Energy Conversion and Management 159 (2018) 264–273

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Energy Conversion and Management

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

Economic analysis of hydrogen production by methane thermal T

decomposition: Comparison to competing technologies
⁎
Tiina Keipi , Henrik Tolvanen, Jukka Konttinen
Laboratory of Chemistry and Bioengineering, Tampere University of Technology, P.O. Box 541, 33101 Tampere, Finland

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

Keywords: This study is a comparative analysis of hydrogen production costs in current and potential future market en-
Methane decomposition vironments. The economic feasibility of hydrogen production by thermal decomposition of methane was com-
Hydrogen pared to two other technologies, namely steam methane reforming and water electrolysis. According to the
Economic analysis results, thermal decomposition of methane would be most suited for on-site demand-driven hydrogen production
Carbon dioxide emissions
in small or medium industrial scale. Hydrogen production by thermal decomposition of methane would be
economically competitive with steam reforming with a product carbon value of at least 280–310 EUR/tonne. By
contrast, the main benefit of thermal decomposition of methane in comparison with water electrolysis is the
feedstock availability via the current natural gas infrastructure, whereas electrolysis is highly dependent on the
cost and availability of renewable electricity. The major factors affecting the economic feasibility were identified
as product carbon value in thermal decomposition of methane, natural gas cost in steam reforming, and elec-
tricity cost in electrolysis. Thus, the effect of these variables on the hydrogen production costs was analyzed.
Additionally, the specific carbon dioxide emissions in hydrogen production by thermal decomposition of me-
thane (40 kg CO2 /MWhH2 ) were found to be much less that by steam reforming coupled with carbon dioxide
capture from the syngas (133 kg CO2 /MWhH2 ).

1. Introduction increases rapidly in the future [1]. Despite the fast growth, it is esti-
mated that electrolysis cannot be applied to wide-scale H2 production
The International Energy Agency (IEA) estimates that the global that would be required in the H2 economy before the second half of the
energy demand will rise by 30% to 2040 and especially the transpor- 21st century [6]. In order to begin developing the H2 infrastructure and
tation sector will undergo a fuel switch from oil to alternative energy promoting the transition to the H2 economy, alternative solutions that
sources [1]. In order to respond to the growing energy demand and enable H2 production with low CO2 emissions are required as soon as
limit the global CO2 emissions, a transition from the current fossil-based possible.
economy to low-carbon economy is required. A possible future option Applying thermal decomposition of methane (TDM) to natural gas
would be the H2 economy since H2 has been identified to be one of the to produce H2 and solid carbon has been proposed as a potential
few potential energy carriers in the low-carbon economy. [2] However, transition-period technology towards the H2 economy [7]. A life-cycle
the current H2 production is based on steam methane reforming (SMR) analyses of TDM and SMR conducted by Dufour et al. [8,9] have re-
of natural gas (48%), or utilization of other fossil fuels (48%) whereas vealed that TDM has a lower fossil energy consumption and total en-
the water electrolysis accounts for 4% of the H2 production [3]. The vironmental impact than SMR even when carbon capture and storage
usage of fossil fuels for H2 production causes annually 500 million (CCS) is coupled to SMR. Moreover, a study of the whole energy system
tonnes of CO2 emissions, which corresponds to around 2% of the global reveals that the H2 economy where H2 is produced by TDM and used in
energy-related CO2 emissions [4]. fuels cells assuming that the natural gas leakages would be in control,
In the future, the H2 production is proposed to occur by electrolysis can potentially reduce the global CO2 equivalent emissions up to 27%
that is powered by renewable electricity [5]. However, due to the in comparison with the current situation [10]. A benefit of TDM is the
electrolyzer technology costs and the cost of renewable electricity, exploitation of the current natural gas infrastructure, and thus, it could
electrolytic H2 is predicted to remain expensive the next decades [2]. provide a near-term solution for less polluting H2 production. More-
The IEA predicts that the renewable electricity production capacity over, H2 production by TDM could be utilized to promote the H2

⁎
Corresponding author.
E-mail address: tiina.keipi@tut.fi (T. Keipi).

https://doi.org/10.1016/j.enconman.2017.12.063
Received 29 August 2017; Received in revised form 14 December 2017; Accepted 17 December 2017
0196-8904/ © 2017 Elsevier Ltd. All rights reserved.
T. Keipi et al. Energy Conversion and Management 159 (2018) 264–273

Fig. 1. Flow chart of the TDM process.

Process Methane recirculation Process
inputs outputs
Product gas Carbon Gas
H2
filter separation

Carbon
RHER separation
Cooling
Natural gas,
feedstock Bed Carbon
material
Heat circulation
Natural gas,
fuel
Furnace Flue gas
Air

infrastructure development, and thus, smoothen the transition to the H2 reaction temperature below 1300 K by applying a suitable catalyst
economy in the future. would further improve the economic feasibility of TDM [16]. A recent
Several techno-economic assessments of various H2 production study [17] discussed the status and perspectives of three alternative
technologies have been published. Mueller-Langer et al. [11] evaluated technologies for H2 production with low CO2 emissions, namely fossil-
the H2 production costs by SMR, coal and biomass gasification, and based H2 production plant coupled with CCS, thermal decomposition on
water electrolysis. They hypothesized that at the early stages of the H2 various hydrocarbons, and H2 processes integrated with nuclear or solar
economy, H2 would be produced in large-scale fossil fuel based units energy. The competitiveness of thermal decomposition process was
combined with CCS. Thus, they proposed that SMR would be the most highlighted to depend on the technology development of the process,
feasible H2 production technology in the near future and calculated that market development for the product carbon from process, and tigh-
the production costs would be 36 EUR/MWh without CCS and tening of the carbon dioxide emission regulation [17].
39.6 EUR/MWh with CCS [11]. Similarly, Simbeck and Chang [12] This paper is a continuation of a previous techno-economic analysis
found SMR as less expensive H2 production technology than coal partial of four commercial scale process concepts for TDM that was conducted
oxidation, biomass and petroleum coke gasification, or water electro- by some of the authors [18]. One of the concepts presented in that study
lysis. In their analysis, the H2 production costs by SMR varied from was taken as a starting point in the current study and the analysis was
30 EUR/MWh to 67 EUR/MWh depending on the sequential H2 delivery complemented by applying the technology development work pre-
solution [12]. Less mature technologies were studied by Khojasteh sented in [19] in the reactor design. Thus, this paper combines the
Salkuyeh et al. [13] who analyzed economics of H2 production from previously conducted technical analysis of TDM with an economic
natural gas by two chemical looping processes in comparison with ex- analysis. As a result, this paper illustrates the market conditions where
isting SMR and auto-thermal reforming of natural gas. According to the TDM would be an economically feasible technology for H2 production
results, chemical looping reforming technology is promising when the in comparison with SMR and electrolysis. In addition to the evaluation
energy efficiency, emissions, and H2 production costs are considered. of the current market situation, i.e. where the current natural gas and
However, due to the technical challenges related to the heat transfer electricity costs are applied, the future market environment is discussed
inside the process, catalyst durability, and continuous operation, fur- as well. In order to take into account the environmental aspects, the
ther research is required until the chemical looping reforming tech- specific CO2 emissions in H2 production in each process were calcu-
nology is commercially available [13]. Furthermore, Yao et al. [14] lated.
conducted a techno-economic assessment of H2 production by biomass
gasification, biogas reforming, and water electrolysis. As a result, the 2. Analyzed processes
economic feasibility of the three processes was about the same when
the H2 production capacity was 1000 Nm3/h [14]. This section introduces the four processes for H2 production that
Yaun et al. [15] evaluated the H2 production costs of various ther- were analyzed in this study. The processes are outlined and the process
mochemical processes using different feedstocks, i.e., natural gas, flow charts are presented.
diesel, methanol, and biomass. One of the technologies in the analysis
was applying catalytic methane decomposition to natural gas in order
2.1. Thermal decomposition of methane process
to produce H2 and carbon nanotubes. According to the results, the H2
production by methane decomposition would be economically compe-
In TDM, methane is converted to gaseous H2 and solid carbon. The
titive with SMR when the value of the product carbon from methane
global reaction equation for methane decomposition is [20]:
decomposition would be more than 440 USD/tC and the CO2 emission
allowance cost would be 35 USD/tCO2 [15]. Parkinson et al. [16] ana- CH 4 (g) → C(s) + 2H2 (g) ΔHr0 = +76 kJ/mol (1)
lyzed the cost of H2 production by TDM that is conducted in a molten
metal process. According to the results, H2 production by TDM was The methane conversion and the properties of the product carbon de-
competitive with SMR with the product carbon value of 200 USD/tC pend on the reaction conditions e.g. temperature, reaction time and
and a carbon tax of 78 USD/tCO2. Moreover, decreasing the TDM catalyst properties if one is applied. The influence of the reaction
conditions on the TDM reaction and product carbon quality have been

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T. Keipi et al. Energy Conversion and Management 159 (2018) 264–273

summarized in [21]. This study focuses on non-catalytic TDM at reac- modification of the TDM process presented above. Here, the solid
tion temperature of 1500 K. carbon produced in the TDM reaction is gasified in order to produce
The TDM process studied in this paper (flow chart shown in Fig. 1) more H2. This could be a viable option if the TDM product carbon has a
was designed based on the process design previously presented by some low value or the separation of the carbon from the bed material turns
of the authors in [18]. The main component in the TDM process is a out expensive or difficult.
regenerative heat exchanger reactor (RHER), which is a TDM reactor As in the TDM process, the TDMG process consists of the RHER
type presented in detail in [18]. In RHER, natural gas is fed into the reactor, H2 separation from the product gas with membranes as well as
reactor and it meets the counter-current flow of solid bed material. The the carbon filtering and handing. These process components are similar
heat in the product gas transfers to the bed material at the end of the than in the TDM process. By contrast, in the TDMG process the carbon
reactor, and on the contrary, the bed material heats up the feedstock that deposits on the bed material in RHER is conveyed by the bed
gas at the beginning of the reactor. Furthermore, the TDM product material circulation to a separate gasification reactor. After the steam
carbon deposits on the surface of the solid bed material, and the carbon gasification, the gas flows to a water–gas shift (WGS) reactor in order to
is conveyed by the bed material circulation from the reactor. The ex- decrease the CO content and to increase the H2 content in the product
ternal heat required for the reactor heat-up and the TDM reaction is gas. Finally, H2 is separated using pressure swing adsorption (PSA)
provided by burning an additional natural gas feed. which is commercially available technology for H2 purification starting
Contrary to the previous process coupling in [18], where the aim from the capacity of 100 NmH23/h [28]. The H2 recovery in PSA was
was to produce H2-rich natural gas, in the current process H2 is sepa- selected as 0.9 [23]. The remaining PSA off-gas is combusted with ex-
rated from the product gas with H2 selective membranes and the un- cess natural gas to provide the heat required in the RHER reactor and in
reacted methane is recirculated to the TDM reactor. Thus, the main the gasification reactor. The H2 separation from the gasification gas
objective is to produce high-purity H2. Commercially available H2 se- cannot be conducted by palladium membranes due to the poisoning
lective palladium membranes with high H2 selectivity (above 1000) effect of CO in the gas [29].
were selected in this study [22]. Membranes are easy to control and
those provide an economic option for H2 separation in small scale ap-
2.3. Steam methane reforming process
plications [23].
The main part of the TDM product carbon (80%) was assumed to
A simplified process flow chart for steam methane reforming (SMR)
deposit on the bed material whereas the remaining carbon flowed out
is shown in Fig. 3. The pretreated natural gas flows to the reformer
from the reactor with the gas flow and was filtered from the product
where it reacts with steam and produces H2 and CO. The next step in
gas. This approximation is based on experiments conducted by the
the process is WGS, where CO reacts with additional steam and pro-
authors with a laboratory-scale test reactor [19]. The separated product
duces more H2 and CO2. In this study, the WGS reactor is divided into
carbon is cooled down below its self-ignition temperature, pelletized
two steps: a high-temperature shift (reactor temperature 723 K) and a
and packed to be ready for marketing.
low-temperature shift (reactor temperature 493 K) [23]. H2 is separated
The product carbon in the non-catalytic TDM reaction at tempera-
from the product gas in a PSA unit where the H2 recovery is 0.9 [23].
tures above 1500 K has been observed to be carbon black [21]. Carbon
The remaining PSA off-gas is burned with additional natural gas in
black is composed of elemental carbon and it has an extremely fine
order to produce the heat and steam needed in the process. SMR is
particle size [24]. Carbon black is utilized as a reinforcing material in
commercially available both in a small scale (H2 production between
rubber products and as a pigment in paints and inks. Depending on the
10 Nm3/h and 1000 Nm3/h ) [30] and in a large scale with H2 production
quality, the carbon black price varies from 500 EUR/t to 2000 EUR/t
up to 100,000 Nm3/h [2]. Additional SMR process values were taken
[25–27].
from [23,31].
Furthermore, a process where SMR is coupled with CCS was ana-
2.2. Thermal decomposition of methane with gasification lyzed in this study. The currently leading technology for CO2 capture
from an SMR process is to capture CO2 from the syngas by using che-
TDM with gasification (TDMG) process (flow chart in Fig. 2) is a mical solvents. Here, CO2 capture from the WGS product gas was

Fig. 2. Flow chart of the TDMG process.

Process Methane recirculation Process
inputs outputs
Product gas Carbon Gas
H2
filter separation

Cooling
Carbon
RHER Product Pressure
Water-gas
carbon swing H2
shift
gasification adsorption
Natural gas,
feedstock Bed
material
circulation
Heat Heat
Natural gas,
fuel PSA off-gas
Furnace Flue gas
Air
Water

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T. Keipi et al. Energy Conversion and Management 159 (2018) 264–273

Fig. 3. Flow chart of the SMR process.

Process Process
inputs outputs

CO2
Natural gas,
Pressure
feedstock Steam Water-gas CO2
swing H2
reforming shift capture
adsorption
Cooling
Natural gas, Heat
fuel PSA off-gas
Furnace Flue gas
Air

Water

assumed to occur by using chemical absorption with CO2 separation confirmed. Similarly, the gas compositions after both WGS steps were
efficiency of 95% [31]. calculated and confirmed to be equal with those presented in [23]. The
energy requirement in electrolysis was calculated using the specific
2.4. Water electrolysis energy consumption (52 kWh/kgH2). The oxygen production in elec-
trolysis was calculated to correspond the amount of the produced H2.
Utilization of water as feedstock in electrolysis enables the pro- The RHER reactor design in the TDM and TDMG processes was
duction of high-purity H2 for demanding applications such as fuel cells conducted by applying the global TDM reaction mechanism with the
[3]. The currently commercially available electrolyzers include kinetic parameters for non-catalytic TDM as presented in [19]. The
polymer electrolyte membrane (PEM) and alkaline electrolyzer tech- reactor dimensioning in the TDM and TDMG processes was conducted
nologies. PEM electrolyzers are available only at a small scale (H2 by taking into account the required gas residence time and the feed-
production up to 100 Nm3/h ) whereas the H2 production capacity of the stock volumetric flows in the reactor. In the TDMG process, the com-
current commercially available alkaline electrolyzers is up to position of the product gas from the TDM product carbon gasification
1000 Nm3/h [32]. Furthermore, the alkaline electrolyzers are less ex- was calculated by using the petroleum coke gasification gas composi-
pensive than other electrolyzer technologies and the technology has tion as a reference [42]. The gas composition after WGS reactor was
been proven as reliable and durable [32]. Thus, alkaline electrolysis calculated by following the WGS reaction equation [23]:
was chosen as the electrolytic H2 production technology in this study. CO + H2 O↔ CO2 + H2 (2)

3. Techno-economic analysis One WGS reactor step was required in order to achieve CO content
below 3% that enables feeding the gas to a PSA unit.
The assumptions made in the analysis are shown in this section. The heat requirement in each reactor was calculated based on the
Moreover, the procedure for both the technical and economic analysis reaction enthalpies and calculated conversion values. The internal heat
is presented. transfer possibilities in each process and the fuel energy of the PSA off-
gas in TDMG and SMR were taken into account when calculating the
3.1. Technical analysis external fuel energy requirement. Moreover, cooling was added to the
processes when needed. The resulting mass balances for each process
After designing the process schemes, the technical values were se- are shown in Table 2.
lected and mass balances were calculated for each process. The H2
production capacity was selected as 1000 Nm3/h, which equals the 3.2. Economic analysis
requirement of a small industrial process in the production of food,
electronics, glass or metals [3]. Additionally, large-scale H2 production The specific H2 production costs in each six processes were ana-
(100,000 Nm3/h) by SMR was taken into account both with and lyzed. In the TDM and TDMG processes, the main process components
without a CCS coupling. This H2 production capacity is sufficient for were listed and the capital expenditure (CAPEX) of each component
large industrial processes in oil refining and in ammonia and methanol was estimated based on the reference costs presented in the literature.
production [3]. Totally, six H2 production processes were analyzed in The costs were evaluated by applying the equation:
this study: small-scale TDM (TDM-SS), small-scale TDMG (TDMG-SS), S
n

small-scale water electrolysis (Electrol.-SS), small-scale SMR (SMR-SS), C2 = C1 ⎛ 2 ⎞

⎜ ⎟

large-scale SMR (SMR-LS), and large-scale SMR with a CCS coupling ⎝ S1 ⎠ (3)
(SMR-LS-CCS). For the sake of simplicity, natural gas was assumed to where C2 is the CAPEX of a component with capacity S2, C1 is the CAPEX
contain 100% of methane. The technical and economic assumptions in of a component with capacity S1 and n is the exponent that most typi-
this study are listed in Table 1. cally has value between 0.4 and 0.9 [34]. The exponent values and the
The calculation boundaries in the mass and energy balance analyses reference plant capacities and costs applied in this study are listed in
are shown in process flow charts (Figs. 1–3). The pre-defined H2 pro- Table 1. The reactor CAPEX evaluation in the TDM and TDMG processes
duction capacities were used as a starting point of these calculations. was carried out by using the RHER reactor cost estimate in the previous
The input mass flows were calculated based on the reaction equations at study [18] as a reference. Furthermore, the TDM product carbon pel-
each stage of the process. In SMR, the reformer product gas composition letizing and packing costs were evaluated based on the CAPEX esti-
was calculated based on the selected reactor values and a correspon- mation presented for pellet production from crops [33]. Applying Eq.
dence to a typical reformer gas composition presented in [23] was (3) allows a preliminary capital cost estimation with accuracy of ± 50%

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Table 1 Table 1 (continued)

The technical and economic assumptions for each H2 production technology.
Technology-specific Unit Description Ref.
Technology-specific Unit Description Ref. values
values
CO2 capture and 8.7 EUR/ [31]
TDM compression cost MWhH2
Methane conversion 0.7 CO2 transport and storage 1.4…11.1 EUR/ [40]
Residence time in reactor 5.4 s cost MWhH2
O&M costa 2 % of CAPEX p.a [18] CO2 capture energy 2.95 GJ/ t CO2 [41]
requirement
Process components:
TDM reactor CAPEX 2740 kEUR [18] a
Operation and maintenance costs excluding electricity, methane and membrane
Carbon pelletizer 121 kEUR Ref. production 8 [33]
OPEX.
CAPEX tons of pellets/h 2
Operation and maintenance costs excluding electricity.
Scale factor 0.6 [34] 3
Operation and maintenance costs excluding methane and electricity.

Membranes:
Reactor CAPEX (excl. 98 kEUR Ref. membrane [35] [34]. In order to avoid underestimating the TDM and TDMG process
membrane tubes) producing costs, a contingency equal to 30% of the equipment cost was added to
4.79 kg H2 /h the CAPEX of these two processes.
Membrane tubes, 273 kEUR Ref. membrane [35] In contrast to the TDM and TDMG processes, where the CAPEX es-
palladium capacity 2 MWH2
timation was conducted for each process component separately, the
Scale factor 0.7 [35]
OPEX of membranes 4 % of total membrane [35] CAPEX evaluation for SMR and electrolysis was based on the invest-
CAPEX ment cost estimations presented in the literature for entire processes.
The CAPEX of alkaline electrolyzers is currently 760–1100 EUR/kW
Waste heat boiler: and due to the technological improvements the cost is expected to be
CAPEX 25 kEUR Ref. plant 493 MWth [36]
370–800 EUR/kW in 2030 [38]. By contrast, the CAPEX for SMR is
Scale factor 1 [36]
2700–4500 EUR/kW for small-scale H2 production (50–5000 Nm3/h )
TDMG and 350–530 EUR/kW for large scale H2 production
Methane conversion 0.7 (50,000–100,000 Nm3/h ) [2].
Residence time in TDM 2.8 s
The economically most feasible targets for CCS applications are the
reactor
O&M costa 3 % of CAPEX p.a [18] large point sources (0.1 million tonnes of CO2), and therefore, in this
study, CCS was coupled to large-scale SMR only (abbreviated as SMR-LS
Process components: +CCS in the results) [43]. The transportation and storage costs of CO2
TDM reactor CAPEX 1465 [18] depend on the distance of the plant from the CO2 storage site. In this
Gasifier CAPEX 211 kEUR Ref. plant with [37]
study, the additional cost of CO2 capture, pressurization, transportation
1 MWth feedstock
input and storage has been assumed to vary between 10.1 EUR/MWh H2 and
PSA CAPEX 302 kEUR Ref. plant with [37] 19.8 EUR/MWh H2 based on estimations in [31,40]. Additionally, the
1 MWth feedstock increased fuel consumption due to CO2 capture was calculated sepa-
input
rately by applying the energy requirement shown in Table 1. The in-
WGS CAPEX 59 kEUR Ref. plant with [37]
1 MWth feedstock
creased fuel consumption was subtracted from the total CCS costs and
input the fuel costs were transferred to the operational costs.
Carbon pelletizer 35 kEUR Ref. production 8 [33] The total CAPEX in each process was divided into an annual capital
CAPEX tons of pellets/h cost for the investment (Annual capital cost = CRF·Total capital cost ) by
Scale factor 0.6 [34]
using the capital recovery factor (CRF) defined as
Membranes:
i (1 + i) N
Reactor CAPEX (excl. 71 kEUR Ref. membrane [35] CRF =
membrane tubes) producing 4.79 (1 + i) N −1 (4)
kg H2 /h
Membrane tubes, 198 kEUR Ref. membrane [35] where i is the interest rate (–), N is the investment period in years [44].
palladium capacity 2 MWH2 In this study, an interest rate of 10% and an investment period of
Scale factor 0.7 [35] 10 years was assumed.
OPEX of membranes 4 % of total CAPEX [35] The operational expenditure (OPEX) in each process consists of the
cost of feedstock, power and CO2 emission allowances as well as other
ELECTROLYSIS
CAPEX (current) 1000 EUR/kW [38] operation and maintenance (O&M) costs. The O&M costs in each pro-
CAPEX (2030) 600 EUR/kW [38] cess depend on the investment costs as presented in Table 1.
O&M cost2 3 % of CAPEX p.a [38] In the cost analyses, both the current market situation and potential
Energy consumption 52 kWh/ [38] market environments in 2030 were evaluated. The current market si-
kg H2
tuation was simulated applying the base case values shown in Table 3.
The natural gas price equals the 5-year average European Energy Ex-
SMR
Pressure drop in reformer 5 % [31] change spot price [45]. Similarly, the electricity price equals the 5-year
and in WGS average Nord Pool system price [46]. The CO2 emission allowance cost
Reformer steam-to-carbon 2.5 [23] slightly higher than the current market value was chosen to highlight
ratio
the effect of CO2 emissions. To be on the safe side, a pessimistic as-
Reformer CH4 conversion 0.8 [23]
CAPEX, small scale 3600 EUR/kW [2]
sumption for the value of the TDM product carbon (0 EUR/t C ) and
CAPEX, large scale 450 EUR/kW [2] oxygen from electrolysis (0 EUR/t O2 ) was chosen. However, the effect of
O&M cost3 5 % of CAPEX p.a. [39] the TDM product carbon value up to 300 EUR/t C and oxygen value up
to 70 EUR/t O2 [47,48] was analyzed as well in this study.
The potential market environments in 2030 were evaluated by using

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T. Keipi et al. Energy Conversion and Management 159 (2018) 264–273

Table 2
The mass balances for the evaluated H2 production processes. SS = small scale, LS = large scale.

TDM-SS TDMG-SS Electrol.-SS SMR-SS SMR-LS SMR-LS + CCS

Technical values
Reactor temperature 1500 1500 – 1123 1123 1123 K
H2 production 1000 1000 1000 1000 100,000 100,000 Nm3/h
H2 purity 0.9995 0.9995 0.9980 0.9995 0.9995 0.9995

Mass balance, input

Methane, feedstock 0.10 0.06 – 0.07 6.9 6.9 kg/s
Methane, fuel 0.02 0.01 – 0.02 2.0 2.4 kg/s
Air 0.30 0.35 – 0.73 73 81 kg/s
Water – 0.09 0.22 0.12 12 12 kg/s

TOTAL 0.41 0.52 0.22 0.94 94 102 kg/s

Mass balance, output

Hydrogen 0.02 0.02 0.02 0.02 2.5 2.5 kg/s
Product carbon 0.07 0.01 – – – – kg/s
Oxygen – – 0.20 – – – kg/s
CO2, emitted 0.04 0.17 - 0.24 24 11 kg/s
CO2, captured – – – – – 14 kg/s
Other flue gases 0.27 0.32 – 0.67 67 74 kg/s

TOTAL 0.41 0.52 0.22 0.94 94 102 kg/s

Table 3 were calculated by taking into account the investment cost estimation
The operational cost values in the base case. ranges presented in the literature for these processes. By contrast, the
uncertainties in the TDM and TDMG processes were calculated by
Base case Ref.
taking into account the accuracy in the order of magnitude cost esti-
Input costs mations for the process components.
Natural gas 20 EUR/MWh [45] In the current market situation, large-scale SMR is the most in-
Electricity 30 EUR/MWh [46] expensive process for H2 production. TDM cannot compete with large-
CO2 emission allowance 10 EUR/t CO2
scale SMR in economic sense in a case where the TDM product carbon
Process water 1 EUR/m3 [34]
does not have a market value. By contrast, the small-scale SMR process
Product values is more expensive than any other process studied here. The CAPEX of
Product carbon 0 EUR/tC electrolysis is currently relatively high, but is expected to decrease
Oxygen 0 EUR/tO2 around 50% until 2030 as the technology develops.
The OPEX in each process was divided into components in Fig. 5.
Electricity is the major OPEX component in H2 production costs by
the following operational costs as a basis of the analysis: CO2 emission
electrolysis. In contrast, in all the other processes, the natural gas cost is
allowances 50 EUR/t CO2 , electricity 50 EUR/MWh and natural gas
the dominating OPEX cost. The CO2 emission cost has a minor effect on
40 EUR/MWh. The natural gas cost estimation was based on a report by
the overall OPEX in the processes.
the U.S. Energy Information Administration [49] that predicts that the
natural gas price will double from the current value by 2030. As the
European gas price was 2.2 times higher than that in US in 2016 [50], it 4.2. Hydrogen production costs
was estimated that the European natural gas price in 2030 would be
40 EUR/MWh, which is double the current price. The availability of The effect of several variables (the cost of natural gas, electricity
renewable electricity at low cost (10–30 EUR/MWh) for electrolysis was and CO2 emission allowances as well as the value of oxygen and the
assumed to be limited (3000 h/a) based on an estimation by the IEA TDM product carbon) on the H2 production costs in each process was
[2]. Moreover, the sensitivity of the H2 production costs towards the analyzed. The analysis results presenting the current market situation
costs of electricity, natural gas, TDM product carbon and oxygen was are shown in Fig. 6. Increasing the CO2 emission allowance cost raises
analyzed in order to simulate various future market environments. more the H2 production costs by SMR (long dash line) than those by
TDM (dash dot line). However, TDM cannot economically compete with
SMR even if the CO2 emission allowance cost is 100 EUR/t CO2 if the
4. Results and discussion TDM product carbon has no market value. In a case that the TDM
product carbon value is 310 EUR/tC, the CO2 emission allowance cost of
This section presents the results of the economic analysis of the H2 10 EUR/tCO2 is sufficient to make H2 production by TDM a less costly
production processes as well as the CO2 emissions associated in each option than by SMR. The results are in line with the ones presented by
process. Parkinson et al. [16] who found that the product carbon value of 200
USD/tC and a carbon tax on 78 USD/tCO2 would make TDM econom-
4.1. Investment and operational costs ically competitive with SMR.
With a moderate value of the TDM product carbon (30–230 EUR/
The process costs were calculated with the base case values and the tC), the cost of H2 production by TDM, by TDMG and by SMR coupled to
OPEX and CAPEX in each process were divided into categories in CCS are within the same cost range. Thus, with the TDM product carbon
Table 4. values below 230 EUR/tC the gasification of the product carbon in order
Additionally, the CAPEX and OPEX in each process are graphically to gain more H2, i.e. the TDMG process, becomes economically more
presented in Fig. 4. The error bars in Fig. 4 represent the uncertainty of feasible than the TDM process. According to the analysis, CO2 allow-
the CAPEX estimations. The uncertainty values in SMR and electrolysis ance cost of 60 EUR/t CO2 is required so that coupling CCS to SMR would

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Table 4
The annual OPEX and the total CAPEX for the evaluated H2 production processes. The costs were calculated using the base case values in Table 3 in order to simulate the current market
situation. SS = small scale, LS = large scale.

TDM-SS TDMG-SS Electrol.-SS SMR-SS SMR-LS SMR-LS + CCS

OPEX
Methane 780 547 – 618 61,753 64,546 kEUR/a
CO2 emission allowances 8 42 – 61 6099 2778 kEUR/a
Electricity – 6 982 11 1064 1064 kEUR/a
Other O&M 27 24 15 87 1089 1089 kEUR/a
TOTAL OPEX 815 620 997 776 70,004 97,662 kEUR/a

CAPEX
Equipment 3233 2361 2974 10,705 133,815 162,000 kEUR
Contingency (30%) 970 708 – – – – kEUR
TOTAL CAPEX 4203 3069 2974 10,705 133,815 162,000 kEUR

TOTAL H2 production cost 72.0 53.8 71.1 117.0 44.1 57.4 EUR/MWh

150
Hydrogen production cost (EUR/MWh)

140

H2 production cost (EUR/MWh)

OPEX
120 120
CAPEX Cost range for electrolysis with
100 electricity cost 30-60 EUR/MWh
80 90

60
60
40
TDMG
20 Cost range for SMR coupled
30
0 with CCS
Cost range for TDM with product
carbon value 100-300 EUR/tC
0
0 25 50 75 100
CO2 emission allowance cost (EUR/t)
Fig. 4. Distribution of the H2 production costs in each process into the CAPEX and OPEX.
Fig. 6. Cost of H2 production by TDM, SMR and electrolysis with economic values re-
The error bars were calculated based on the uncertainty in the CAPEX estimations.
presenting the current market situation: electricity cost 30 EUR/MWh (in electrolysis
SS = small scale, LS = large scale.
30–60 EUR/MWh), natural gas cost 20 EUR/MWh, TDM product carbon value
0–300 EUR/tC, oxygen value 0 EUR/tO2 and full load hours 7000 h/a.
100%
Proportion of the total OPEX

80% 200
H2 production cost (EUR/MWh)

60% 160

40%
120
20% SMR (large scale)
80
Cost range for electrolysis with electricity
0% cost 10-30 EUR/MWh, 3000 h/a
40 Cost range for SMR coupled with CCS
Cost range for TDM with product
carbon value 100-300 EUR/tC
0
Fuel Electricity CO2 emission allowances Other O&M 20 40 60 80
Fig. 5. The OPEX distribution in each H2 production process. SS = small scale, LS = large Natural gas cost (EUR/MWh)
scale, O&M = operation and maintenance.
Fig. 7. Cost of H2 production by TDM, SMR and electrolysis with economic values re-
presenting a potential market situation in 2030: electricity price 50 EUR/MWh (in elec-
be an economically feasible option. This is in line with the analysis trolysis 10–30 EUR/MWh), CO2 emission allowance 50 EUR/t CO2 , TDM product carbon
results in [2] where the same CO2 cost requirement was found. The cost value 0–300 EUR/tC, oxygen value 0 EUR/t O2 and full load hours 7000 h/a (in electrolysis

of electrolytic H2 is notably high in comparison with TDM when the 3000 h/a).

electricity cost is between 30 EUR/MWh and 60 EUR/MWh (light gray

area). Among the studied processes, SMR in a small scale is the most An illustration of the possible market environments in the future in
expensive H2 production method in the current market situation 2030 is shown in Fig. 7. The major differences in this case in compar-
(dotted line). ison with the current market situation are the increased costs of

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electricity, natural gas and CO2 emission allowances as well as the costs of H2 transportation that are essential to centralized production.
decreased CAPEX in electrolysis due to the technology development as H2 transportation has been estimated to cause an additional cost of
was described in Section 3.2. Moreover, a limited amount of renewable 45 EUR/MWh H2 at transportation distances longer than 100 km and
electricity at low cost was assumed to be available for electrolysis. 22 EUR/MWh H2 at transportation distances below 50 km [53]. Adding
Since natural gas is used as feedstock both in TDM and in SMR, the high transportation cost to the H2 produced by SMR makes SMR
increasing the natural gas cost does not improve the competitiveness of more expensive technology than TDM regardless of the TDM product
TDM in comparison with SMR. Due to the environmental aspects, the carbon value. Moreover, the current natural gas network can be utilized
fossil natural gas could be replaced with alternative non-fossil methane to supply feedstock to the on-site TDM plants.
feedstocks e.g. synthetic natural gas (SNG) or biomethane. SNG pro-
duction from CO2 could provide a suitable application for the fluctu- 4.3. Sensitivity analysis
ating renewable electricity. The cost range for SNG with the availability
of 3000 h/a has been predicted to vary from 40 EUR/MWh to 390 EUR/ The most important factors affecting the H2 production costs were
MWh in the current market situation, and from 72 EUR/MWh to identified in the following. The natural gas cost has a major impact and
218 EUR/MWh in the market situation of 2050 depending on the as- the CO2 allowance minor impact on the H2 production costs by SMR
sumptions of the electricity cost, oxygen value and heat utilization [51]. based on the calculations. By contrast, electrolytic H2 production costs
Altogether, the production cost of SNG is much higher than the cost of are highly dependent on the electricity cost. Additionally, the product
fossil natural gas and the production is dependent on the availability carbon value was found to cause the greatest uncertainties in H2 pro-
and cost of renewable electricity [51]. The production cost of bio- duction costs by TDM.
methane has been estimated as 70 EUR/MWh [51], which is also high Furthermore, the effect of varying the interest rate between 1% and
in comparison with fossil natural gas. Therefore, alternative methane 20% on the H2 production costs was studied. As a result, the interest
sources as feedstock for TDM or SMR are not able to compete with fossil rate has the greatest impact on the H2 production costs when the capital
natural gas unless the production cost of these feedstocks would de- costs have a significant role as is the case in small-scale SMR, in TDM, as
crease considerably or the CO2 neutrality of SNG or biomethane would well as in current electrolysis technology. Varying the interest rate
be considered as a significant benefit. between 1% and 20% reduced or increased, respectively, the overall H2
With an extremely low electricity cost, 10 EUR/MWh, electrolysis is production costs in each technology up to 25%.
a more inexpensive H2 production method than SMR when the natural Accordingly, the effect of varying the scale factor in the TDM re-
gas cost is above 16 EUR/MWh. However, the availability of renewable actor cost analysis was studied by applying values between 0.4 and 0.9.
electricity with this low cost is limited in this study to 3000 h/a based As a result, the H2 production costs in TDM or TDMG processes re-
on the prediction of the IEA [2]. The limited availability of renewable spectively increased or reduced by 20%. However, the results show that
electricity results in fluctuating H2 production, and therefore, it cannot the product carbon value has a greater impact especially on the TDM
be utilized for demand-driven H2 production. process economics.
Another graph presenting the prospective future (2030) market
environments is shown in Fig. 8. The graph highlights that adding an 4.4. Carbon dioxide emissions
oxygen value of 70 EUR/t O2 to the electrolysis OPEX decreases the
electrolytic H2 production costs by 17 EUR/MWh. The electricity cost The CO2 emissions from each process were divided by the amount of
below 56 EUR/MWh is required so that electrolysis with the oxygen H2 produced and the results are shown in Table 5. The specific CO2
value of 70 EUR/t O2 would be cost competitive in H2 production in emissions (kgCO2/MWh H2) of H2 produced by SMR are the highest but
comparison with SMR. In order to TDM to be able to compete with SMR those can be reduced by adding CO2 capture to the process. The SMR
in this market situation, the TDM product carbon value above 280 EUR/ coupling with CCS studied here, where CO2 is captured from the WGS
tC is required. A similar value (350 USD/tC) has been previously found product gas, does not enable capturing all of the CO2 from the process,
as a break-even price for the TDM product carbon [52]. since burning the additional natural gas flow in the furnace causes
According to the results, small or medium industrial scale H2 pro- emissions as well. Theoretically, up to 60% of the overall CO2 emissions
duction that occurs on-site is the most suitable application for TDM. from the SMR process could be sequestered when CO2 is captured from
The advantage of distributed H2 production by TDM is avoiding the the syngas [54]. This means that the theoretical minimum value for the
specific CO2 emissions of the H2 produced by SMR coupled to CO2
220 capture from the syngas is 112 kgCO2/MWh H2 . This is still roughly
200 Cost range for electrolysis with threefold the specific emissions from the TDM process. Further reduc-
H2 production cost (EUR/MWh)

oxygen value 30-70 EUR/tO2

180 tion of the CO2 emissions requires capturing CO2 additionally from the
furnace flue gas, which would cause additional costs [54].
160
Electrolysis enables the production of CO2-free H2. However, the
140 overall CO2 emissions from electrolysis are highly dependent on the
120 TDM (prod. carbon 0 EUR/tC) electricity generation technology. For example, powering electrolysis
100 by the European grid electricity, which currently has the specific CO2
emissions of 454 kgCO2/MWh el [55], would cause specific CO2 emissions
80
60 SMR (large scale)
Table 5
Cost range for SMR
40 coupled with CCS
The specific CO2 emissions of H2 production with the evaluated technologies. Electrolysis
is assumed to be powered by CO2-free electricity.
20 Cost range for TDM with product
carbon value 100-300 EUR/t C Process Emissions
0
0 30 60 90 120
TDM 40 kgCO2 /MWhH2
Electricity cost (EUR/MWh)
TDMG 203 kgCO2 /MWhH2
Fig. 8. Cost of H2 production by TDM, SMR and electrolysis with economic values re- SMR 293 kgCO2 /MWhH2
presenting a potential market situation in 2030: natural gas price 40 EUR/MWh, CO2 SMR coupled with CCS 133 kgCO2 /MWhH2
emission allowance 50 EUR/t CO2 , TDM product carbon value 0–300 EUR/tC, oxygen value
Electrolysis 0 kgCO2 /MWhH2
0–70 EUR/t O2 and full load hours 7000 h/a.

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