills industry. These fuels are
due to formation alkali silicates which tend to become sticky commonly used in combined heat and power plants and are
thus causing the bed material to adhere together and cause considered to be suitable for this process.
agglomeration [60]. This issue is however not expected with In order to obtain a CO2-rich gas stream suitable for pipe-
bed materials as for example manganese ore or ilmenite, line transportation, flue gas cleaning is required. In case CM it
which have been shown to have less agglomeration ten- is assumed that no flue gas cleaning is required, and that the
dencies with biomass at high bed temperatures [57]. An CO2 is ready for transportation after condensing the steam
overview of challenges with fluidized bed combustion fuelled and CO2 compression. In case CB, oxygen polishing and a
with biomass is presented by Khan et al. [61]. conventional biomass-fired CFB flue gas cleaning system
Thirdly, in order to further reduce the CO2 emissions, this including feeding lime and active carbon for removal of water-
process is designed to have a higher H2 yield than the refer- soluble gases (including SO2, HCl, HF, NH3) as well as bag
ence process to increase the NG-to-H2 yield. This increases the house filters to remove fine particulate matter are considered.
biomass thermal input to the process. The two measures The resulting process outline can be observed in Fig. 4. The
chosen in this work was to use a higher steam-to-carbon ratio scheme is similar to the one presented for case CM in Fig. 2
in the reformer compared to the plant in case CM and a LT where the main differences being the addition of oxygen
WGS reactor is added. polishing, ASU, LT WGS reactor and minor changes in the
Fourthly, it is a challenge to ensure complete conversion of steam cycle. The scheme does not include flue gas cleaning
the biomass in the fuel reactor. In order to achieve this suc- steps other than oxygen polishing.
cessful biomass char gasification and volatiles combustion
has to take place. Since biomass contains a lot of volatiles
which, when released can have poor contact with the oxygen Model description
carrier [23,62] and result in unburnt fuel leaving the FR. This in
turn increases the required thermal input to the FR as well as Aspen Plus model design
the need for downstream conditioning.
Among the possible solutions to achieve this, several The two processes were studied using a similar approach as
different processes could be considered such as using in-bed described in part 1 of this study [1] in regard to the process
feeding, Chemical looping with oxygen uncoupling (CLOU) simulation in Aspen Plus and differences in the overall model
materials [63,64], recycling of flue gas [65] and multi-stage fuel are described in this section. Assumptions related to both
reactors [65]. This work however does not focus on specifically steam reforming process, strategy for thermal integration,
addressing this challenge since it is focused on the overall steam cycle, pressure drops and compression of the H2 prod-
techno-economic assessment. Therefore, the FR is assumed to uct are the same as in Part 1. Heat surplus in the processes is
Fig. 4 e Schematic illustration of case CB where the reformer is integrated with a FBHE unit in the AR of a CLC system.
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used for preheating the feed stream to the reformer, HP steam the same. All units with chemical reactions (fluidized beds,
production as well as some additional LP steam production WGS reactors, oxygen polishing unit etc.) are modelled as
was included in case CB. The choice to also include additional RGibbs equilibrium reactors apart from the furnace in case CB
LP steam production in case CB resulted from the fact that this which is modelled as a RStoich reactor.
case operates with a higher S/C ratio which in turn leads to The delivered CO2 stream has 110 bar pressure and a
more heat available in the syngas and flue gas streams. This maximum temperature of 30 C [16,67,73] which is suitable for
heat is recovered in the steam cycle thus resulting in a higher transportation by pipeline. The CO2 compression is carried out
feedwater demand. The key differences in the model as- as suggested by the EBTF-report serving as a benchmark for
sumptions for case CM and CB compared to case A are pre- evaluation of CO2 capture technologies [67].
sented in Table 2. The biomass included in the process was based on the ul-
The outlet temperature of the FBHE units is defined based on timate analysis of wood chips presented by Hannula et al. [74]
the estimation of the heat transfer coefficient from bed to tube (see Table A3 in Appendix). Based on this data an equivalent
in the same manner as for case OM in Part 1 of this work. Both biomass composition was estimated which represents the
air reactor (AR) and fuel reactor (FR) were modelled as RGibbs fuel composition of the biomass used in the Aspen Plus model
reactors where the heat required for steam reforming was where both mass and energy balance was conserved.
withdrawn from FR in case CM and from AR in case CB. The air In addition to case CM and CB, two alternative configura-
to fuel ratio is based on the amount of reduced oxygen carrier tions of these processes (one for each case) were considered in
fed to the air reactor. The relation between oxidized oxygen this work. For case CM an alternative placement of the FBHE in
carrier and the amount of fuel fed to the fuel reactor is based on the AR instead of in the FR was attempted in CM2. For case CB
having an oxygen transport of 1.25 wt-% to ensure long-term it was considered interesting to study the effect of operating
durability. The oxygen transport represents the mass of oxy- with process parameters similar to case CM with a lower S/C
gen consumed in the FR in relation to the total mass of oxygen ratio (2.7) and no LT WGS reactor resulting in a lower hydrogen
carrier at the outlet of the AR expressed as a percentage. yield (case CB2).
The models for case CM and CB both include oxygen car-
riers which are defined as conventional solid components in Reactor design
ASPEN PLUS. In order to model the reactions of the oxygen
carrier, the heat of reaction in the oxidation and reduction The design of the FBHE units is carried out in the same
reactions in AR and FR belong to the key characteristics to approach as presented for case OM in Part 1 [1] as well as the
include. In the Aspen Plus model 20 mol-% nickel oxide (NiO) estimation of the number of reformer tubes where all cases
is used on 80 mol-% inert magnesium aluminate (MgAl2O4) are operating with the same residence time of gas in the tubes
support material. The use of NiO here was for modelling as in Part 1. The aim with the FBHE reactor design is to present
purpose only. Differences in heat of reaction for nickel oxide a design which presents a reasonable flue gas temperature
and the oxygen carrier materials C28 (used in case CM) and and supplies the required heat to the steam reforming. The
manganese ore (used in case CB) were compensated for and flue gas temperature in the reformer furnace is for all cases
included in the Aspen Plus model [56]. calculated based on the procedure presented in Part 1 [1]. Fig. 5
The biomass char is modelled as graphite is therefore in Part 1 [1] explains the calculation procedure where an
assumed to be combusted completely in the FR. Biomass char estimation of the bed-ot-tube heat transfer for each case
could be transferred to the air reactor (and burnt there) or lost makes up an essential part.
with the fuel reactor exhaust gas but this risk is neglected In the FBHE, an even number of tube passes for the vertical
since biomass char is more reactive than other char and that reformer tube bundle is assumed. A ratio of 2:1 between width
sufficient residence times should be reached [71]. It was and depth was assumed for both FBHE and CFB. The used
assumed that 10% of the volatiles entering the fuel reactor oxygen carrier in the FBHE was assumed to have the same
(CH4, CO and H2) remain unconverted and therefore converted properties as presented in Part 1 with a mean particle size of
downstream. This assumption is close to the recently pub- 180 mm and a bulk density of 1600 kg/m3. The CFB units are
lished experimental results for various biomass-fuelled CLC assumed to use a superficial gas velocity of 5 m/s which is
[72]. Steam released from the biomass drying and CO2-rich limited by the risk of furnace erosion for these units [75]
PSA off-gas (approximately 67 vol-% CO2) is assumed to act as whereas the FBHE reactors are operated with a superficial gas
gasification agents. Additional gasification gas could be pro- velocity of 0.5 m/s. The gas velocities are estimated based on
vided based on the large quantity of LP steam which is the operating temperature and pressure for these units where
generated at the plant. the pressure is close to atmospheric conditions in the fluid-
The required oxygen could be fed to a separate unit or be ized bed units. The FBHE is as previously mentioned placed in
included in the FR cyclone where good gas-solid contact can the FR in case CM and in the AR in case CM2.
be expected. The oxygen polishing unit (post-oxidation Based on the most commonly used oxygen carriers and
chamber) is modelled as an adiabatic RGibbs reactor placed fuels in CLC systems the heat of reaction is always more
directly after the fuel reactor operating with 5% excess oxy- exothermic in the AR compared to the FR, resulting in a higher
gen. The air separation unit (ASU) is modelled according to temperature in the AR. This argues for placing the FBHE in the
literature data [69,70]. It should be mentioned that the elec- AR based on a larger temperature driving force for heat ex-
tricity consumption could be higher. change. There are however several reasons for placing the
For both case CM and CB, the Aspen Plus model for the FBHE in the FR instead. Firstly, the volume of gas fed to the AR
reforming as in the two cases presented in Part 1 are generally roughly two times higher than the gas flow to the FR which
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m_ H2 ,LHVH2
hH2 ¼ (3)
m_ biomass ,LHVbiomass þ m_ NG;tot ,LHVNG
Table 3 e Cost calculation assumptions for the units not included in Part 1.
Equipment unit Scaling parameter Ref. capacity, So Ref erected cost (MV) Scale factor Cost year
Cyclone Volumetric flow [m3std =sec] 47.74 2.24 [79] 0.6 2002
CO2 compressor Compressor power [MW] 13 9.95 [67] 0.67 2008
Air separation unit (ASU) Oxygen produced (kg/s) 28.9 26.6 [80] 0.7 2008
estimated in a similar way as the fluidized bed units (see Results and discussion
additional information in Part 1).
The CO2 avoidance cost (CCA) was estimated according to Thermodynamic evaluation
Eq. (7) and represents the added cost to capture CO2 for a
certain case (i) compared to a reference plant with no capture The composite curves for case CM and CB are included in Fig. 6
which is represented by case A in Part 1 [1]. The cost is pre- and Fig. 7 respectively where the sections for the flue gas,
sented in the unit V/ton CO2. syngas and oxygen depleted air streams are included.
Several differences can be observed between case CM
LCOHi LCOHcase A
CCA ¼ (7) and CB when consulting Figs. 6 and 7. The flue gas section
ECO2 ; case A ECO2 ;i
looks similar overall although the heat load is overall larger
Just as in Part 1, the economic value of LP steam has been for case CB resulting in more excess heat generation. This
neglected in this analysis since there is generally little use of can be explained by that the overall thermal input to the
this low-value heat source at a refinery. The biomass cost is furnace is higher in case CB which in turn can be explained
assumed to be 183 SEK/MWh (approx. 20 $/MWh) which was by that the heating value of the biomass is lower than for
the average price for wood chips during 2015 for industries in the natural gas and that the fuel conversion in the FR is
Sweden [82]. Feedstock preparation costs and the handling incomplete in case CB.
costs are not included in this analysis. In the syngas section more heat is available in the syngas
The cost of the biomass derived flue gas cleaning was stream in case CB compared to CM mainly as a result of a higher
estimated using industrial data from Valmet based on the S/C ratio. The section with the oxygen depleted air is similar for
targeted fuel and assumed flue gas flow to approximately case CM and CB where the outlet temperature is higher in case
1.7 MV [83] in case CB and CB2. This contact was also used to CM. The amount of LP steam to export is equal to 7.6 kg/s in
estimate some of the variable costs including necessary case CM and 9.2 kg/s in case CB which are still significantly
chemicals for continuous removal of contaminants. The lower than in the conventional plant (see case A in Part 1).
electricity consumption for the baghouse filter and the feeding The results from the thermodynamic evaluation of case
system for the lime and active carbon were estimated to be CM and CB including the thermal efficiency to produce
negligible and as a result not included in the variable costs. hydrogen and the CO2 emissions from the plants are pre-
Other relevant O&M costs are found in Part 1 and presented in sented in Table 5 together with the result for case CM2 and
Table 4. CB2 and the two cases from Part 1 which are included for
The lifetime of the oxygen carrier in case CM is estimated comparison.
to the same value as was assumed in case OM which was CO2 compression adds a significant electricity consump-
based on loss of fines from operation with a 10 kWth CLC unit tion in the cases with CO2 capture. The compression work is
for natural gas [89]. The cost of C28 is the same as presented in highest for case CB and CB2 since additional CO2 is com-
Part 1 of this work, 1225 V/ton. For case CB the lifetime of the pressed resulting overall in electricity demand in case CM,
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Fig. 6 e Hot and cold composite curves for the syngas system, flue gas and oxygen depleted air section in the plant where
SMR is integrated with CLC with NG as supplementary fuel (case CM).
Fig. 7 e Hot and cold composite curves for the syngas system, flue gas and oxygen depleted air section in the plant where
SMR is integrated with CLC with biomass as supplementary fuel (case CB).
CM2, CB and CB2. The electricity consumption of the ASU adds balance over the fuel reactor is overall endothermic. In case
additional electricity consumption for case CB and CB2. CB the net heat of reaction is exothermic in both FR and AR.
In case CB the H2 yield is significantly higher compared to It can be observed that the off-gas stream is the same in all
the other cases as a result of a higher S/C ratio and the use of a cases apart from case CB where a higher hydrogen yield is
LT WGS reactor which results in that the NG feed stream can achieved resulting in less combustible compounds such as
be reduced while still producing same hydrogen amount. This CH4 and CO in the off-gas which is compensated by adding
is also the reason why the furnace duty transferred to the 5.9 kg/s of biomass.
reformer tubes is slightly smaller in case CB although there is In terms of CO2 emissions, case CM has no specific CO2
more inert steam in the tubes and that more endothermic emissions (100% capture) and the equivalent CO2 emissions
steam reforming reaction takes place. are negative for the process if the excess heat can be utilized.
When comparing the NG consumption of case OM and CM The CO2 emissions are in this case considered as negative
it can be observed that the consumption increases when since it assumes that the utilization of the excess heat means
adding CO2 capture, but it is still clearly lower than for case A. replacing heat which would otherwise have resulted in CO2
The difference is small between CM and CM2 and the con- emissions. In case CB the specific CO2 emissions from the
sumption is significantly lower in case CB where no NG is used plant are net negative (without considering possible use of
as supplementary fuel and the NG feed stream is reduced. excess heat nor electricity) and resulting in emissions which
The heat balance over the FR in case CM considering the are 0.29 Mton CO2/year which is 142% lower than for the
fuel oxidation and the OC reduction indicates that the net heat benchmark plant (Case A).
of reaction should be exothermic but since a significant When consulting the presented hydrogen production effi-
amount of heat is also extracted to steam reforming the heat ciencies in Table 5 it can be observed that the energy penalty for
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Table 5 e Energy streams and performance parameters of the plant configurations (positive numbers imply production and
negative numbers imply consumption).
Case A Case OM Case CM Case CM2 Case CB Case CB2
Electricity production/consumption
Air blowers MWel 1.0 0.6 2.2 2.4 2.3
H2 compressors MWel 3.8 3.8 3.8 3.8 3.8 3.8
CO2 compressors MWel 8.8 8.8 11.5 10.3
Steam turbines MWel 16.9 8.0 10.2 10.2 12.6 13.3
Pumps MWel 0.8 0.5 0.6 0.6 0.8 0.7
Pumps for heat rejection MWel 0.1 0.2 0.4 0.4 0.6 0.4
Air separation unit MWel 0.7 0.8
Net electric power MWel 12.3 2.6 4.1 5.6 7.3 5.3
Heat production/consumption
Total cooling requirement MWheat 12.3 22.1 55.6 55.3 73.4 54.3
Steam export (160 C, 6 bar) kg/s 18.8 4.1 7.6 7.7 9.2 13.2
Furnace duty transferred to reformer tubes MW 97.9 97.9 97.9 97.9 96.0 97.9
Efficiency and emission data
Hydrogen yield after reformer, YH2,ref % 68.1 68.1 68.1 68.1 79.8 68.1
Hydrogen yield after WGS, YH2,WGS % 78.5 78.5 78.5 78.5 93.1 78.5
Total NG consumption m_ NG;tot kg/s 9.10 8.15 8.45 8.43 6.43 7.64
Thermal input off-gas MWLHV 113.5 113.5 113.5 113.5 54.3 113.5
Thermal input supplementary fuel MWLHV 68.0 23.9 37.8 36.6 115.4 53.0
Total thermal input to furnace MWLHV 181.4 137.3 151.2 150.1 169.7 166.5
H2 production efficiency hH2 % 70.7 79.0 76.2 76.4 72.2 73.3
H2 production efficiency hH2;eq % 83.9 82.1 78.4 78.2 73.9 78.0
H2 production efficiency h0eq;H2 % 75.8 80.2 75.4 75.1 70.1 72.0
CO2 specific emissions ECO2 gCO2 /MJH2 produced 80.7 72.2 0 0 34.1 15.7
Equivalent CO2 specific emissions ECO2 ;eq gCO2 /MJH2 produced 68.0 69.5 2.1 1.7 35.9 20.0
Equivalent CO2 specific emissions E0CO2 ;eq gCO2 /MJH2 produced 75.3 71.1 0.8 1.3 32.3 14.9
Total plant CO2 emissions Mton CO2/year 0.69 0.61 0 0 0.29 0.13
adding CO2 capture is limited when comparing case OM and correction factor closer to 1 as a result of less dense tube
case CM. The main reasons for the energy penalty are a higher spacing compared to case OM and CM. It can be observed that
air consumption as a result of a higher AFR, air reactor being the estimated flue gas temperatures from the reformer
heated to a higher temperature than the FBHE in case OM and a furnace is significantly lower in the cases with FBHE as a result
lower fuel gas inlet temperature (400 C vs 266 C). In this regard of the high heat transfer in the fluidized beds. CB2 has almost
it is also interesting to point out that the placement of the FBHE identical heat transfer coefficients as in case CB where the
seems to have a limited effect on the hydrogen production ef- minor differences in gas composition in the AR flue gas has
ficiency since case CM2 has only a slightly higher efficiency. almost no effect on the estimated heat transfer coefficient on
Despite the mentioned energy penalties, the hydrogen produc- the outside of the reformer tubes when comparing case CB
tion efficiency hH2 is 7.7e8.0% higher in case CM and CM2 than and CB2.
for the reference SMR plant. It can be observed that case CB has The estimated temperature levels for the dual-fluidized
a lower thermodynamic efficiency than case CM. This is mainly systems are considered to be suitable for combustion of both
explained by the incomplete fuel conversion in the fuel reactor gaseous and solid fuel in the FR based on previous operational
and a higher S/C ratio. The equivalent hydrogen production ef- experience [23]. The design specifications for the reformer
ficiency is lower for case CM, CM2, CB and CB2 compared to case furnaces in case CM, CM2 and CB are presented in Table 7
A and OM which to a large extent can be explained by the sig- together with the values for the cases presented in Part 1.
nificant electricity consumption for CO2 compression. It can be observed that the FBHE reactor size is of the same
order of magnitude for case OM presented in Part 1. The di-
Reactors design mensions are however different as a result of different gas
flows. The gas flow fed to the FBHE in case CM is approxi-
The results of the heat transfer calculations required for FBHE mately 25% of the gas flow passing through the FBHE in case
reactor design for case CM, CM2 and CB are presented in Table OM. In order to maintain a tube pitch above two tube di-
6 as well as the corresponding values for reformer furnaces in ameters (2Dto) for this case it is therefore necessary to use 2
the two cases presented in Part 1. tube passes instead of 4 as in case OM. This results in a higher
It can be observed in Table 6 that all cases with FBHE units bed height and a higher pressure drop over the bed. This
display high heat transfer coefficients although some differ- pressure drop should be acceptable since the PSA off-gas is
ences can be seen. The radiative heat transfer coefficient is assumed to be delivered at a pressure above 1.5 bar. The ob-
similar for the different fluidized bed heat exchangers. In the tained particle flux in the CFB is below the set limit of 50 kg/
estimation of the corrected bed-to-tube heat transfer coeffi- (m2s) for case CM. The fact that the cross-sectional area of the
cient it can be observed that case CM2, CB and CB2 has a FBHE is significantly smaller in case CM compared to case OM,
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 2 5 3 5 5 e2 5 3 7 5 25367
Overall heat transfer coefficient 118 370 396 374 359 342
(Uo) (W/(m2K))
Required heat transfer area (m2) 1841 1841 1841 1841 2192 1841
Flue gas temperature (C) 1201 935 929 934 922 934
for example, should be seen as an advantage of this process similar to case CB despite that more reformer tubes are pre-
since space at the plant may be limited. A result of smaller sent in the latter (which is a result of larger gas flow), with very
reactor dimensions also results in a less OC inventory in case limited effect on the reactor dimensions and required oxygen
CM compared to case OM. carrier inventory.
In case CM2, CB and CB2 the cross-section of the FBHE is The CFB unit in CM2 is significantly smaller (96% in terms
larger compared to case CM mainly as a result of the place- of volume) than in case CM since the gas flow to the CFB is
ment in the air reactor where the gas flow is larger. Despite the smaller. The resulting particle flux is however higher than the
larger gas flow, it is not possible to use 4 tube passes but maximum value considered and a possible bottleneck for case
instead 2 tube passes are used for case CM2, CB and CB2. The CM2 has been identified.
estimated pressure drop for the three mentioned units are It could be possible to operate with a higher degree of
therefore the same as for case CM. Case CB2 is overall very reduction of the oxygen carrier than assumed in this work but
25368 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 2 5 3 5 5 e2 5 3 7 5
it may lead to fragmentation. This could for example be also more expensive since these are operated with a higher
possible by using an oxygen carrier with higher oxygen carrier CO2 flow rate. It should also be said that some flue gas
capacity (e.g. Cu-based material). This would then result in a cleaning is most likely needed also for all the other systems
lower circulation rate. A separate riser could also be used to (which has not been included in this work), but the result of
provide circulation as proposed in 10e100 kW units [90,91]. In this work should still provide a good comparison between
that case additional gas could be used to circulate part of the the requirements of case CB in relation to the other cases.
particles to maintain a particle flux below the limit in the CFB The variable costs however are actually the lowest for this
riser. case despite that this case has the highest cost for electricity
The specific bed inventory for the different FBHE units are import (3.4 MV/y). The main reason is the lower cost of the
similar to the value in case OM. For the air reactors it is in line fuel feedstock (NG þ biomass) justified by the higher H2 yield
with what is observed in larger CLC pilots today [23] whereas as explained in the section before (23 MV/year compared to
the FBHE has a significantly higher value, but this is reason- case A). The lower cost for oxygen carrier make up could also
able considering the purpose of the unit. justify the use of a synthetic and more expensive material if
this would benefit the overall performance and operation
Economic assessment strategies.
It should in this regard be accentuated that the price of
The results from the economic analysis are documented in the biomass has a high impact on the LCOH for case CB
Table 8 which includes individual component costs, fixed and (here assumed to be roughly half the price of the NG). The
variable costs which together add up to the levelized hydrogen effect of the biomass fuel price is investigated further in the
production costs for all presented cases. economic sensitivity analysis presented in section
In a comparison of the costs of the reference SMR plant Economic sensitivity analysis. The cost of landfilling is in
(case A) and case CM it is possible to see that the equipment this case negligible.
cost is higher for case CM which to a large extent is depen- When comparing case CB2 with CB the most significant
dent on the cost of the CO2 compressor. Additional in- reduction in equipment cost can be traced to the absence of
vestments for air reactor, cyclone and a larger cooling water the LT WGS reactor in case CB2 while other equipment cost
system corresponding to an additional 21.1 MV/year are also such as the FBHE, and HXs are less relevant. In terms of var-
contributing in this regard. It can however be noted that the iable costs, case CB2 presents a higher fuel cost (þ9.0 MV/y)
cost for the heat exchangers is lower for case CM compared and lower oxygen carriers make-up. The cost for oxygen car-
to both reference plant and case OM. When considering the rier make-up is even lower in case CB2 which is originating
variable costs, it should be noted that oxygen carrier make- from a lower thermal input of biomass compared to case CB.
up cost is 42% lower in case CM compared to case OM as a The LCOH is fairly similar for case CB and CB2. Case CB2 could
result of less bed material use. Case CM still has a higher be seen as more interesting from an economic point of view
production cost than case OM (þ6%), but it could be said that while case CB appears as the best option from an environ-
the incremental cost for CO2 capture is small compared to mental point of view.
the possibility to reduce the NG cost compared to case A. This The cost of CO2 avoidance is negative for all but one of
results in that the levelized hydrogen production cost is the suggested cases when comparing it to the reference
lower than for the reference SMR plant and the estimated plant case A, despite that these include CO2 capture and
CO2 avoidance cost is 4.28 V/tonCO2. This option looks very compression work. In this regard, it should however be said
interesting to enable hydrogen production with cost-efficient that the cost of CO2 avoidance, with respect to case OM,
CO2 capture. show a positive cost (þ16.9e20.5 V/tonCO2) for case CM and
When comparing the equipment costs of CM and CM2, it CM2, while the CB cases are ranging between þ14.4e17.7
can be observed that the FBHE is cheaper in case CM as V/tonCO2. This results are still better than existing technol-
expected but the cost of the CFB and cyclones is higher. The ogies proposed for H2 production with CO2 capture
total cost of these two units is higher in case CM (þ1.0 MV). [16,92e95] thus underlining the incremental environmental
The cost of the flue gas HX and air blower is however more and economic advantage of a biomass co-fuelled plant.
expensive in case CM2 which results in a slightly higher There are two main reasons which explains why the CO2
equipment cost in that case. When considering the variable avoidance cost is so low for these processes:
costs, it can be seen that case CM2 has as a lower NG cost
(0.4 MV) but higher oxygen carrier make up cost (þ1.6 MV) The cost of the fuel makes up some 60e70% of the levelized
and higher electricity consumptions (þ0.7 MV). The net production cost in general so measures where the fuel
result of these differences is that case CM has a slightly consumption of NG can be limited or where cheaper fuels
lower LCOH. can be incorporated in the process such as in case CB, the
In case of CB, the overall equipment costs are significantly variable costs can be decreased significantly which can
higher (þ12.5 MV/year compared to CM) due to the addition compensate for more expensive capital investments.
of a LT WGS, a larger bigger FBHE reactor with more reformer CLC is known to provide low energy penalty and low in-
tubes as well as the ASU and flue gas cleaning. The cost of cremental costs for CO2 capture and this study highlights
HXs is also remarkably higher (þ8.6 MV) which results from this opportunity where the cost is still higher than for case
higher amount of heat exchanged and larger flowrate (as OM which is a very similar process but not including any
represented in Figs. 6 and 7). The cost of CO2 compressors is CO2 capture.
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 2 5 3 5 5 e2 5 3 7 5 25369
Table 8 e Cost comparison including the cases with CO2 capture and case A and OM presented in Part 1.
Hydrogen production process Case A Case OM Case CM Case CM2 Case CB Case CB2
Bare Erected Cost (MV (% of total BEC))
Desulfurization 0.71 (0.8%) 0.71 (0.8%) 0.71 (0.7%) 0.71 (0.7%) 0.64 (0.5%) 0.71 (0.6%)
Pre-reformer 6.16 (6.9%) 6.16 (6.8%) 6.16 (6.2%) 6.16 (6.2%) 5.42 (4.0%) 6.16 (5.6%)
PSA unit 20.72 (23.3%) 20.72 (23.0%) 20.72 (20.8%) 20.72 (20.8%) 20.22 (14.8%) 20.72 (18.7%)
H2 compressor 1.86 (2.1%) 1.86 (2.1%) 1.86 (1.9%) 1.86 (1.9%) 1.87 (1.4%) 1.87 (1.7%)
HT WGS reactor 5.32 (6.0%) 5.32 (5.9%) 5.32 (5.3%) 5.32 (5.3%) 4.74 (3.5%) 5.32 (4.8%)
LT WGS reactor e e e e 18.98 (13.9%) e
Steam turbine 6.23 (7.0%) 4.17 (4.6%) 4.43 (4.4%) 4.45 (4.5%) 5.64 (4.1%) 5.84 (5.3%)
Pump 0.24 (0.3%) 0.20 (0.2%) 0.22 (0.2%) 0.22 (0.2%) 0.31 (0.2%) 0.29 (0.3%)
Syngas cooling HX 10.57 (11.9%) 13.05 (14.5%) 11.62 (11.7%) 11.59 (11.6%) 12.52 (9.2%) 10.96 (9.9%)
Flue gas/oxygen depleted air cooling HX 24.95 (28.0%) 21.78 (24.1%) 18.78 (18.9%) 19.84 (19.9%) 26.64 (19.4%) 23.60 (21.3%)
Cooling water system 3.44 (3.9%) 5.10 (5.7%) 9.47 (9.5%) 9.43 (9.4%) 11.39 (8.4%) 9.32 (8.4%)
Reformer furnace/FBHE 8.82 (9.9%) 10.88 (12.1%) 9.78 (9.8%) 10.71 (10.7%) 12.30 (9.0%) 10.78 (9.7%)
Air blower e 0.28 (0.3%) 0.19 (0.2%) 0.47 (0.5%) 0.49 (0.4%) 0.47 (0.4%)
CFB e e 1.45 (1.5%) 0.41 (0.4%) 0.99 (0.7%) 0.95 (0.9%)
Cyclones e e 1.33 (1.3%) 0.48 (0.5%) 0.84 (0.6%) 0.77 (0.7%)
CO2 compressor þ pump e e 7.45 (7.5%) 7.44 (7.5%) 8.93 (6.6%) 8.29 (7.5%)
Air separation unit (ASU) e e e e 2.28 (1.7%) 2.68 (2.4%)
Oxygen polishing unit e e e e 0.50 (0.4%) 0.49 (0.4%)
Flue gas cleaning e e e e 1.70 (1.2%) 1.7 (1.5%)
Bare Erected Cost (BEC) 89.0 90.2 99.5 99.8 136.2 110.9
Total Plant Cost (TPC) 210.1 212.9 234.8 235.5 321.4 261.7
Total Plant Cost (MV/year) 30.3 30.7 33.9 34.0 46.4 37.8
Labor costs 1.20 (8.0%) 1.20 (8.7%) 1.80 (11.8%) 1.80 (11.7%) 1.80 (8.8%) 1.80 (10.8%)
Maintenance cost 5.25 (35.0%) 5.32 (38.7%) 5.87 (38.5%) 5.89 (38.3%) 8.04 (39.3%) 6.54 (39.3%)
Insurance cost 4.20 (28.0%) 4.26 (30.9%) 4.70 (30.8%) 4.71 (30.7%) 6.43 (31.4%) 5.23 (31.5%)
HT< WGS catalyst 0.19 (1.2%) 0.19 (1.3%) 0.19 (1.2%) 0.19 (1.2%) 0.93 (4.6%) 0.19 (1.1%)
Reformer tube replacement 1.22 (8.1%) 0.61 (4.4%) 0.61 (4.0%) 0.61 (4.0%) 0.73 (3.5%) 0.61 (3.7%)
Pre-reformer and reformer catalyst 1.31 (8.7%) 1.31 (9.5%) 1.31 (8.6%) 1.31 (8.5%) 1.61 (7.9%) 1.31 (7.9%)
Desulfurization catalyst 0.33 (2.2%) 0.33 (2.4%) 0.33 (2.1%) 0.33 (2.1%) 0.28 (1.3%) 0.33 (2.0%)
Internal þ external insulation 1.33 (8.8%) 0.56 (4.1%) 0.45 (3.0%) 0.54 (3.5%) 0.64 (3.1%) 0.62 (3.7%)
Total O&M fixed costs (MV/year) 15.0 13.8 15.2 15.4 20.5 16.6
Natural gas 140.2 (99.5%) 125.6 (97.7%) 130.2 (97.0%) 129.79 (95.3%) 99.09 (81.2%) 117.68 (90.7%)
Biomass e e e e 17.78 (14.6%) 8.16 (6.3%)
Electricity e e 1.90 (1.4%) 2.62 (1.9%) 3.40 (2.8%) 2.45 (1.9%)
Cooling water make-up 0.06 (0%) 0.10 (0.1%) 0.26 (0.2%) 0.26 (0.2%) 0.34 (0.3%) 0.25 (0.2%)
Process water 0.71 (0.5%) 0.71 (0.5%) 0.69 (0.5%) 0.71 (0.5%) 0.72 (0.6%) 0.69 (0.5%)
Oxygen carrier make-up e 2.1 (1.6%) 1.20 (0.9%) 2.82 (2.1%) 0.55 (0.5%) 0.25 (0.6%)
Cost of landfill e e e e 0.19 (0.2%) 0.09 (0.1%)
Cost of lime & active carbon e e e e 0.21 (0.2%) 0.21 (0.2%)
Total O&M variable cost (MV/year) 140.9 128.5 134.2 136.2 122.1 129.8
Table 10 e Parameters for the economic sensitivity analysis with studied ranges where the results from using the lowest
and highest value within the range is presented. Both estimated LCOH (V/Nm3H2 ) and price change in % in relation to the
respective base case.
Operating parameter Range LCOH for Case CM LCOH for Case CB
Low Mid High Low Mid High
Cost of FBHE including reformer tubes (% of estimated cost) 50e200 1.2% Base þ2.4% 1.5% Base þ2.9%
Base ¼ 100 0.2298 0.2381 0.2362 0.2466
Plant availability 50e100 þ21.1% Base 2.6% þ27.6% Base 3.5%
(%) Base ¼ 90 0.2817 0.2264 0.3058 0.2314
Capital Charge Factor (CCF) (%/year) 5e20 12.1% Base þ7.1% 16.1% Base þ9.5%
Base ¼ 14.4 0.2045 0.2491 0.2012 0.2623
Reformer tube lifetime 25 000e100000 þ1.0% e Base þ1.2% e Base
(hours) Base ¼ 100 000 0.2349 0.2424
Price of LP steam 0e40 Base e 4.75% Base e 5.6%
(V/ton) Base ¼ 0 0.2215 0.2263
Natural gas price 5e20 40.6% Base þ50.7% 30.0% Base þ37.4%
(V/GJ) Base ¼ 11.67 0.1382 0.3504 0.1678 0.3294
Biomass price 97e287 e e e 4.4% Base þ5.4%
(SEK/MWh) Base ¼ 183 0.2291 0.2525
Oxygen carrier price 0e1000 0.7% Base þ6.2% 0.3% Base þ2.6%
(% of assumed price) Base ¼ 100 0.2208 0.236 0.2390 0.2460
Cost to emit CO2 0e100 Base e þ0.0% Base e 15.3%
(V/ton) Base ¼ 0 0.2323 0.2029
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